Co-reporter:Tianzhi Liu, Nan Zhang, Zhigang Wang, Meiying Wu, Yu Chen, Ming Ma, Hangrong Chen, and Jianlin Shi
ACS Nano September 26, 2017 Volume 11(Issue 9) pp:9093-9093
Publication Date(Web):August 10, 2017
DOI:10.1021/acsnano.7b03772
High intensity focused ultrasound (HIFU) surgery generally suffers from poor precision and low efficiency in clinical application, especially for cancer therapy. Herein, a multiscale hybrid catalytic nanoreactor (catalase@MONs, abbreviated as C@M) has been developed as a tumor-sensitive contrast and synergistic agent (C&SA) for ultrasound-guided HIFU cancer surgery, by integrating dendritic-structured mesoporous organosilica nanoparticles (MONs) and catalase immobilized in the large open pore channels of MONs. Such a hybrid nanoreactor exhibited sensitive catalytic activity toward H2O2, facilitating the continuous O2 gas generation in a relatively mild manner even if incubated with 10 μM H2O2, which finally led to enhanced ablation in the tissue-mimicking PAA gel model after HIFU exposure mainly resulting from intensified cavitation effect. The C@M nanoparticles could be accumulated within the H2O2-enriched tumor region through enhanced permeability and retention effect, enabling durable contrast enhancement of ultrasound imaging, and highly efficient tumor ablation under relatively low power of HIFU exposure in vivo. Very different from the traditional perfluorocarbon-based C&SA, such an on-demand catalytic nanoreactor could realize the accurate positioning of tumor without HIFU prestimulation and efficient HIFU ablation with a much safer power output, which is highly desired in clinical HIFU application.Keywords: catalytic nanoreactor; HIFU ablation; hybrid nanostructure; mesoporous organosilica nanoparticles; tumor microenvironment;
Co-reporter:Luodan Yu, Yu Chen, Hangrong Chen
Chinese Chemical Letters 2017 Volume 28, Issue 9(Volume 28, Issue 9) pp:
Publication Date(Web):1 September 2017
DOI:10.1016/j.cclet.2017.05.023
The fast progress of stimuli-responsive theranostic nanomedicine can achieve the specific and high-performance diagnosis and therapy of various diseases. Especially, H2O2-responsive theranostic nanomedicine is recently emerging as a new stimuli-responsive modality showing the great potential for the theranostic of diseases with overexpressed H2O2 because H2O2 is associated with several kinds of human diseases as the most stable and abundant reactive oxygen species. This review summarizes and discusses the very-recent developments of H2O2-responsive theranostic nanoplatforms for versatile biomedical applications, including diagnostic imaging, attenuating tumor hypoxia, enhancing the therapeutic efficiency of photodynamic therapy/radiation therapy/chemotherapy and theranostic of inflammation/diabetic. The facing challenges and future developments of H2O2-responisve theranostics are also briefly discussed to further promote the clinical translation of this new responsive theranostic modality. It is highly believed that H2O2-responsive theranostic nanomedicine will be extensively developed a new specific and efficient theranostic modality to benefit the personalized biomedicine in the near future.Download high-res image (91KB)Download full-size imageThis review summarizes and discusses the very-recent developments of H2O2-responsive theranostic nanoplatforms for versatile biomedical applications, including diagnostic imaging, attenuating tumor hypoxia, enhancing the therapeutic efficiency of photodynamic therapy/radiation therapy/chemotherapy and theranostic of inflammation/diabetic. It is highly believed that H2O2-responsive theranostic nanomedicine will be extensively developed a new specific and efficient theranostic modality to benefit the personalized biomedicine in the near future.
Co-reporter:Ming Ma 马明;Yanhong Yan 颜燕宏;Chao Qi 漆超;Shengcai Qi 祁胜财
Science China Materials 2017 Volume 60( Issue 6) pp:516-528
Publication Date(Web):16 May 2017
DOI:10.1007/s40843-017-9038-5
Biomedical applications of porous calcium carbonate (CaCO3) microspheres have been mainly restricted by their aqueous instability and low remineralization rate. To overcome these obstacles, a novel symmetry-breaking assembled porous calcite microsphere (PCMS) was constructed in an ethanol/water mixed system using a two-step vapor-diffusion/aging crystallization strategy. In contrast to the conventional additive-induced crystallization method, the present strategy was performed under mild conditions and was free from any foreign additives, thus avoiding the potential contamination of the final product. Meanwhile, the prepared PCMSs were characterized by their highly uniform spherical morphology and large open pores, which are favorable for large protein delivery. An antimicrobial study of immunoglobulin Y (IgY)-loaded PCMSs revealed excellent antimicrobial activity against Streptococcus mutans. More importantly, they showed surprisingly rapid transformation to bone minerals in physiological medium. Evaluation of the in vitro efficacy of PCMSs in dentinal tubule occlusion demonstrated their powerful potential to serve as a catalyst in the repair of dental hard tissue. Therefore, the developed PCMSs show great promise as multifunctional biomaterials for dental treatment applications.多孔碳酸钙微球的弱水溶液稳定性和低再矿化速率限制了其在生物医药领域的应用. 为了解决该问题, 本论文通过“气体扩散-陈化” 两步策略制备了具有大孔结构和方解石相的碳酸钙微球材料. 该合成策略反应条件温和, 同时不需要使用模板剂和晶型导向剂, 能够确 保微球产物的生物安全性. 所制备的碳酸钙微球可以吸附大量的免疫球蛋白IgY, 并表现出增强抑制口腔变形链球菌的能力. 此外, 研究显 示该微球可以在水溶液中保持较高的结构稳定性, 而在人体体液和唾液环境中快速再矿化并转变成羟基磷灰石结构, 对牙本质小管具有 较佳的封闭效果, 为其用于治疗牙本质过敏症提供了依据.
Co-reporter:
ChemSusChem 2017 Volume 10(Issue 3) pp:499-505
Publication Date(Web):2017/02/08
DOI:10.1002/cssc.201601396
AbstractA nitrogen-doped vesicle-like porous carbon with well-integrated dual iron-based catalytic sites was developed through direct pyrolysis of inexpensive and abundant precursors. Benefiting from the mesoporous structures with synchronous construction of Fe–Nx and Fe/Fe3C@NC sites, the optimized catalyst exhibited outstanding performance for the oxygen reduction reaction (ORR) in alkaline media, even superior to the commercial Pt/C catalyst. Detailed characterizations revealed that Fe/Fe3C@NC sites can make major catalytic contributions in basic media, whereas the Fe–Nx sites were found to play an indispensable role for ORR in acidic media.
Co-reporter:Gang Wan;Ce Yang;Wanpeng Zhao;Qianru Li;Ning Wang;Tao Li;Hua Zhou;Jianlin Shi
Advanced Materials 2017 Volume 29(Issue 47) pp:
Publication Date(Web):2017/12/01
DOI:10.1002/adma.201703436
AbstractThe introduction of active transition metal sites (TMSs) in carbon enables the synthesis of noble-metal-free electrocatalysts for clean energy conversion applications; however, there are often multiple existing forms of TMSs, which are of different natures and catalytic models. Regulating the evolution of distinctive TMSs is highly desirable but remains challenging to date. Anions, as essential elements involved in the synthesis, have been totally neglected previously in the construction of TMSs. Herein, the effects of anions on the creation of different types of TMSs are investigated for the first time. It is found that the active cobalt–nitrogen sites tend to be selectively constructed on the surface of N-doped carbon by using chloride, while metallic cobalt nanoparticles encased in protective graphite layers are the dominant forms of cobalt species with nitrate ions. The obtained catalysts demonstrate cobalt-sites-dependent activity for oxygen reduction reaction and hydrogen evolution reaction in acidic media. The remarkably enhanced catalytic activities approaching that of benchmark Pt/C in an acidic medium have been obtained on the catalyst dominated with cobalt–nitrogen sites, confirmed by the advanced spectroscopic characterization. This finding demonstrates a general paradigm of anion-regulated evolution of distinctive TMSs, providing a new pathway for enhancing performances of various targeted reactions related with TMSs.
Co-reporter:Xiaoxia Zhou, Yu Chen, Tongguang Ge, Zile Hua, ... Jianlin Shi
Science Bulletin 2017 Volume 62, Issue 14(Volume 62, Issue 14) pp:
Publication Date(Web):30 July 2017
DOI:10.1016/j.scib.2017.06.009
Hierarchically porous single-crystalline nanosized zeolites as heterogeneous catalysts show great potential in fine chemistry because they offer more rich hierarchically porous channels for the mass transfer and molecular diffusion. However, the synthesis of hierarchically porous nanosized zeolites generally requires the assistance of templates acting as the mesoporogens, which limits its popularity. Herein, we report a one-pot and template-free synthesis of hierarchically porous single-crystalline nanosized zeolite beta only by introducing sodium carbonate in precursor solution. The resulted sample features the extraordinary properties, including the uniform nanocrystal (200–300 nm), high pore volume (0.65 cm3 g−1) and the hierarchical pore-size distribution (e.g., 2–8 and 90–150 nm). After slicing processing, it is interestingly found that a large number of interconnected mesopores penetrate throughout whole material, which enables the hierarchically porous nanosized zeolite beta remarkably superior catalytic activity than the conventional zeolite beta in condensation of benzaldehyde with ethanol at room temperature. More importantly, this one-pot sodium carbonate-assisted synthetic strategy is highly versatile, which has also been successfully developed to synthesize hierarchically porous nanosized single-crystalline zeolites ZSM-5 and TS.Download high-res image (168KB)Download full-size image
Co-reporter:Han Zhao;Xiaoxia Zhou;Min Wang;Zhiguo Xie;Jianlin Shi
RSC Advances (2011-Present) 2017 vol. 7(Issue 6) pp:3233-3239
Publication Date(Web):2017/01/04
DOI:10.1039/C6RA25738K
A series of MnOx–CeO2 composites have been prepared via a facile coprecipitation method and used as catalysts for diesel soot combustion. It is found that the content of manganese oxide has a considerable influence on both the morphology and catalytic activity for diesel soot combustion in the copresence of NOx and O2. Superior catalytic activity (Tf = 360 °C) was obtained over the optimized catalyst CM20 [Mn/(Mn + Ce) equals to 20 at%], which is believed to be attributable to the following two aspects: (1) the abundant pore structure, presenting between the loosely-packed homogeneous particles with similar sizes to that of the soot particles, which is beneficial for mass transfer and heat diffusion as well as the sufficient contact between catalyst and soot; (2) high concentration of Mn4+ and Ce3+ cations derived from the charge transfer between Mn and Ce species as active sites can adsorb and activate NO and O2, and then greatly facilitate NO2 production.
Co-reporter:H. Zhao;X. X. Zhou;L. Y. Pan;M. Wang;H. R. Chen;J. L. Shi
RSC Advances (2011-Present) 2017 vol. 7(Issue 33) pp:20451-20459
Publication Date(Web):2017/04/05
DOI:10.1039/C7RA01971H
A series of Cu–Mn mixed oxides were prepared via a facile co-precipitation method and used as catalysts for diesel soot combustion in NOx/O2/N2. It is found that the chemical composition in the Cu–Mn mixed oxides has a significant influence on both morphology and catalytic activity. When the Cu/Mn atomic ratio was optimized to be 1, a distinctive pure spinel phase of Cu1.5Mn1.5O4 was obtained (named Cu1Mn1), which exhibited superior catalytic activity (e.g., finishing combustion temperature (Tf) = 360 °C, in loose contact mode). The excellent catalytic activity of Cu1Mn1 was mainly attributed to the following aspects: (1) distinct morphological features: the well-dispersed Cu1Mn1 microspheres with a rough surface could contact soot particles sufficiently, and the stacked pores between the loosely packed nanoparticles within the microspheres could facilitate the diffusion of gaseous O2, NO and NO2; and (2) the high intrinsic activity of the Cu1.5Mn1.5O4 phase: the abundant adsorbed oxygen species (Oads) is beneficial to the direct oxidation of soot into CO2, and the enormous Cu+–Mnλ+ (λ = 3, 4, hereinafter inclusive) cation pairs could facilitate the production of the strong oxidant NO2, and the interaction between Cu2+ and NO2 would lead to high enhancement efficiency of NO2 for soot combustion. This facile strategy for the high activity spinel phase towards catalytic soot combustion shows great promise for practical applications.
Co-reporter:X. X. Zhou;H. Zhao;W. M. Huang;H. R. Chen;J. L. Shi
Dalton Transactions 2017 vol. 46(Issue 18) pp:6111-6116
Publication Date(Web):2017/05/09
DOI:10.1039/C7DT00918F
TiO2 and spinel Cu1.5Mn1.5O4 co-modified hierarchically porous zeolite Beta (Ti/Cu1.5Mn1.5O4-HBeta) with 3D interpenetrating micro–mesoporosity has been synthesized, which showed highly efficient catalytic activity to the soot oxidation in the presence of O2/NO/N2 due to the rich moderate intensity acidic sites and chemisorbed oxygen species. In the presence of SO2/O2/NO/N2, the SO2 could be preferentially adsorbed on the Ti/Cu1.5Mn1.5O4-HBeta and the resulting sulfates could easily decompose at elevated temperatures, thus leading to significantly improved sulfur-resistance. Furthermore, the excellent water-resistance and cycling stability were achieved on the catalyst Ti/Cu1.5Mn1.5O4-HBeta owing to its crystalline zeolite framework and highly dispersed active components.
Co-reporter:Linyu Pan, Xiaoxia Zhou, Han Zhao, Gang Wan, Qianru Li, Ning Wang, Weimin Huang, Hangrong Chen
Catalysis Communications 2017 Volume 97(Volume 97) pp:
Publication Date(Web):5 July 2017
DOI:10.1016/j.catcom.2017.04.020
•Nanoflower Mg/MnOx was synthesized via a facile and scalable redox-precipitation.•Nanoflower Mg/MnOx catalyst shows good performance on low-concentration NOx removal.•The superior monolithic catalyst indicates great potential in actual application.•The accumulated NO2 covering active sites and its delayed desorption induce gradual deactivation.Nanoflower-like Mg doped MnOx (Mg/MnOx) is synthesized via a facile and scalable redox reaction strategy for facile removal of low-concentration NOx at room temperature. The optimized sample Mg/MnOx exhibits good activity, giving 100% NO removal efficiency at room temperature for 10 h under extremely high space velocity of 120,000 mL− 1 g− 1 h− 1 and low NO inlet concentration of 10 ppm. The Mg/MnOx is found to gradually get inactive resulted from the generated NO2 and large amount of adsorbed NO covering active sites based on the results of characterizations and performance. Furthermore, the superior monolithic catalyst indicates great potential in actual application.Download high-res image (116KB)Download full-size image
Co-reporter:Luodan Yu, Yu Chen, Meiying Wu, Xiaojun Cai, Heliang Yao, Linlin Zhang, Hangrong Chen, and Jianlin Shi
Journal of the American Chemical Society 2016 Volume 138(Issue 31) pp:9881-9894
Publication Date(Web):July 21, 2016
DOI:10.1021/jacs.6b04299
Biodegradability of inorganic nanoparticles is one of the most critical issues in their further clinical translations. In this work, a novel “metal ion-doping” approach has been developed to endow inorganic mesoporous silica-based nanoparticles with tumor-sensitive biodegradation and theranostic functions, simply by topological transformation of mesoporous silica to metal-doped composite nanoformulations. “Manganese extraction” sensitive to tumor microenvironment was enabled in manganese-doped hollow mesoporous silica nanoparticles (designated as Mn-HMSNs) to fast promote the disintegration and biodegradation of Mn-HMSNs, further accelerating the breakage of Si–O–Si bonds within the framework. The fast biodegradation of Mn-HMSNs sensitive to mild acidic and reducing microenvironment of tumor resulted in much accelerated anticancer drug releasing and enhanced T1-weighted magnetic resonance imaging of tumor. A high tumor-inhibition effect was simultaneously achieved by anticancer drug delivery mediated by PEGylated Mn-HMSNs, and the high biocompatibility of composite nanosystems was systematically demonstrated in vivo. This is the first demonstration of biodegradable inorganic mesoporous nanosystems with specific biodegradation behavior sensitive to tumor microenvironment, which also provides a feasible approach to realize the on-demand biodegradation of inorganic nanomaterials simply by “metal ion-doping” strategy, paving the way to solve the critical low-biodegradation issue of inorganic drug carriers.
Co-reporter:Gang Wan, Ming Ma, Alec (Yi) Jia, Lisong Chen, Yu Chen, Xiangzhi Cui, Hangrong Chen and Jianlin Shi
Journal of Materials Chemistry A 2016 vol. 4(Issue 30) pp:11625-11629
Publication Date(Web):04 Jul 2016
DOI:10.1039/C6TA03930H
A 3D assembly of crumpled nitrogen-doped carbon nanosheets with hierarchical frameworks and encased ultrafine iron carbide nanoparticles on the subunits was constructed via a template-free bottom-up self-assembly strategy. The optimized structure design and catalytic-site integration endow the electrocatalyst with outstanding PH-universal ORR performance, serving as a good alternative for the Pt/C catalyst.
Co-reporter:Ming Ma, Fei Yan, Minghua Yao, Zijun Wei, Dongliang Zhou, Heliang Yao, Hairong Zheng, Hangrong Chen, and Jianlin Shi
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 44) pp:29986
Publication Date(Web):October 24, 2016
DOI:10.1021/acsami.6b10370
Entirely differing from the common templating-based multistep strategy for fabricating multifunctional hollow mesoporous silica nanoparticles (HMSN), a facile and template-free synthetic strategy has been established to construct a unique hollow/mesoporous organosilica nanocapsule (OSNC) concurrently encapsulating both isopentyl acetate (PeA) liquid and superparamagnetic iron oxides inside (denoted as PeA@OSNC). This novel material exhibits ultrasmall and uniform particle size (∼82 nm), high surface area (∼534 m2·g–1), and excellent colloidal stability in aqueous solution. The oil-phase PeA with relatively low boiling point (142 °C) and high volatility not only plays a crucial role in formation of a large hollow cavity from the viewpoint of structural design but also enables the PeA@OSNC to act as an efficient enhancement agent in high-intensity focused ultrasound (HIFU) therapy. Moreover, the unique satellite-like distribution of Fe3O4 nanoparticles (NP) on the organosilica shell offered excellent magnetic resonance imaging (MRI) contrast capability of PeA@OSNC in vitro and in vivo. More importantly, such a novel theranostic agent has favorable biosafety, which is very promising for future clinical application in MRI-guided HIFU therapy.Keywords: contrast agent; HIFU; hollow mesoporous nanoparticle; organosilica; theranostic
Co-reporter:Kun Zhang, Huixiong Xu, Xiaoqing Jia, Yu ChenMing Ma, Liping Sun, Hangrong Chen
ACS Nano 2016 Volume 10(Issue 12) pp:
Publication Date(Web):November 22, 2016
DOI:10.1021/acsnano.6b04921
Inspired by considerable application potential in various diseases, nitric oxide (NO) has gained increasing attention. Nevertheless, current NO release scaffolds suffer from some inevitable drawbacks, for example, high toxicity for NO donor byproducts, poor specificity, shallow penetration depth, and strong ionizing irradiation for triggers, all of which remain obstacles to clinical application. Herein, an ultrasound-triggered NO on-demand release system is constructed using natural l-arginine as NO donor and local ultrasound as trigger. The focused ultrasound can activate H2O2 to generate more oxygen-contained species (ROS) of stronger oxidation ability than H2O2 for oxidizing LA via the energy transformation from ultrasound mechanical energy to chemical energy, and thus produce more NO for ultimately suppressing the highly aggressive and lethal Panc-1 tumor. Moreover, a blood vessel–intercellular matrix–cell “relay” targeting strategy has been established and relying on it, over 7-fold higher retention of such NO release system in a subcutaneous xenograft mouse model of Panc-1 is obtained, which consequently results in a more evident inhibitory effect and a prolonged survival rate (80% ± 5% improvement in 60-day survival).Keywords: l-arginine donor; Nitric oxide; oxygen-contained species; Panc-1 tumor; ultrasound trigger; “relay” targeting;
Co-reporter:Xiaojun Cai, Wei Gao, Linlin Zhang, Ming Ma, Tianzhi Liu, Wenxian Du, Yuanyi Zheng, Hangrong ChenJianlin Shi
ACS Nano 2016 Volume 10(Issue 12) pp:
Publication Date(Web):November 14, 2016
DOI:10.1021/acsnano.6b05990
Prussian blue (PB) has been used as a photothermal conversion agent to generate heat to induce localized damage to tumor. However, its therapeutic efficiency is far from satisfactory. One of the major obstacles is that the maximum NIR absorption peak of PB within 690–720 nm cannot be optimized near the wavelength of the laser to enhance its therapeutic efficiency. Herein, we report that the integration of Gd3+ into PB nanocrystals (GPB NCs) enables PB with tunable localized surface plasmon resonances (LSPRs) from 710 to 910 nm, achieving the maximum NIR peak near the wavelength of the laser. Concurrently, the efficiency of dual-mode imaging including photoacoustic imaging and magnetic resonance imaging has been greatly improved. These enhancements in dual-mode imaging and photothermal therapy enable PB with low nanomaterial dose and laser flux. Additionally, it is found that GPB NCs show the capability of not only acting as a chemical probe with tunable sensitivity but also scavenging reactive oxygen species. The integration of functional ions into a photothermal conversion agent is an efficient strategy to improve the synergy of nanoagent, enchancing tumor theranostic efficiency.Keywords: magnetic resonance imaging; photoacoustic imaging; photothermal therapy; Prussian blue; reactive oxygen species scavenger; tunable localized surface plasmon resonances;
Co-reporter:Shige Wang;Xiang Li;Yu Chen;Xiaojun Cai;Heliang Yao;Wei Gao;Yuanyi Zheng;Xiao An;Jianlin Shi
Advanced Materials 2015 Volume 27( Issue 17) pp:2775-2782
Publication Date(Web):
DOI:10.1002/adma.201500870
Co-reporter:Xiaojun Cai;Wei Gao;Ming Ma;Meiying Wu;Linlin Zhang;Yuanyi Zheng;Jianlin Shi
Advanced Materials 2015 Volume 27( Issue 41) pp:6382-6389
Publication Date(Web):
DOI:10.1002/adma.201503381
Co-reporter:Shige Wang;Yu Chen;Xiang Li;Wei Gao;Linlin Zhang;Jun Liu;Yuanyi Zheng;Jianlin Shi
Advanced Materials 2015 Volume 27( Issue 44) pp:7117-7122
Publication Date(Web):
DOI:10.1002/adma.201503869
Co-reporter:Xiaojun Cai;Xiaoqing Jia;Wei Gao;Kun Zhang;Ming Ma;Shige Wang;Yuanyi Zheng;Jianlin Shi
Advanced Functional Materials 2015 Volume 25( Issue 17) pp:2520-2529
Publication Date(Web):
DOI:10.1002/adfm.201403991
The integration of efficient imaging for diagnosis and synergistic tumor therapy into a single-component nanoplatform is much promising for high efficacy tumor treatment but still in a great challenge. Herein, a smart and versatile nanotheranostic platform based on hollow mesoporous Prussian blue nanoparticles (HMPBs) with perfluoropentane (PFP) and doxorubicin (DOX) inside, has been designed, for the first time, to achieve the distinct in vivo synergistic chemo-thermal tumor therapy and synchronous diagnosis and monitoring by ultrasound (US)/photoacoustic (PA) dual mode imaging. The prepared HMPBs show excellent photothermal conversion properties with large molar extinction coefficient (≈1.2 × 1011m−1 cm−1) and extremely high photothermal conversion efficiency (41.4%). Such a novel theranostic nanoplatform is expected to overcome the inevitable tumor recurrence and metastasis resulting from the inhomogeneous ablation of single thermal therapy, which will find a promising prospect in the application of noninvasive cancer therapy.
Co-reporter:Xiaoxia Zhou, Hangrong Chen, Guobin Zhang, Jin Wang, Zhiguo Xie, Zile Hua, Lingxia Zhang and Jianlin Shi
Journal of Materials Chemistry A 2015 vol. 3(Issue 18) pp:9745-9753
Publication Date(Web):18 Mar 2015
DOI:10.1039/C5TA00094G
A hierarchically porous zeolite beta has been designed via a facile combined surfactant-assisted hydrothermal treatment and subsequent alkali etching approach. High contents of the Cu and Mn species were then highly dispersed into the as-synthesized hierarchically porous zeolite beta. The prepared composite catalyst exhibits highly active, stable and recyclable catalytic performances for soot oxidation, and extraordinarily low T50 (260 °C) and T90 (300 °C) values can be achieved in the presence of NO. A synergetic catalytic effect between valence-varied active species Cun+ and Mnn+ has been proposed, which features the promoted generations of highly active oxygen species O−/O2− and active intermediate NO2. In addition, the obtained catalyst shows an excellent water resistance performance in soot oxidation due to the hydrophobic crystalline zeolite framework and the interaction between soot and water vapor.
Co-reporter:Jin Wang, Jinzhen Zhu, Xiaoxia Zhou, Yanyan Du, Weimin Huang, Jianjun Liu, Wenqing Zhang, Jianlin Shi and Hangrong Chen
Journal of Materials Chemistry A 2015 vol. 3(Issue 14) pp:7631-7638
Publication Date(Web):25 Feb 2015
DOI:10.1039/C5TA00468C
The efficient removal of low-concentration nitric oxide at room temperature from a semi-closed space is becoming a crucial but challenging issue in the context of increasingly serious air pollution. A novel nanoflower-like weak crystallization manganese oxide (WMO) has been synthesized via a facile and scalable strategy for low-concentration nitric oxide oxidation at room temperature. The prepared WMO shows the nanoflower-like morphology with abundant water molecules and Mn vacancies inside. Such WMO could easily adsorb NO and quickly convert it into NO2via catalytic oxidization. Herein, the weak crystallization structure and the presence of Mn vacancies are identified to be mainly responsible for the adsorption and catalytic oxidation of NO. More importantly, it shows much longer lifetime in a moist stream of simulated feed gas than that under dry conditions, which can be attributed to the relative stability of the catalyst with hydrated surfaces. Comparative DFT-calculations are performed to reveal the catalytic effect of Mn-vacancies and hydrated surfaces in reducing the reaction barriers of rate-determining steps.
Co-reporter:Xiaoqing Jia, Xiaojun Cai, Yu Chen, Shige Wang, Huixiong Xu, Kun Zhang, Ming Ma, Huixia Wu, Jianlin Shi, and Hangrong Chen
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 8) pp:4579
Publication Date(Web):February 3, 2015
DOI:10.1021/am507443p
Hollow mesoporous nanomaterials have gained tremendous attention in the fields of nanomedicine and nanobiotechnology. Herein, n-perfluoropentane (PFP)-encapsulated hollow mesoporous Prussian blue (HPB) nanocubes (HPB-PFP) with excellent colloidal stability have been synthesized for concurrent in vivo tumor diagnosis and regression. The HPB shell shows excellent photothermal conversion efficiency that can absorb near-infrared (NIR) laser light and convert it into heat. The generated heat can not only cause tumor ablation by raising the temperature of tumor tissue but also promote the continuous gasification and bubbling of encapsulated liquid PFP with low boiling point. These formed PFP bubbles can cause tissue impedance mismatch, thus apparently enhancing the signal of B-mode ultrasound imaging in vitro and generating an apparent echogenicity signal for tumor tissues of nude mice in vivo. Without showing observable in vitro and in vivo cytotoxicity, the designed biocompatible HPB-PFP nanotheranostics with high colloidal stability and photothermal efficiency are anticipated to find various biomedical applications in activated ultrasound imaging-guided tumor detection and therapy.Keywords: cancer; n-perfluoropentane; photothermal therapy; Prussian blue; ultrasound imaging
Co-reporter:Kun Zhang, Hangrong Chen, Pei Li, Xiaowan Bo, Xiaolong Li, Zeng Zeng, and Huixiong Xu
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 33) pp:18590
Publication Date(Web):August 6, 2015
DOI:10.1021/acsami.5b04999
Despite great efforts having been devoted to the design of multimodal imaging probe, almost all design principles of nanotheranostic agents subordinate to simple assemblies of building blocks, resulting in complex preparation process and discounted ability, that is, 1 + 1 < 2. In this report, a novel design strategy, marriage of structure design and composition design that can maximize imaging ability of each building block, ultimately achieving 1 + 1 ≥ 2, has been established. Moreover, a high-efficient ultrasound (US) & MR & CT trimodal contrast agent acts as model to instantiate this design strategy, wherein nanoparticles-induced nonlinear scattering and rattle-type structure-induced double scattering enhancing US imaging, and uniform distribution of Mn2+ paramagentic centers and “core–satellite” structure of Au atoms favoring enhanced MR imaging and CT imaging, respectively have been validated, achieving optimization of structure design. Importantly, the selected components, silica, Au and MnO are endowed with excellent biocompatibility, displaying the marriage strategy of composition design with aforementioned structure optimization. In in vivo evaluations, such a biocompatible trimodal probe is demonstrated of excellent performance in intensifying CT, MR and US imaging in vivo, especially after positively charged modification by PEI promoting more probes retained in tumor. More importantly, as a universal design strategy, the involved principles in constructing such a US&MR&CT trimodal imaging probe promise great potentials in guiding designs of other materials-based multimodal imaging probe.Keywords: composition & structure marriage; core−satellite; double scattering; enhanced nonlinear scattering; ultrasound & MR & CT trimodal imaging probe; uniform distribution;
Co-reporter:Yu Chen;Jianlin Shi
Advanced Healthcare Materials 2015 Volume 4( Issue 1) pp:158-165
Publication Date(Web):
DOI:10.1002/adhm.201400127
The successful cancer eradication in a noninvasive manner is the ultimate objective in the fight against cancer. As a “bloodless scalpel,” high-intensity focused ultrasound (HIFU) is regarded as one of the most promising and representative noninvasive therapeutic modalities for cancer surgery. However, large-scale clinical applications of HIFU are still in their infancy because of critical efficiency and safety issues which remain to be solved. Fortunately, recently developed nanobiotechnology provides an alternative efficient approach to improve such important issues in HIFU, especially for cancer therapy. This Research News presents the very recent exciting progresses on the elaborate design and fabrication of organic, inorganic, and organic/inorganic hybrid nanoparticles for enhancing the HIFU ablation efficiency against tumor tissues. It is highly expected that this Research News can arouse more extensive research enthusiasm on the development of functional nanomaterials for highly efficient HIFU-based synergistic therapy, which will give a promising noninvasive therapeutic modality for the successful cancer therapy with minimal damage to surrounding normal tissues, due to the noninvasive and site-specific therapeutic features of HIFU.
Co-reporter:Ming Ma;Jianlin Shi
Science Bulletin 2015 Volume 60( Issue 13) pp:1170-1183
Publication Date(Web):2015 July
DOI:10.1007/s11434-015-0829-5
Ultrasound (US) imaging in combination with US contrast agents (UCAs) is a powerful tool in the modern biomedical field because of its high spatial resolution, easy access to patients and minimum invasiveness. The microbubble-based UCAs have been widely used in clinical diagnosis; however, they are only limited to the blood pool imaging and not applicable to the tissue-penetrated imaging due to their large particle size and structural instability. Inorganic nanoparticles (NPs), such as silica, gold and FexOy, featured with both satisfactory echogenic properties and structural stability have the potential to be used as a new generation of UCAs. In this review, we present the most recent progresses in the tailored construction of inorganic UCAs and their biomedical applications in the US imaging-involved fields. Firstly, the typical inorganic NPs with different structures including solid, hollow and multiple-layer forms will be comprehensively introduced in terms of their structure design, physicochemical property, US imaging mechanism and diverse applications; secondly, the recent progress in exploring the gas-generating inorganic NP system for US imaging purpose will be reviewed, and these intelligent UCAs are multifunctional for simultaneous US imaging and disease therapy; thirdly, several nanocomposite platforms newly constructed by combining inorganic UCAs with other functional components will be presented and discussed. These multifunctional NPs are capable of further enhancing the imaging resolution by providing more comprehensive anatomical information simultaneously. Last but not the least, the design criteria for developing promising UCAs to satisfy both clinical demands and optimized US imaging capability will be discussed and summarized in this review.超声造影成像因其非侵入性、风险低、价格低和轻便快捷等优势,在肿瘤诊断方面得到了广泛的应用。伴随着分子影像技术的进步和发展,针对肿瘤的靶向超声造影剂的制备和应用成为了材料和医学界的研究热点。然而,由于粒径较大和结构稳定性差等因素,目前常用的微泡造影剂在体内循环和成像时间较短,同时难以渗透到肿瘤组织和细胞内部实现有效的肿瘤造影成像。针对以上问题,目前国际科学界开展了氧化硅、金和氧化铁等无机基质的纳米超声造影剂的制备和应用研究,力求在结构和成像性能等方面大幅度提高材料的超声造影性能。本综述主要从3个方面介绍无机纳米超声造影剂的研究进展:(1) 新型实心、空心和多壁结构无机SiO2纳米超声造影剂的制备、成像机理和诊断应用研究;(2) 新型相转变智能超声造影剂的合成和诊疗应用进展;(3) 与光声造影成像、磁性能和肿瘤靶向性能复合的几种代表性多功能超声造影剂的介绍,并着重总结目前国际上关于光热治疗和超声造影复合纳米材料的研究进展。此外,为了进一步提高无机超声造影剂的安全性和有效性,提出了材料设计和临床前研究的指导性思路。
Co-reporter:Ming Ma, Yan Huang, Hangrong Chen, Xiaoqing Jia, Shige Wang, Zizheng Wang, Jianlin Shi
Biomaterials 2015 37() pp: 447-455
Publication Date(Web):
DOI:10.1016/j.biomaterials.2014.10.001
Co-reporter:Shige Wang, Kai Li, Yu Chen, Hangrong Chen, Ming Ma, Jingwei Feng, Qinghua Zhao, Jianlin Shi
Biomaterials 2015 39() pp: 206-217
Publication Date(Web):
DOI:10.1016/j.biomaterials.2014.11.009
Co-reporter:Juan Mou, Chengbo Liu, Pei Li, Yu Chen, Huixiong Xu, Chenyang Wei, Liang Song, Jianlin Shi, Hangrong Chen
Biomaterials 2015 57() pp: 12-21
Publication Date(Web):
DOI:10.1016/j.biomaterials.2015.04.020
Co-reporter:Juan Mou;Yu Chen;Ming Ma;Kun Zhang;Chenyang Wei
Science China Materials 2015 Volume 58( Issue 4) pp:294-301
Publication Date(Web):2015 April
DOI:10.1007/s40843-015-0044-3
A kind of multifunctional perfluoropentane (PFP) and ultrasmall Cu2−xS nanodots (u-Cu2−xS NDs) co-incorporated liposome (PFP@ u-Cu2−xS NDs@liposome) nanocomposite has been facilely and successfully synthesized for enhanced ultrasound/infrared thermal/photoacoustic multimodal imaging and photothermal therapy upon near infrared (NIR) laser irradiation. Such a liposome-based nanocomposite possesses a number of advantages, such as high dispersity and stability, excellent biocompatibility, small particle size (<100 nm), well-defined core/shell structure, strong NIR absorption and photo-triggered vaporization of PFP, etc. The detailed in vitro investigations demonstrate that the as-synthesized PFP@ u-Cu2−xS NDs@ liposome nanocomposite is capable of enhancing the contrasts of ultrasound/infrared thermal/photoacoustic multimodal imaging, and substantially improving the photothermal therapeutic efficacy. This novel liposome-based theranostic nanoplatform shows great potentials in the future cancer diagnosis and therapy.包裹氟碳化合物的脂质体已被广泛用作超声成像造影剂; 而硫化铜由于具有表面等离子体共振效应在近红外区域具有强光学吸收特性, 可以同时作为一种性能优异的近红外热/光声成像造影剂和光热治疗剂. 本文以有机脂质体为载体, 同时包裹氟碳化合物和硫化铜, 在近红外激光照射下, 硫化铜吸收光能将其转化为热能, 达到氟碳化合物的相变温度时使氟碳化合物 由液态变为气态, 产生的气泡可增强超声成像造影能力, 从而构建了单一波长激光诱导的超声/近红外热/光声多模式成像引导下的光热治疗, 极大提高了癌症治疗的安全性和治疗效率. 体外实验结果表明该有机无机复合物不仅能克服单纯有机脂质体的不稳定性等缺点, 而且具有显著增强的多模式成像造影能力和优异的光热治疗效果, 具有重要的临床应用前景.
Co-reporter:Yu Chen, Hang-Rong Chen, and Jian-Lin Shi
Accounts of Chemical Research 2014 Volume 47(Issue 1) pp:125
Publication Date(Web):August 14, 2013
DOI:10.1021/ar400091e
Colloidal hollow mesoporous silica nanoparticles (HMSNs) are aspecial type of silica-based nanomaterials with penetrating mesopore channels on their shells. HMSNs exhibit unique structural characteristics useful for diverse applications: Firstly, the hollow interiors can function as reservoirs for enhanced loading of guest molecules, or as nanoreactors for the growth of nanocrystals or for catalysis in confined spaces. Secondly, the mesoporous silica shell enables the free diffusion of guest molecules through the intact shell. Thirdly, the outer silica surface is ready for chemical modifications, typically via its abundant Si–OH bonds.As early as 2003, researchers developed a soft-templating methodto prepare hollow aluminosilicate spheres with penetrating mesopores in a cubic symmetry pattern on the shells. However, adapting this method for applications on the nanoscale, especially for biomedicine, has proved difficult because the soft templating micelles are very sensitive to liquid environments, making it difficult to tune key parameters such as dispersity, morphology and structure. In this Account, we present the most recent developments in the tailored construction of highly dispersive and monosized HMSNs using simple silica-etching chemistry, and we discuss these particles’ excellent performance in diverse applications. We first introduce general principles of silica-etching chemistry for controlling the chemical composition and the structural parameters (particle size, pore size, etching modalities, yolk-shell nanostructures, etc.) of HMSNs. Secondly, we include recent progress in constructing heterogeneous, multifunctional, hollow mesoporous silica nanorattles via several methods for diverse applications. These elaborately designed HMSNs could be topologically transformed to prepare hollow mesoporous carbon nanoparticles or functionalized to produce HMSN-based composite nanomaterials. Especially in biomedicine, HMSNs are excellent as carriers to deliver either hydrophilic or hydrophobic anti-cancer drugs, to tumor cells, offering enhanced chemotherapeutic efficacy and diminished toxic side effects. Most recently, research has shown that loading one or more anticancer drugs into HMSNs can inhibit metastasis or reverse multidrug resistance of cancer cells. HMSNs could also deliver hydrophobic perfluorohexane (PFH) molecules to improve high intensity focused ultrasound (HIFU) cancer surgery by changing the tissue acoustic environment; and HMSNs could act as nanoreactors for enhanced catalytic activity and/or durability. The versatility of silica-etching chemistry, a simple but scalable synthetic methodology, offers great potential for the creation of new types of HMSN-based nanostructures in a range of applications.
Co-reporter:Yu Chen;Ling Jiang;Ronghui Wang;Ming Lu;Qunxia Zhang;Yang Zhou;Zhigang Wang;Guangming Lu;Ping Liang;Haitao Ran;Yuanyi Zheng
Advanced Materials 2014 Volume 26( Issue 44) pp:7468-7473
Publication Date(Web):
DOI:10.1002/adma.201402509
Co-reporter:Ming Ma;Huixiong Xu;Xiaoqing Jia;Kun Zhang;Qi Wang;Shuguang Zheng;Rong Wu;Minghua Yao;Xiaojun Cai;Faqi Li;Jianlin Shi
Advanced Materials 2014 Volume 26( Issue 43) pp:7378-7385
Publication Date(Web):
DOI:10.1002/adma.201402969
Co-reporter:Yu Chen;Pengfei Xu;Meiying Wu;Qingshuo Meng;Zhu Shu;Jin Wang;Lingxia Zhang;Yaping Li;Jianlin Shi
Advanced Materials 2014 Volume 26( Issue 25) pp:4294-4301
Publication Date(Web):
DOI:10.1002/adma.201400303
Co-reporter:Yu Chen;Pengfei Xu;Zhu Shu;Meiying Wu;Lianzhou Wang;Shengjian Zhang;Yuanyi Zheng;Jin Wang;Yaping Li;Jianlin Shi
Advanced Functional Materials 2014 Volume 24( Issue 28) pp:4386-4396
Publication Date(Web):
DOI:10.1002/adfm.201400221
Construction of multifunctional stimuli-responsive nanosystems intelligently responsive to inner physiological and/or external irradiations based on nanobiotechnology can enable the on-demand drug release and improved diagnostic imaging to mitigate the side-effects of anticancer drugs and enhance the diagnostic/therapeutic outcome simultaneously. Here, a triple-functional stimuli-responsive nanosystem based on the co-integration of superparamagnetic Fe3O4 and paramagnetic MnOx nanoparticles (NPs) onto exfoliated graphene oxide (GO) nanosheets by a novel and efficient double redox strategy (DRS) is reported. Aromatic anticancer drug molecules can interact with GO nanosheets through supramolecular π stacking to achieve high drug loading capacity and pH-responsive drug releasing performance. The integrated MnOx NPs can disintegrate in mild acidic and reduction environment to realize the highly efficient pH-responsive and reduction-triggered T1-weighted magnetic resonance imaging (MRI). Superparamagnetic Fe3O4 NPs can not only function as the T2-weighted contrast agents for MRI, but also response to the external magnetic field for magnetic hyperthermia against cancer. Importantly, the constructed biocompatible GO-based nanoplatform can inhibit the metastasis of cancer cells by downregulating the expression of metastasis-related proteins, and anticancer drug-loaded carrier can significantly reverse the multidrug resistance (MDR) of cancer cells.
Co-reporter:Kun Zhang, Hangrong Chen, Xiaoxia Zhou, Yun Gong, Guobin Zhang, Xia Wang, Yu Chen and Jianlin Shi
Journal of Materials Chemistry A 2014 vol. 2(Issue 5) pp:1515-1523
Publication Date(Web):15 Nov 2013
DOI:10.1039/C3TA14171C
A useful and interesting unconventional phenomenon of Pd nanoparticle formation, i.e., significantly inhibited particle growth at elevated temperatures, has been observed for the first time by growing Pd nanoparticles on a type of nonreactor, amino group-functionalized hollow mesoporous silica nanoparticles (amino-HMSNs). Such an unconventional effect is evidenced to be a competitive result between temperature-dependent coordination and reduction action of amino groups on the shell of HMSNs based on a series of experiments of probing the coordination and reduction capability of the amino groups to a Pd precursor K2PdCl6. A possible mechanism has been proposed to demonstrate and clarify the unconventional growth of Pd nanoparticles on the shell of amino-HMSNs. The as-synthesized Pd nanoparticles on the amino-HMSNs, therefore, show a tunable temperature-dependent small size range (<10 nm) and high dispersity, and can be used as efficient Heck reaction catalysts. Such a finding of unconventional particle growth effect may offer a novel protocol for particle size modulation during materials design and fabrication.
Co-reporter:Ming Ma, Shuguang Zheng, Hangrong Chen, Minghua Yao, Kun Zhang, Xiaoqing Jia, Juan Mou, Huixiong Xu, Rong Wu and Jianlin Shi
Journal of Materials Chemistry A 2014 vol. 2(Issue 35) pp:5828-5836
Publication Date(Web):24 Jun 2014
DOI:10.1039/C3TB21666G
A novel modification route integrating the copolymers of positive charged quaternary amines and polyethylene glycol (PEG) units using a combination of reversible addition–fragmentation chain-transfer polymerization (RAFT) and “Graft From” strategy, has been proposed and developed, for the first time, to decorate the surface of mesoporous silica nanoparticles (MSNs). These MSNs are shown to have a greatly reduced hydrodynamic particle size in physiological solution. It is demonstrated that such an efficient copolymer surface modification strategy, resulting in PEG coating with high positive zeta potential, can achieve a nearly 2-fold enhanced permeability and retention (EPR) effect, and longer blood half-life compared to coating with PEG only. Besides, the in vivo results demonstrated that this surface modification strategy could lead to a higher efficacy of doxorubicin (DOX) drug delivery and greater suppression of side effects compared to the free drug. Based on this novel strategy of combining “RAFT” and “Graft From” polymerization, it is anticipated that this efficient modification of tumor-specific targeting of MSNs can be widely used in future nanomedicine research.
Co-reporter:Jinjin Zhao, Wenna Wang, Lingxia Zhang, Xiangzhi Cui, Yan Zhu, Wei Wu, Hangrong Chen and Jianlin Shi
Dalton Transactions 2014 vol. 43(Issue 2) pp:406-409
Publication Date(Web):09 Oct 2013
DOI:10.1039/C3DT52623B
Superparamagnetic mesoporous zeolite microspheres with a large mesopore size of 13 nm and a high surface area of 382 m2 g−1 were synthesized for the capacious enrichment of proteins and enzymes. A high degree of ovalbumin immobilization was obtained (491 mg g−1) at pH 6, which is nearly twice that previously reported in the literature.
Co-reporter:Yu Chen, Hangrong Chen, and Jianlin Shi
Molecular Pharmaceutics 2014 Volume 11(Issue 8) pp:2495-2510
Publication Date(Web):November 13, 2013
DOI:10.1021/mp400596v
Biocompatible inorganic material-based nanosystems provide a novel choice to effectively circumvent the intrinsic drawbacks of traditional organic materials in biomedical applications, especially in overcoming the multidrug resistance (MDR) of cancer cells due to their unique structural and compositional characteristics, for example, high stability, large surface area, tunable compositions, abundant physicochemical multifunctionalities, and specific biological behaviors. In this review, we focus on the recent developments in the construction of inorganic nanoparticles-based drug codelivery nanosystems (mesoporous SiO2, Fe3O4, Au, Ag, quantum dots, carbon nanotubes, graphene oxide, LDH, etc.) to efficiently circumvent the MDR of cancer cells, including the well-known codelivery of small molecular anticancer drug/macromolecular therapeutic gene and codelivery of small molecular chemosensitizer/anticancer drug, and very recently explored codelivery of targeting ligands/anticancer drug, codelivery of energy/anticancer drug, and codelivery of contrast agent for diagnostic imaging and anticancer drug. The unsolved issues, future developments, and potential clinical translations of these codelivery nanosystems are also discussed. These elaborately designed biocompatible inorganic materials-based nanosystems offer an unprecedented opportunity and show the encouraging bright future for overcoming the MDR of tumors in clinic personalized medicine and the pharmaceutical industry.Keywords: cancer; codelivery; inorganic nanoparticles; multidrug resistance; nanotechnology;
Co-reporter:Kun Zhang, Hangrong Chen, Faqi Li, Qi Wang, Shuguang Zheng, Huixiong Xu, Ming Ma, Xiaoqing Jia, Yu Chen, Juan Mou, Xia Wang, Jianlin Shi
Biomaterials 2014 35(22) pp: 5875-5885
Publication Date(Web):
DOI:10.1016/j.biomaterials.2014.03.043
Co-reporter:Yu Chen;Pengfei Xu;Yongsheng Li;Wenbo Bu;Zhu Shu;Yaping Li;Jiamin Zhang;Lingxia Zhang;Limin Pan;Xiangzhi Cui;Zile Hua;Jin Wang;Linlin Zhang;Jianlin Shi
Advanced Materials 2013 Volume 25( Issue 22) pp:3100-3105
Publication Date(Web):
DOI:10.1002/adma.201204685
Co-reporter:Yu Chen;Pengfei Xu;Yongsheng Li;Wenbo Bu;Zhu Shu;Yaping Li;Jiamin Zhang;Lingxia Zhang;Limin Pan;Xiangzhi Cui;Zile Hua;Jin Wang;Linlin Zhang;Jianlin Shi
Advanced Materials 2013 Volume 25( Issue 22) pp:
Publication Date(Web):
DOI:10.1002/adma.201370144
Co-reporter:Yu Chen;Jianlin Shi
Advanced Materials 2013 Volume 25( Issue 23) pp:3144-3176
Publication Date(Web):
DOI:10.1002/adma.201205292
Abstract
The remarkable progress of nanotechnology and its application in biomedicine have greatly expanded the ranges and types of biomaterials from traditional organic material-based nanoparticles (NPs) to inorganic biomaterials or organic/inorganic hybrid nanocomposites due to the unprecedented advantages of the engineered inorganic material-based NPs. Colloidal mesoporous silica NPs (MSNs), one of the most representative and well-established inorganic materials, have been promoted into biology and medicine, and shifted from extensive in vitro research towards preliminary in vivo assays in small-animal disease models. In this comprehensive review, the recent progresses in chemical design and engineering of MSNs-based biomaterials for in vivo biomedical applications has been detailed and overviewed. Due to the intrinsic structural characteristics of elaborately designed MSNs such as large surface area, high pore volume and easy chemical functionalization, they have been extensively investigated for therapeutic, diagnostic and theranostic (concurrent diagnosis and therapy) purposes, especially in oncology. Systematic in vivo bio-safety evaluations of MSNs have revealed the evidences that the in vivo bio-behaviors of MSNs are strongly related to their preparation prodecures, particle sizes, geometries, surface chemistries, dosing parameters and even administration routes. In vivo pharmacokinetics and pharmacodynamics further demonstrated the effectiveness of MSNs as the passively and/or actively targeted drug delivery systems (DDSs) for cancer chemotherapy. Especially, the advance of nano-synthetic chemistry enables the production of composite MSNs for advanced in vivo therapeutic purposes such as gene delivery, stimuli-responsive drug release, photothermal therapy, photodynamic therapy, ultrasound therapy, or anti-bacteria in tissue engineering, or as the contrast agents for biological and diagnostic imaging. Additionally, the critical issues and potential challenges related to the chemical design/synthesis of MSNs-based “magic bullet” by advanced nano-synthetic chemistry and in vivo evaluation have been discussed to highlight the issues scientists face in promoting the translation of MSNs-based DDSs into clinical trials.
Co-reporter:Xiaoxia Zhou, Xiangzhi Cui, Hangrong Chen, Yan Zhu, Yudian Song and Jianlin Shi
Dalton Transactions 2013 vol. 42(Issue 4) pp:890-893
Publication Date(Web):13 Nov 2012
DOI:10.1039/C2DT32144K
The hierarchically porous and iron-functionalized zeolite ZSM-5 has been fabricated as a Fenton photocatalyst by a facile post-treatment process, which exhibits an excellent visible-light catalytic property in the adsorption/degradation of organic pollutants under mild reaction conditions.
Co-reporter:Yun Gong, Hangrong Chen, Qianjun He, Jianlin Shi, Lianjun Wang, Wan Jiang
Ceramics International 2013 Volume 39(Issue 8) pp:8865-8868
Publication Date(Web):December 2013
DOI:10.1016/j.ceramint.2013.04.079
Abstract
A novel upconversion luminescence transparent glass has been successfully synthesized from Er3+/Yb3+ co-doped zeolite powder by Spark Plasma Sintering (SPS) method through the order–disorder transition process. XRD was used to detect the order–disorder transition process of each phase after SPS. These zeolite-derived silica glasses showed enhanced upconversion luminescence under the excitation of 980 nm diode laser, which was caused by the change of phonon energy according to the results of Raman spectrum, and the corresponding energy transfer mechanism was also discussed in detail.
Co-reporter:Yun Gong, Hangrong Chen, Yu Chen, Xiangzhi Cui, Yan Zhu, Xiaoxia Zhou, Jianlin Shi
Microporous and Mesoporous Materials 2013 Volume 173() pp:112-120
Publication Date(Web):June 2013
DOI:10.1016/j.micromeso.2013.02.013
A novel Cu/Mn co-loaded mesoporous ZrO2–TiO2 (ZT) composite has been successfully synthesized, in which Cu species were first introduced by co-hydrolysis of copper precursor with zirconium and titanium precursors, following on loading with Mn species via an in situ redox reaction between KMnO4 and the surfactant template. The prepared samples were characterized by XRD, N2 sorption, TEM, SEM, H2-TPR, UV–vis and XPS techniques, etc. CO catalytic oxidation was chosen as a model reaction to investigate the distinctively synergetic catalytic effect in the prepared co-loaded sample. Compared with single component of Cu or Mn loaded samples, the co-loaded CuMnZT demonstrated much enhanced catalytic activity at the Cu content of ⩾2.2 wt%. A possible synergetic catalytic effect among the Cu, Mn species and mesoporous ZrO2–TiO2 matrix was proposed and discussed in detail.Graphical abstractA novel two-step successional loading approach was firstly developed to synthesize a Cu/Mn co-loaded mesoporous ZrO2–TiO2 composite, which demonstrated a remarkably synergetic catalytic effect among Cu, Mn species and mesoporous ZrO2–TiO2 matrix towards CO oxidation.Highlights► Mesoporous CuMn/ZT was synthesized by a novel two-step successional loading approach. ► Cu species was incorporated into ZT framework and enhanced the chemical stability. ► Mn species can be homogeneously dispersed into the mesoporous channels of ZT. ► Cu/Mn co-loaded mesoporous ZrO2–TiO2 catalysts show enhanced CO oxidation activity. ► A synergetic catalytic effect among Cu, Mn species and ZT matrix was proposed.
Co-reporter:Dr. Xiaoxia Zhou; Hangrong Chen;Dr. Yan Zhu;Yudian Song;Dr. Yu Chen;Dr. Yongxia Wang;Dr. Yun Gong;Dr. Guobin Zhang;Dr. Zhu Shu;Dr. Xiangzhi Cui;Dr. Jinjin Zhao; Jianlin Shi
Chemistry - A European Journal 2013 Volume 19( Issue 30) pp:10017-10023
Publication Date(Web):
DOI:10.1002/chem.201300245
Abstract
Dual-mesoporous ZSM-5 zeolite with highly b axis oriented large mesopores was synthesized by using nonionic copolymer F127 and cationic surfactant CTAB as co-templates. The product contains two types of mesopores—smaller wormlike ones of 3.3 nm in size and highly oriented larger ones of 30–50 nm in diameter along the b axis—and both of them interpenetrate throughout the zeolite crystals and interconnect with zeolite microporosity. The dual-mesoporous zeolite exhibits excellent catalytic performance in the condensation of benzaldehyde with ethanol and greater than 99 % selectivity for benzoin ethyl ether at room temperature, which can be ascribed to the zeolite lattice structure offering catalytically active sites and the hierarchical and oriented mesoporous structure providing fast access of reactants to these sites in the catalytic reaction. The excellent recyclability and high catalytic stability of the catalyst suggest prospective applications of such unique mesoporous zeolites in the chemical industry.
Co-reporter:Xia Wang, Hangrong Chen, Yuanyi Zheng, Ming Ma, Yu Chen, Kun Zhang, Deping Zeng, Jianlin Shi
Biomaterials 2013 34(8) pp: 2057-2068
Publication Date(Web):
DOI:10.1016/j.biomaterials.2012.11.044
Co-reporter:Xia Wang;Yu Chen;Ming Ma;Kun Zhang;Faqi Li;Yuanyi Zheng;Deping Zeng;Qi Wang;Jianlin Shi
Advanced Materials 2012 Volume 24( Issue 6) pp:785-791
Publication Date(Web):
DOI:10.1002/adma.201104033
Co-reporter:Yu Chen;Yu Gao;Deping Zeng;Yaping Li;Yuanyi Zheng;Faqi Li;Xiufeng Ji;Xia Wang;Feng Chen;Qianjun He;Linlin Zhang;Jianlin Shi
Advanced Functional Materials 2012 Volume 22( Issue 8) pp:1586-1597
Publication Date(Web):
DOI:10.1002/adfm.201102052
Abstract
A novel drug-formulation protocol is developed to solve the delivery problem of hydrophobic drug molecules by using inorganic mesoporous silica nanocapsules (IMNCs) as an alternative to traditional organic emulsions and liposomes while preserving the advantages of inorganic materials. The unique structures of IMNCs are engineered by a novel fluoride-silica chemistry based on a structural difference-based selective etching strategy. The prepared IMNCs combine the functions of organic nanoemulsions or nanoliposomes with the properties of inorganic materials. Various spherical nanostructures can be fabricated simply by varying the synthetic parameters. The drug loading amount of a typical highly hydrophobic anticancer drug-camptothecin (CPT) in IMNCs reaches as high as 35.1 wt%. The intracellular release of CPT from carriers is demonstrated in situ. In addition, IMNCs can play the role of organic nanoliposome (multivesicular liposome) in co-encapsulating and co-delivering hydrophobic (CPT) and hydrophilic (doxorubicin, DOX) anticancer drugs simultaneously. The co-delivery of multi-drugs in the same carrier and the intracellular release of the drug combinations enables a drug delivery system with efficient enhanced chemotherapeutic effect for DOX-resistant MCF-7/ADR cancer cells. The special IMNCs-based “inorganic nanoemulsion”, as a proof-of-concept, can also be employed successfully to encapsulate and deliver biocompatible hydrophobic perfluorohexane (PFH) molecules for high intensity focused ultrasound (HIFU) synergistic therapy ex vivo and in vivo. Based on this novel design strategy, a wide range of inorganic material systems with similar “inorganic nanoemulsion or nanoliposome” functions will be developed to satisfy varied clinical requirements.
Co-reporter:Kun Zhang, Hangrong Chen, Yuanyi Zheng, Yu Chen, Ming Ma, Xia Wang, Lijun Wang, Deping Zeng and Jianlin Shi
Journal of Materials Chemistry A 2012 vol. 22(Issue 25) pp:12553-12561
Publication Date(Web):26 Apr 2012
DOI:10.1039/C2JM31504A
A novel and general in situ hydrophobic shell-protected selective etching strategy has been developed to synchronously synthesize and modify hollow mesoporous silica nanoparticles (HMSNs) and rattle-type mesoporous silica nanoparticles (RMSNs) with well-defined morphology, effectively avoiding the drawbacks of post-modification. The key point of the strategy lies in the hydrophilicity differences between the pure silica inner core and the organic hybrid silica shell, which results in the preferential etching of the pure silica inner core. Except that amino group functionalized HMSNs (amino-HMSNs) can be synthesized via this strategy, it can be readily applied for the synthesis of HMSNs and RMSNs synchronously grafted with different kinds of functional groups by employing other silane coupling agents, directly indicating the generality of this strategy. Furthermore, adding no additional reduction agents, the amino-HMSNs can be regarded as nanoreactors, and a distinctively heterogeneous rattle-type structure, Au@HMSN/Au, with an entrapped size-tunable Au nanoparticle and some small Au nanocrystals embedded in the hollow cavity and shell of each nanoparticle, respectively, is obtained. As hybrid ultrasound contrast agents (UCAs), unlike micro-sized organic UCAs merely confined to blood pool imaging, the as-synthesized nano-sized amino-HMSNs can achieve excellent in vitro ultrasound imaging, and potentially be applied in cell-level imaging. More importantly, relying on the process merits of our strategy, such as the doping of silane coupling agents and no calcination treatment, amino-HMSNs exhibit enhanced ultrasound imaging to some certain extent compared to the calcined ones.
Co-reporter:Ming Ma, Hangrong Chen, Yu Chen, Kun Zhang, Xia Wang, Xiangzhi Cui and Jianlin Shi
Journal of Materials Chemistry A 2012 vol. 22(Issue 12) pp:5615-5621
Publication Date(Web):10 Feb 2012
DOI:10.1039/C2JM15489G
Hyaluronic acid-conjugated mesoporous silica nanoparticles (MSNs-HA) have been synthesized via a facile amidation reaction. This novel strategy can efficiently solve the agglomeration problem of MSNs in physiological fluids. The cellular experiments showed that MSNs-HA is capable of selectively targeting specific cancer cells over-expressing the CD44 protein, leading to rapid and concentration-dependent uptake by the cancer cells through the receptor-mediated endocytosis mechanism. In contrast, no selective targeting of MSNs-HA can be found to the CD44 low-expressing cells, such as MCF-7 and L929 cells. The hydrophobic camptothecin (CPT) drug was encapsulated into MSNs-HA, which showed enhanced cytotoxicity to the Hela cells compared to both free CPT and CPT-loaded MSNs-HA in the presence of excess free HA.
Co-reporter:Yu Chen, Qi Yin, Xiufeng Ji, Shengjian Zhang, Hangrong Chen, Yuanyi Zheng, Yang Sun, Haiyun Qu, Zheng Wang, Yaping Li, Xia Wang, Kun Zhang, Linlin Zhang, Jianlin Shi
Biomaterials 2012 33(29) pp: 7126-7137
Publication Date(Web):
DOI:10.1016/j.biomaterials.2012.06.059
Co-reporter:Yu Chen, Hangrong Chen, Shengjian Zhang, Feng Chen, Shikuan Sun, Qianjun He, Ming Ma, Xia Wang, Huixia Wu, Lingxia Zhang, Linlin Zhang, Jianlin Shi
Biomaterials 2012 33(7) pp: 2388-2398
Publication Date(Web):
DOI:10.1016/j.biomaterials.2011.11.086
Co-reporter:Ming Ma, Hangrong Chen, Yu Chen, Xia Wang, Feng Chen, Xiangzhi Cui, Jianlin Shi
Biomaterials 2012 33(3) pp: 989-998
Publication Date(Web):
DOI:10.1016/j.biomaterials.2011.10.017
Co-reporter:Yu Chen;Shengjian Zhang;Feng Chen;Lingxia Zhang;Jiamin Zhang;Min Zhu;Huixia Wu;Limin Guo;Jingwei Feng;Jianlin Shi
Advanced Functional Materials 2011 Volume 21( Issue 2) pp:270-278
Publication Date(Web):
DOI:10.1002/adfm.201001495
Abstract
A general polyelectrolyte-mediated self-assembly technique is adopted to prepare multifunctional mesoporous nanostructures as an effective biological bimodal imaging probe and magnetically targeted anticancer drug (doxorubicin) delivery systems (DDSs). A positively charged polyelectrolyte (PAH) and negatively charged fluorescent quantum dots (QDs) are successfully assembled onto the surface of ellipsoidal Fe3O4@SiO2@mSiO2 composite nanostructures to combine the merits of tunable fluorescent/magnetic properties, mesoporous nanostructures for drug loading, and the uniform ellipsoidal morphology for enhanced uptake by cancer cells. The resultant nanoellipsoids are homogeneously coated with four layers of PAH/QDs, with an additional PAH layer to make the ellipsoidal surface positively charged. This acts to enhance cellular uptake, which is driven by electrostatic interactions between the positive nanoparticle surface and the negative cell surface. The high biocompatibility of the achieved multifunctional nanoellipsoids is demonstrated by a cell-cytotoxicity assay, hemolyticity against human red blood cells, and coagulation evaluation of fresh human blood plasma after exposure to the nanoparticles. Moreover, confocal microscopy and bio-TEM observations show that the cell uptake of nanocarriers is dose-dependent, and the nanoparticles accumulate mostly in the cytoplasm. The excellent capability of the nanocarriers as contrast agents for MRI is demonstrated by the relatively high r2 value (143 mM−1s−1) and preliminary in vivo characterization. More importantly, the doxorubicin-loaded DDSs show higher cytotoxicity than the free doxorubicin drug as contributed by the intracellular release pathway of doxorubicin from the DDSs, indicating the potential application of the obtained multifunctional mesoporous nanoellipsoids as highly effective bimodal imaging probes and DDSs for cancer diagnosis and chemotherapy, simultaneously.
Co-reporter:Yu Chen, Hangrong Chen, Ming Ma, Feng Chen, Limin Guo, Lingxia Zhang and Jianlin Shi
Journal of Materials Chemistry A 2011 vol. 21(Issue 14) pp:5290-5298
Publication Date(Web):22 Feb 2011
DOI:10.1039/C0JM04024J
A general electrostatic interaction-based self-assembly strategy has been developed to synthesize various composite nanostructures with double mesoporous silica shells. The outer (second) mesoporous silica shell was coated on the surface of an inner (first) mesoporous silica nanostructure (nanosphere or nanolayer), which was templated by silane coupling agent (C18TMS), according to an electrostatic interaction mechanism between the negatively charged surface of inner mesoporous silica shell/sphere and positively charged cationic surfactant (C16TAB) for directing the second shell. The two adjacent shells directed by different pore-making agents show hierarchical pore size distributions and diverse pore structure orderings. This general strategy can be extended to synthesize a series of novel double-shelled mesoporous nanostructures with various morphologies, compositions and structures by altering the structural designing scheme in nanoscale (seven novel nanostructures created in this work). Importantly, the deposition of the second mesoporous shell on the surface of initial mesoporous nanostructures significantly increases the surface areas and pore volumes of as-prepared materials, which provides an alternative and versatile post-treatment approach to tune the key structural parameters of mesoporous nanomaterials. The double shelled hollow mesoporous silica spheres were found to be highly biocompatible, and were explored as both hydrophilic and hydrophobic anticancer drug delivery vehicles against cancer cells. The results show that the deposition of a second mesoporous silica shell could lead to a sustained release of a hydrophilic anticancer drug (irinotecan) from the carriers, and moreover, the double shelled mesoporous silica spheres exhibit high hydrophobic anticancer drug (docetaxel) loading capacity (15.24%), large amount uptake by cancer cells and enhanced anticancer efficiency, indicating the potential applications of synthesized nanoparticles in nanomedicine for cancer chemotherapy.
Co-reporter:Hangrong Chen, Zhengqing Ye, Xiangzhi Cui, Jianlin Shi, Dongsheng Yan
Microporous and Mesoporous Materials 2011 Volume 143(2–3) pp:368-374
Publication Date(Web):September 2011
DOI:10.1016/j.micromeso.2011.03.021
A polycopolymer-assisted self-assembly process under hydrothermal condition has been developed for preparing mesostructured alumina–ceria–zirconia tri-component nanocomposite. This composite showed a uniform worm-like mesoporous structure with nanocrystallite framework, sharp pore-size distribution, high surface area (>180 m2/g), high thermal stability (>1000 °C) and excellent oxygen storage capacity (OSC). Small amounts of precious metals can be homogeneously loaded into the worm-like pore structure, which could maintain their high dispersity even when calcined at 1000 °C. Such a nanocomposite catalyst showed high performance for the three-way exhaust catalytic conversion with low ignition temperatures at engine start-up and high thermal stability against aging.Graphical abstractA mesostructured alumina–ceria–zirconia tri-component nanocomposite of uniform worm-like meoporous structure with high thermal stability and excellent oxygen storage capacity (OSC) has been synthesized. Small amounts of precious metals can be homogeneously loaded into the worm-like pore structure, which could maintain their high dispersity even when calcined at 1000 °C..Highlights► Mesostructured Al2O3–CeO2–ZrO2 tricomponent nanocomposite has been synthesized. ► This nanocomposite has uniform worm-like mesopores and high thermal stability. ► Alumina doping greatly enhances the oxygen storage/release capacity. ► Noble metals can be homogeneously loaded into the worm-like pore structure. ► Noble metal nanoparticles can maintain their high dispersity even at 1000 °C.
Co-reporter:Nan Wang;Yu Chen;Zhengqing Ye;Jianlin Shi
Chinese Journal of Chemistry 2011 Volume 29( Issue 3) pp:483-488
Publication Date(Web):
DOI:10.1002/cjoc.201190109
Abstract
Alumina doping and sulfation in hierarchically porous zirconia solid acids have been achieved simultaneously via one-pot and bi-surfactant-assisted self-assembly process, using aluminum sulfate as both Al and SO42− sources. The prepared composite solid acids showed much enhanced acidity and recycling catalytic activity for an esterification reaction compared with sulfated zirconia without alumina doping and Al-doped sulfated zirconia without hierarchically porous structure.
Co-reporter:Dr. Yu Chen;Dr. Hangrong Chen;Dr. Yang Sun;Dr. Yuanyi Zheng;Dr. Deping Zeng;Dr. Faqi Li;Dr. Shengjian Zhang;Dr. Xia Wang;Dr. Kun Zhang;Dr. Ming Ma;Dr. Qianjun He;Dr. Linlin Zhang;Dr. Jianlin Shi
Angewandte Chemie International Edition 2011 Volume 50( Issue 52) pp:12505-12509
Publication Date(Web):
DOI:10.1002/anie.201106180
Co-reporter:Jiaqi Li, Fangming Cui, Feng Chen, Hangrong Chen, Jianlin Shi
Materials Letters 2010 Volume 64(Issue 14) pp:1626-1629
Publication Date(Web):31 July 2010
DOI:10.1016/j.matlet.2010.03.071
An in-situ reduction method is adopted to incorporate MnO2 nanoparticles into mesochannels of silica thin films by using KMnO4 as the oxidizing agent and manganese precursor. As the reduction time in KMnO4 solution increases, the ordered mesostructure collapses, and the loaded MnO2 nanoparticles become bigger in size, resulting in a narrower band gap. Z scan measurement demonstrates a large third-order nonlinear susceptibility of the composite films under the picosecond Nd:YAG laser excitation. A sign reversion of the third-order nonlinear refractive index coefficient in the sample with longer reduction time is also observed, which can be attributed to the variation in the band gap energy.
Co-reporter:Yu Chen, Hangrong Chen, Limin Guo, Qianjun He, Feng Chen, Jian Zhou, Jingwei Feng and Jianlin Shi
ACS Nano 2010 Volume 4(Issue 1) pp:529
Publication Date(Web):December 30, 2009
DOI:10.1021/nn901398j
A novel “structural difference-based selective etching” strategy has been developed to fabricate hollow/rattle-type mesoporous nanostructures, which was achieved by making use of the structural differences, rather than traditional compositional differences, between the core and the shell of a silica core/mesoporous silica shell structure to create hollow interiors. Highly dispersed hollow mesoporous silica spheres with controllable particle/pore sizes could be synthesized by this method, which show high loading capacity (1222 mg/g) for anticancer drug (doxorubicin). Hemolyticity and cytotoxicity assays of hollow mesoporous silica spheres were conducted, and the synthesized hollow mesoporous silica spheres with large pores show ultrafast immobilization of protein-based biomolecules (hemoglobin). On the basis of this strategy, different kinds of heterogeneous rattle-type nanostructures with inorganic nanocrystals, such as Au, Fe2O3, and Fe3O4 nanoparticles, as the core and mesoporous silica as the shell were also prepared. This strategy could be extended as a general approach to synthesize various hollow/rattle-type nanostructures by creating adequate structural differences between cores and shells in core/shell structures in nanoscale.Keywords: heterogeneous structure; hollow mesoporous silica; homogeneous templating; rattle structure; selective etching; structural difference
Co-reporter:Yu Chen, Hangrong Chen, Deping Zeng, Yunbo Tian, Feng Chen, Jingwei Feng, and Jianlin Shi
ACS Nano 2010 Volume 4(Issue 10) pp:6001
Publication Date(Web):September 3, 2010
DOI:10.1021/nn1015117
A potential platform for simultaneous anticancer drug delivery and MRI cell imaging has been demonstrated by uniform hollow inorganic core/shell structured multifunctional mesoporous nanocapsules, which are composed of functional inorganic (Fe3O4, Au, etc.) nanocrystals as cores, a thin mesoporous silica shell, and a huge cavity in between. The synthetic strategy for the creation of huge cavities between functional core and mesoporous silica shell is based on a structural difference based selective etching method, by which solid silica middle layer of Fe2O3@SiO2@mSiO2 (or Au@SiO2@mSiO2) composite nanostructures was selectively etched away while the mesoporous silica shell could be kept relatively intact. The excellent biocompatibility of obtained multifunctional nanocapsules (Fe3O4@mSiO2) was demonstrated by very low cytotoxicity against various cell lines, low hemolyticity against human blood red cells and no significant coagulation effect against blood plasma. The cancer cell uptake and intracellular location of the nanocapsules were observed by confocal laser scanning microscopy and bio-TEM. Importantly, the prepared multifunctional inorganic mesoporous nanocapsules show both high loading capacity (20%) and efficiency (up to 100%) for doxorubicin simultaneously because of the formation of the cavity, enhanced surface area/pore volume and the electrostatic interaction between DOX molecules and mesoporous silica surface. Besides, the capability of Fe3O4@mSiO2 nanocapsules as contrast agents of MRI was demonstrated both in vitro and in vivo, indicating the simultaneous imaging and therapeutic multifunctionalities of the composite nanocapsules. Moreover, the concept of multifunctional inorganic nanocapsules was extended to design and prepare Gd−Si−DTPA grafted Au@mSiO2 nanocapsules for nanomedical applications, further demonstrating the generality of this strategy for the preparation of various multifunctional mesoporous nanocapsules.Keywords: Au; drug delivery; Fe3O4; mesoporous silica; MRI; nanocapsules
Co-reporter:Jinjin Zhao, Jian Zhou, Yu Chen, Qianjun He, Meiling Ruan, Limin Guo, Jianlin Shi and Hangrong Chen
Journal of Materials Chemistry A 2009 vol. 19(Issue 41) pp:7614-7616
Publication Date(Web):16 Sep 2009
DOI:10.1039/B916862A
Mesoporous microspheres of zeolite have been fabricated through direct self-assembly between an aluminosilicate precursor, tetrapropylammonium hydroxide (TPAOH) and poly(methyl methacrylate) (PMMA) nanospheres, where the PMMA nanospheres act as dual-functional templates for the generation of both mesoporosity and spherical morphology.
Co-reporter:Jinjin Zhao, Zile Hua, Zhicheng Liu, Yongsheng Li, Limin Guo, Wenbo Bu, Xiangzhi Cui, Meiling Ruan, Hangrong Chen and Jianlin Shi
Chemical Communications 2009 (Issue 48) pp:7578-7580
Publication Date(Web):10 Nov 2009
DOI:10.1039/B913920F
We report the direct fabrication of mesoporous zeolite with a hollow spherical/ellipsoidal capsule structure by using conventional TPAOH and CTAB as soft micro- and mesopore generating templates; the mesoporous zeolite shows a high surface area of 717 m2 g−1 and small mesopore size of around 3 nm.
Co-reporter:Kun Zhang, Pei Li, Yaping He, Xiaowan Bo, Xiaolong Li, Dandan Li, Hangrong Chen, Huixiong Xu
Biomaterials (August 2016) Volume 99() pp:34-46
Publication Date(Web):August 2016
DOI:10.1016/j.biomaterials.2016.05.014
Co-reporter:Kun Zhang, Pei Li, Yaping He, Xiaowan Bo, Xiaolong Li, Dandan Li, Hangrong Chen, Huixiong Xu
Biomaterials (August 2016) Volume 99() pp:34-46
Publication Date(Web):August 2016
DOI:10.1016/j.biomaterials.2016.05.014
Despite gaining increasing attention, chelation of multiple active targeting ligands greatly increase the formation probability of protein corona, disabling active targeting. To overcome it, a synergistic retention strategy of RGD-mediated active targeting and radiofrequency (RF) electromagnetic field-enhanced permeability has been proposed here. It is validated that such a special synergistic retention strategy can promote more poly lactic-co-glycolic acid (PLGA)-based capsules encapsulating camptothecin (CPT) and solid DL-menthol (DLM) to enter and retain in tumor in vitro and in vivo upon exposure to RF irradiation, receiving an above 8 fold enhancement in HeLa retention. Moreover, the PLGA-based capsules can respond RF field to trigger the entrapped DLM to generate solid-liquid-gas (SLG) tri-phase transformation for enhancing RF ablation and CPT release. Therefore, depending on the enhanced RF ablation and released CPT and the validated synergistic retention effect, the inhibitory outcome for tumor growth has gained an over 10-fold improvement, realizing RF ablation & chemotherapy synergistic treatment against HeLa solid tumor, which indicates a significant promise in clinical RF ablation.
Co-reporter:Juan Mou, Tianquan Lin, Fuqiang Huang, Hangrong Chen, Jianlin Shi
Biomaterials (April 2016) Volume 84() pp:13-24
Publication Date(Web):April 2016
DOI:10.1016/j.biomaterials.2016.01.009
Substantially different from traditional combinatorial-treatment of photothermal therapy (PTT) and photodynamic therapy (PDT) by using multi-component nanocomposite under excitation of separate wavelength, a novel single near infrared (NIR) laser-induced multifunctional theranostic nanoplatform has been rationally and successfully constructed by a single component black titania (B–TiO2−x) for effective imaging-guided cancer therapy for the first time. This multifunctional PEGylated B–TiO2−x shows high dispersity/stability in aqueous solution, excellent hemo/histocompatibility and broad absorption ranging from NIR to ultraviolet (UV). Both in vitro and in vivo results well demonstrated that such a novel multifunctional theranostic nanoplaform could achieve high therapeutic efficacy of simultaneous and synergistic PTT/PDT under the guidance of infrared thermal/photoacoustic (PA) dual-modal imaging, which was triggered by a single NIR laser. This research circumvents the conventional obstacles of using multi-component nanocomposites, UV light and high laser power density. Furthermore, negligible side effects to blood and main tissues could be found in 3 months' investigation, facilitating its potential biomedical application.A novel single near infrared (NIR) laser-induced multifunctional theranostic nanoplatform based on single component black titania (B–TiO2−x) has been successfully constructed for in vivo effective dual–modal imaging-guided cancer therapy for the first time. This highly biocompatible B–TiO2−x with PEGylation shows broad optical absorption property ranging from NIR to ultraviolet (UV), and has been demonstrated both in vitro and in vivo, to be capable of serving as a new multifunctional theranostic nanoplatform for infrared thermal/photoacousitc (PA) dual-modal imaging-guided simultaneous photothermal therapy (PTT) and photodynamic therapy (PDT), upon a single NIR laser irradiation.
Co-reporter:Juan Mou, Tianquan Lin, Fuqiang Huang, Hangrong Chen, Jianlin Shi
Biomaterials (April 2016) Volume 84() pp:13-24
Publication Date(Web):April 2016
DOI:10.1016/j.biomaterials.2016.01.009
Co-reporter:Yu Chen, Hangrong Chen, Ming Ma, Feng Chen, Limin Guo, Lingxia Zhang and Jianlin Shi
Journal of Materials Chemistry A 2011 - vol. 21(Issue 14) pp:NaN5298-5298
Publication Date(Web):2011/02/22
DOI:10.1039/C0JM04024J
A general electrostatic interaction-based self-assembly strategy has been developed to synthesize various composite nanostructures with double mesoporous silica shells. The outer (second) mesoporous silica shell was coated on the surface of an inner (first) mesoporous silica nanostructure (nanosphere or nanolayer), which was templated by silane coupling agent (C18TMS), according to an electrostatic interaction mechanism between the negatively charged surface of inner mesoporous silica shell/sphere and positively charged cationic surfactant (C16TAB) for directing the second shell. The two adjacent shells directed by different pore-making agents show hierarchical pore size distributions and diverse pore structure orderings. This general strategy can be extended to synthesize a series of novel double-shelled mesoporous nanostructures with various morphologies, compositions and structures by altering the structural designing scheme in nanoscale (seven novel nanostructures created in this work). Importantly, the deposition of the second mesoporous shell on the surface of initial mesoporous nanostructures significantly increases the surface areas and pore volumes of as-prepared materials, which provides an alternative and versatile post-treatment approach to tune the key structural parameters of mesoporous nanomaterials. The double shelled hollow mesoporous silica spheres were found to be highly biocompatible, and were explored as both hydrophilic and hydrophobic anticancer drug delivery vehicles against cancer cells. The results show that the deposition of a second mesoporous silica shell could lead to a sustained release of a hydrophilic anticancer drug (irinotecan) from the carriers, and moreover, the double shelled mesoporous silica spheres exhibit high hydrophobic anticancer drug (docetaxel) loading capacity (15.24%), large amount uptake by cancer cells and enhanced anticancer efficiency, indicating the potential applications of synthesized nanoparticles in nanomedicine for cancer chemotherapy.
Co-reporter:Ming Ma, Hangrong Chen, Yu Chen, Kun Zhang, Xia Wang, Xiangzhi Cui and Jianlin Shi
Journal of Materials Chemistry A 2012 - vol. 22(Issue 12) pp:NaN5621-5621
Publication Date(Web):2012/02/10
DOI:10.1039/C2JM15489G
Hyaluronic acid-conjugated mesoporous silica nanoparticles (MSNs-HA) have been synthesized via a facile amidation reaction. This novel strategy can efficiently solve the agglomeration problem of MSNs in physiological fluids. The cellular experiments showed that MSNs-HA is capable of selectively targeting specific cancer cells over-expressing the CD44 protein, leading to rapid and concentration-dependent uptake by the cancer cells through the receptor-mediated endocytosis mechanism. In contrast, no selective targeting of MSNs-HA can be found to the CD44 low-expressing cells, such as MCF-7 and L929 cells. The hydrophobic camptothecin (CPT) drug was encapsulated into MSNs-HA, which showed enhanced cytotoxicity to the Hela cells compared to both free CPT and CPT-loaded MSNs-HA in the presence of excess free HA.
Co-reporter:Kun Zhang, Hangrong Chen, Yuanyi Zheng, Yu Chen, Ming Ma, Xia Wang, Lijun Wang, Deping Zeng and Jianlin Shi
Journal of Materials Chemistry A 2012 - vol. 22(Issue 25) pp:NaN12561-12561
Publication Date(Web):2012/04/26
DOI:10.1039/C2JM31504A
A novel and general in situ hydrophobic shell-protected selective etching strategy has been developed to synchronously synthesize and modify hollow mesoporous silica nanoparticles (HMSNs) and rattle-type mesoporous silica nanoparticles (RMSNs) with well-defined morphology, effectively avoiding the drawbacks of post-modification. The key point of the strategy lies in the hydrophilicity differences between the pure silica inner core and the organic hybrid silica shell, which results in the preferential etching of the pure silica inner core. Except that amino group functionalized HMSNs (amino-HMSNs) can be synthesized via this strategy, it can be readily applied for the synthesis of HMSNs and RMSNs synchronously grafted with different kinds of functional groups by employing other silane coupling agents, directly indicating the generality of this strategy. Furthermore, adding no additional reduction agents, the amino-HMSNs can be regarded as nanoreactors, and a distinctively heterogeneous rattle-type structure, Au@HMSN/Au, with an entrapped size-tunable Au nanoparticle and some small Au nanocrystals embedded in the hollow cavity and shell of each nanoparticle, respectively, is obtained. As hybrid ultrasound contrast agents (UCAs), unlike micro-sized organic UCAs merely confined to blood pool imaging, the as-synthesized nano-sized amino-HMSNs can achieve excellent in vitro ultrasound imaging, and potentially be applied in cell-level imaging. More importantly, relying on the process merits of our strategy, such as the doping of silane coupling agents and no calcination treatment, amino-HMSNs exhibit enhanced ultrasound imaging to some certain extent compared to the calcined ones.
Co-reporter:Ming Ma, Shuguang Zheng, Hangrong Chen, Minghua Yao, Kun Zhang, Xiaoqing Jia, Juan Mou, Huixiong Xu, Rong Wu and Jianlin Shi
Journal of Materials Chemistry A 2014 - vol. 2(Issue 35) pp:NaN5836-5836
Publication Date(Web):2014/06/24
DOI:10.1039/C3TB21666G
A novel modification route integrating the copolymers of positive charged quaternary amines and polyethylene glycol (PEG) units using a combination of reversible addition–fragmentation chain-transfer polymerization (RAFT) and “Graft From” strategy, has been proposed and developed, for the first time, to decorate the surface of mesoporous silica nanoparticles (MSNs). These MSNs are shown to have a greatly reduced hydrodynamic particle size in physiological solution. It is demonstrated that such an efficient copolymer surface modification strategy, resulting in PEG coating with high positive zeta potential, can achieve a nearly 2-fold enhanced permeability and retention (EPR) effect, and longer blood half-life compared to coating with PEG only. Besides, the in vivo results demonstrated that this surface modification strategy could lead to a higher efficacy of doxorubicin (DOX) drug delivery and greater suppression of side effects compared to the free drug. Based on this novel strategy of combining “RAFT” and “Graft From” polymerization, it is anticipated that this efficient modification of tumor-specific targeting of MSNs can be widely used in future nanomedicine research.
Co-reporter:Jin Wang, Jinzhen Zhu, Xiaoxia Zhou, Yanyan Du, Weimin Huang, Jianjun Liu, Wenqing Zhang, Jianlin Shi and Hangrong Chen
Journal of Materials Chemistry A 2015 - vol. 3(Issue 14) pp:NaN7638-7638
Publication Date(Web):2015/02/25
DOI:10.1039/C5TA00468C
The efficient removal of low-concentration nitric oxide at room temperature from a semi-closed space is becoming a crucial but challenging issue in the context of increasingly serious air pollution. A novel nanoflower-like weak crystallization manganese oxide (WMO) has been synthesized via a facile and scalable strategy for low-concentration nitric oxide oxidation at room temperature. The prepared WMO shows the nanoflower-like morphology with abundant water molecules and Mn vacancies inside. Such WMO could easily adsorb NO and quickly convert it into NO2via catalytic oxidization. Herein, the weak crystallization structure and the presence of Mn vacancies are identified to be mainly responsible for the adsorption and catalytic oxidation of NO. More importantly, it shows much longer lifetime in a moist stream of simulated feed gas than that under dry conditions, which can be attributed to the relative stability of the catalyst with hydrated surfaces. Comparative DFT-calculations are performed to reveal the catalytic effect of Mn-vacancies and hydrated surfaces in reducing the reaction barriers of rate-determining steps.
Co-reporter:Gang Wan, Ming Ma, Alec (Yi) Jia, Lisong Chen, Yu Chen, Xiangzhi Cui, Hangrong Chen and Jianlin Shi
Journal of Materials Chemistry A 2016 - vol. 4(Issue 30) pp:NaN11629-11629
Publication Date(Web):2016/07/04
DOI:10.1039/C6TA03930H
A 3D assembly of crumpled nitrogen-doped carbon nanosheets with hierarchical frameworks and encased ultrafine iron carbide nanoparticles on the subunits was constructed via a template-free bottom-up self-assembly strategy. The optimized structure design and catalytic-site integration endow the electrocatalyst with outstanding PH-universal ORR performance, serving as a good alternative for the Pt/C catalyst.
Co-reporter:Jinjin Zhao, Zile Hua, Zhicheng Liu, Yongsheng Li, Limin Guo, Wenbo Bu, Xiangzhi Cui, Meiling Ruan, Hangrong Chen and Jianlin Shi
Chemical Communications 2009(Issue 48) pp:NaN7580-7580
Publication Date(Web):2009/11/10
DOI:10.1039/B913920F
We report the direct fabrication of mesoporous zeolite with a hollow spherical/ellipsoidal capsule structure by using conventional TPAOH and CTAB as soft micro- and mesopore generating templates; the mesoporous zeolite shows a high surface area of 717 m2 g−1 and small mesopore size of around 3 nm.
Co-reporter:X. X. Zhou, H. Zhao, W. M. Huang, H. R. Chen and J. L. Shi
Dalton Transactions 2017 - vol. 46(Issue 18) pp:NaN6116-6116
Publication Date(Web):2017/04/12
DOI:10.1039/C7DT00918F
TiO2 and spinel Cu1.5Mn1.5O4 co-modified hierarchically porous zeolite Beta (Ti/Cu1.5Mn1.5O4-HBeta) with 3D interpenetrating micro–mesoporosity has been synthesized, which showed highly efficient catalytic activity to the soot oxidation in the presence of O2/NO/N2 due to the rich moderate intensity acidic sites and chemisorbed oxygen species. In the presence of SO2/O2/NO/N2, the SO2 could be preferentially adsorbed on the Ti/Cu1.5Mn1.5O4-HBeta and the resulting sulfates could easily decompose at elevated temperatures, thus leading to significantly improved sulfur-resistance. Furthermore, the excellent water-resistance and cycling stability were achieved on the catalyst Ti/Cu1.5Mn1.5O4-HBeta owing to its crystalline zeolite framework and highly dispersed active components.
Co-reporter:Xiaoxia Zhou, Xiangzhi Cui, Hangrong Chen, Yan Zhu, Yudian Song and Jianlin Shi
Dalton Transactions 2013 - vol. 42(Issue 4) pp:NaN893-893
Publication Date(Web):2012/11/13
DOI:10.1039/C2DT32144K
The hierarchically porous and iron-functionalized zeolite ZSM-5 has been fabricated as a Fenton photocatalyst by a facile post-treatment process, which exhibits an excellent visible-light catalytic property in the adsorption/degradation of organic pollutants under mild reaction conditions.
Co-reporter:Jinjin Zhao, Wenna Wang, Lingxia Zhang, Xiangzhi Cui, Yan Zhu, Wei Wu, Hangrong Chen and Jianlin Shi
Dalton Transactions 2014 - vol. 43(Issue 2) pp:NaN409-409
Publication Date(Web):2013/10/09
DOI:10.1039/C3DT52623B
Superparamagnetic mesoporous zeolite microspheres with a large mesopore size of 13 nm and a high surface area of 382 m2 g−1 were synthesized for the capacious enrichment of proteins and enzymes. A high degree of ovalbumin immobilization was obtained (491 mg g−1) at pH 6, which is nearly twice that previously reported in the literature.
Co-reporter:Xiaoxia Zhou, Hangrong Chen, Guobin Zhang, Jin Wang, Zhiguo Xie, Zile Hua, Lingxia Zhang and Jianlin Shi
Journal of Materials Chemistry A 2015 - vol. 3(Issue 18) pp:NaN9753-9753
Publication Date(Web):2015/03/18
DOI:10.1039/C5TA00094G
A hierarchically porous zeolite beta has been designed via a facile combined surfactant-assisted hydrothermal treatment and subsequent alkali etching approach. High contents of the Cu and Mn species were then highly dispersed into the as-synthesized hierarchically porous zeolite beta. The prepared composite catalyst exhibits highly active, stable and recyclable catalytic performances for soot oxidation, and extraordinarily low T50 (260 °C) and T90 (300 °C) values can be achieved in the presence of NO. A synergetic catalytic effect between valence-varied active species Cun+ and Mnn+ has been proposed, which features the promoted generations of highly active oxygen species O−/O2− and active intermediate NO2. In addition, the obtained catalyst shows an excellent water resistance performance in soot oxidation due to the hydrophobic crystalline zeolite framework and the interaction between soot and water vapor.
Co-reporter:Kun Zhang, Hangrong Chen, Xiaoxia Zhou, Yun Gong, Guobin Zhang, Xia Wang, Yu Chen and Jianlin Shi
Journal of Materials Chemistry A 2014 - vol. 2(Issue 5) pp:NaN1523-1523
Publication Date(Web):2013/11/15
DOI:10.1039/C3TA14171C
A useful and interesting unconventional phenomenon of Pd nanoparticle formation, i.e., significantly inhibited particle growth at elevated temperatures, has been observed for the first time by growing Pd nanoparticles on a type of nonreactor, amino group-functionalized hollow mesoporous silica nanoparticles (amino-HMSNs). Such an unconventional effect is evidenced to be a competitive result between temperature-dependent coordination and reduction action of amino groups on the shell of HMSNs based on a series of experiments of probing the coordination and reduction capability of the amino groups to a Pd precursor K2PdCl6. A possible mechanism has been proposed to demonstrate and clarify the unconventional growth of Pd nanoparticles on the shell of amino-HMSNs. The as-synthesized Pd nanoparticles on the amino-HMSNs, therefore, show a tunable temperature-dependent small size range (<10 nm) and high dispersity, and can be used as efficient Heck reaction catalysts. Such a finding of unconventional particle growth effect may offer a novel protocol for particle size modulation during materials design and fabrication.
Co-reporter:Jinjin Zhao, Jian Zhou, Yu Chen, Qianjun He, Meiling Ruan, Limin Guo, Jianlin Shi and Hangrong Chen
Journal of Materials Chemistry A 2009 - vol. 19(Issue 41) pp:NaN7616-7616
Publication Date(Web):2009/09/16
DOI:10.1039/B916862A
Mesoporous microspheres of zeolite have been fabricated through direct self-assembly between an aluminosilicate precursor, tetrapropylammonium hydroxide (TPAOH) and poly(methyl methacrylate) (PMMA) nanospheres, where the PMMA nanospheres act as dual-functional templates for the generation of both mesoporosity and spherical morphology.