Co-reporter:Chang Guo;Minmin Xu;Suying Xu
Nanoscale (2009-Present) 2017 vol. 9(Issue 21) pp:7163-7168
Publication Date(Web):2017/06/01
DOI:10.1039/C7NR01858D
Fluorescence is widely used for cell imaging due to its high sensitivity and rich color choice but limited for in vivo imaging because of its low light penetration. Meanwhile, magnetic resonance imaging (MRI) is widely applied for in vivo diagnosis but not suitable for cell imaging because of its low resolution. Compared to 1H-MRI, 19F-MRI is more suitable for clinical application due to its high sensitivity but fabricating 19F-MRI probes is a great challenge. Therefore, it is highly desirable to develop a dual-modal imaging probe for both cell fluorescence imaging and in vivo19F-MRI with high sensitivity and deep penetration. In this study, 19F moiety loaded nanocomposites with an organic fluorescent core were successfully prepared via a facile strategy by encapsulating organic dyes with oleylamine-functionalized polysuccinimide and 1H,1H,2H,2H-perfluorodecyltriethoxysilane (PDTES). The aggregation of organic fluorescent dyes in the core results in significant fluorescence for optical imaging, while the 19F moieties on PDTES allow for simultaneous 19F MRI. Moreover, the nanocomposites exhibited high water dispersibility and excellent biocompatibility. These properties make them promising for both cell imaging and in vivo imaging applications.
Co-reporter:Chenqi Shen;Xiang Lan;Chenggan Zhu;Wei Zhang;Qiangbin Wang
Advanced Materials 2017 Volume 29(Issue 16) pp:
Publication Date(Web):2017/04/01
DOI:10.1002/adma.201606533
Plasmonic motifs with precise surface recognition sites are crucial for assembling defined nanostructures with novel functionalities and properties. In this work, a unique and effective strategy is successfully developed to pattern DNA recognition sites in a helical arrangement around a gold nanorod (AuNR), and a new set of heterogeneous AuNR@AuNP plasmonic helices is fabricated by attaching complementary-DNA-modified gold nanoparticles (AuNPs) to the predesigned sites on the AuNR surface. AuNR is first assembled to one side of a bifacial rectangular DNA origami, where eight groups of capture strands are selectively patterned on the other side. The subsequently added link strands make the rectangular DNA origami roll up around the AuNR into a tubular shape, therefore giving birth to a chiral patterning of DNA recognition sites on the surface of AuNR. Following the hybridization with the AuNPs capped with the complementary strands to the capture strands on the DNA origami, left-handed and right-handed AuNR@AuNP helical superstructures are precisely formed by tuning the pattern of the recognition sites on the AuNR surface. Our strategy of nanoparticle surface patterning innovatively realizes hierarchical self-assembly of plasmonic superstructures with tunable chiroptical responses, and will certainly broaden the horizon of bottom-up construction of other functional nanoarchitectures with growing complexity.
Co-reporter:Xiaoquan Lu 鹿晓泉;Yuanbao Li 李远豹;Xilin Bai 白熙林;Gaofei Hu 胡高飞
Science China Materials 2017 Volume 60( Issue 8) pp:777-788
Publication Date(Web):24 July 2017
DOI:10.1007/s40843-017-9068-6
The doping of radiocontrast agent such as bismuth (Bi) in copper chalcogenide nanocrystals for computed tomography (CT) imaging guided photothermal therapy (PTT) has drawn increasing attention. However, the doping of Bi often suffers from the weak CT signal due to the low Bi doping concentration and deteriorates the PTT efficacy of copper chalcogenides. Here we report a multifunctional nanoprobe by encapsulating both Cu1.94S and Bi2S3 nanocrystals into a biocompatible poly(amino acid) matrix with size of ~85 nm for CT imaging guided PTT. The amount of nanocrystals and the ratio of Cu1.94S-to-Bi2S3 in the multifunctional nanocomposites (NCs) are tunable toward both high photothermal conversion efficiency (~31%) and excellent CT imaging capability (27.8 HU g L−1). These NCs demonstrate excellent effects for photothermal ablation of tumors after intratumoral injection on 4T1 tumor-bearing mice. Our study may provide a facile strategy for the fabrication of multi-functional theranostics towards simultaneous strong CT signal and excellent PTT.铋掺杂硫化铜纳米晶用于CT成像指导的光热治疗已经引起了人们的广泛关注. 然而, 低剂量的铋掺杂CT信号弱, 高剂量铋掺杂又会减弱硫化铜的光热效果. 本文报道了一种多功能纳米探针, 用两亲性高分子将油溶性Cu1.94S和Bi2S3纳米晶同时封装于约85 nm大小的纳米微球中,用于CT成像指导光热治疗. 多功能纳米探针中Cu1.94S和Bi2S3纳米晶的量和比例能够灵活调节, 从而得到较高的光热转换效率(~31%)和良好的CT成像能力(27.8 HU g L−1). 这些纳米探针在4T1荷瘤小鼠进行瘤内注射后, 显示了良好的CT成像与肿瘤光热治疗效果. 该复合纳米探针的制备方法还可用于其他多功能纳米探针的制备.
Co-reporter:Wenli Lu 卢文礼;Jiabin Cui 崔家斌;Rui Jiang 姜瑞;Yueguang Chen 陈玥光
Science China Materials 2017 Volume 60( Issue 10) pp:929-936
Publication Date(Web):28 September 2017
DOI:10.1007/s40843-017-9112-4
The development of ultrasmall transition-metal dichalcogenide (such as MoS2, MoSe2) nanostructures is an efficient strategy to increase the active edge sites and overall performance for hydrogen evolution reaction. Here, we report an in-situ tearing strategy to produce the carbon nanotube supported subnanometer ternary MoSeS (denoted as CNTs@NiSe@MoSeS) for efficient hydrogen evolution. Large (18.3 ± 1.1 nm in length) multilayer MoS2 sheets grown on Ni (OH)2 thin film are torn into subnanometer (5.2 ± 0.7 nm in length) MoSeS via a subsequent selenization progress, along with the transformation of Ni(OH)2 thin film into small NiSe nanoplates. The resulting nanocomposite exhibits abundant active edge sites, outstanding 10,000-cycle stability and ultrahigh activity with a low overpotential of 189 mV at a high current density of 200 mA cm−2 toward hydrogen evolution.制备超小型层状金属硫属化合物是一种有效增加边缘活性位点和高效提升析氢性能的方法. 本文首次报道了一种原位撕裂的方法来制备由碳纳米管(CNTs)支撑的三元MoSeS纳米复合析氢催化剂. 生长在CNTs@Ni(OH)2薄膜上的大尺寸多层MoS2片(18.3± 1.1 nm), 通过原位的硒化过程被撕裂成超小的MoSeS(5.2 ± 0.7nm)纳米片, 同时Ni(OH)2薄膜也被转化为小尺寸的NiSe纳米晶, 最终得到的纳米复合催化剂具有丰富的边缘活性位点,表现出超高的活性, 在200 mA cm−2高的电流密度下, 过电势只要189 mV; 同时在10000次循环下, 依旧保持优异的稳定性. 该工作为纳米晶催化剂的设计和应用打下了良好的基础.
Co-reporter:Hengli Zhu, Rui Jiang, Xiaoqing Chen, Yueguang Chen, Leyu Wang
Science Bulletin 2017 Volume 62, Issue 20(Volume 62, Issue 20) pp:
Publication Date(Web):30 October 2017
DOI:10.1016/j.scib.2017.09.012
Active, stable and low-cost oxygen evolution reaction (OER) catalyst for electrochemical water splitting is key to efficient energy conversion and storage. Here, we report a three-dimensional (3D) nanonetwork as noble-metal-free electrode consisting of nickel cobalt diselenide (NiCoSe2) nanobrush arrays on Ni foam (NF) through the initial hydrothermal reaction and subsequent thermal selenization process. Introducing ammonium fluoride as surface controller, different NiCoSe2 hierarchical architecture can be modulated from nanorods, nanobrush to nanosheets. The unique brush-like NiCoSe2 possesses high surface area for mass transfer, rough surface with rich active sites, 3D nanostructure preventing the accumulation of O2 bubbles. Compared to NiCoSe2 nanorods/NF, NiCoSe2 nanosheets/NF and commercial RuO2, NiCoSe2 nanobrush/NF exhibits an enhanced OER performance in alkaline media to reach a low overpotential of 274 mV at the current density of 10 mA/cm2, small Tafel slope and a long-term stability. The developed 3D nanonetwork highlights the nanoscale engineering and offers a promising alternative to noble metal catalysts for electrochemical water oxidation.
Co-reporter:Jiabin Cui 崔家斌;Suying Xu 许苏英 汪乐余
Science China Materials 2017 Volume 60( Issue 4) pp:352-360
Publication Date(Web):2017 April
DOI:10.1007/s40843-017-9019-4
Sensitive and selective detection of Hg(II) contamination is of great importance with concern of public health. Herein, we successfully fabricated monolayer MoS2 (S-MoS2) decorated Cu7S4-Au (Cu7S4-Au@S-MoS2) nanocomposite modified electrode for the sensitive and selective detection of Hg(II) via anodic stripping voltammetric technique. Due to the excellent electrocatalytic reduction performance arisen from the abundant active edge sites of smallmonolayer MoS2 and good affinity of Au toward Hg, the current method displayed high sensitivity (LOD = 190 nmol L−1) and enhanced selectivity. As control, nanostructures including Cu7S4-Au, Cu7S4@S-MoS2 and Cu7S4-Au@M-MoS2 (M: multilayer) were also investigated, but showed low response to Hg(II), suggesting that both Au domains and active edge sites of monolayer MoS2 have crucial synergistic effects on the high-performance for recognition of Hg(II). Moreover, the developed method displays satisfied performance for the detection of Hg(II) in real samples, which indicates its potentials in practical applications.汞的灵敏选择性检测对于人类的公共安全至关重要. 本文成功制备了单层二硫化钼修饰的Cu7S4-Au纳米结构(Cu7S4-Au@S-MoS2), 通过阳极溶出伏安法实现了对汞的灵敏选择性分析检测. 基于超小(<10 nm)单层MoS2丰富的活性位点及金对汞的良好亲和性, 该方法灵 敏度高(检出限为190 nmol L−1)、选择性好(常见Cd2+、Pb2+、Cu2+等均无干扰), 并成功用于实际样品中汞的灵敏分析. 研究发现Cu7S4-Au与 Cu7S4@S-MoS2 对Hg(II) (1.0 μmol L−1)无响应, 而多层MoS2修饰的Cu7S4-Au(Cu7S4-Au@M-MoS2)对Hg(II) (1.0 μmol L−1) 有弱响应, 结果表明 超小单层MoS2丰富的活性位点及金对汞的良好亲和性对分析检测起到了协同催化作用.
Co-reporter:Gaofei Hu, Nannan Li, Juan Tang, Suying Xu, and Leyu Wang
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 35) pp:22830
Publication Date(Web):August 18, 2016
DOI:10.1021/acsami.6b05510
19F magnetic resonance imaging (MRI), due to its high sensitivity and negligible background, is anticipated to be a powerful noninvasive, sensitive, and accurate molecular imaging technique. However, the major challenge of 19F MRI is to increase the number of 19F atoms while maintaining the solubility and molecular mobility of the probe. Here, we successfully developed a facile and general strategy to synthesize the multifunctional 19F MRI nanoprobes by encapsulating the hydrophobic inorganic nanoparticles (NPs) into a hybrid polymer micelle consisting of hydrolysates of 1H,1H,2H,2H-perfluorodecyltriethoxysilane (PDTES) and oleylamine-functionalized poly(succinimide) (PSIOAm). Due to their good water dispersibility, excellent molecular mobility resulting from the ultrathin coating, and high 19F atom numbers, these nanoprobes generate a separate sharp singlet of 19F nuclear magnetic resonance (NMR) signal (at −82.8 ppm) with half peak width of ∼28 Hz, which is highly applicable for 19F MRI. Significantly, by varying the inorganic core from metals (Au), oxides (Fe3O4), fluorides (NaYF4:Yb3+/Er3+), and phosphates (YPO4) to semiconductors (Cu7S4 and Ag2S, ZnS:Mn2+) NPs, which renders the nanoprobes’ multifunctional properties such as photothermal ability (Au, Cu7S4), magnetism (Fe3O4), fluorescence (ZnS:Mn2+), near-infrared (NIR) fluorescence (Ag2S), and upconversion (UC) luminescence. Meanwhile, the as-prepared nanoprobes possess relatively small sizes (about 50 nm), which is beneficial for long-time circulation. The proof-of-concept in vitro 19F NMR and photothermal ablation of ZnS:Mn2+@PDTES/PSIOAm and Cu7S4@PDTES/PSIOAm nanoprobes further suggest that these nanoprobes hold wide potentials for multifunctional applications in biomedical fields.Keywords: 19F magnetic resonance imaging; hydrolyzation; multifunctional nanoprobes; perfluorodecyltriethoxysilane; poly(succinimide)
Co-reporter:Shiguo Wang, Suying Xu, Gaofei Hu, Xilin Bai, Tony D. James, and Leyu Wang
Analytical Chemistry 2016 Volume 88(Issue 2) pp:1434
Publication Date(Web):December 21, 2015
DOI:10.1021/acs.analchem.5b04194
Aqueous sulfides are emerging signaling agents implicated in various pathological and physiological processes. The development of sensitive and selective methods for the sensing of these sulfides is therefore very important. Herein, we report that the as-synthesized 1-oxo-1H-phenalene-2,3-dicarbonitrile (OPD) compound provides promising fluorescent properties and unique reactive properties toward aqueous sulfides. It was found that OPD showed high selectivity and sensitivity toward Na2S over thiols and other inorganic sulfur compounds through a sulfide involved reaction which was confirmed by high-resolution mass spectroscopy (HRMS) and nuclear magnetic resonance (NMR) results. The fluorescence intensity increases linearly with sulfide concentration in the range of 1.0–30 μM with a limit of detection of 52 nM. This novel fluorescent probe was further exploited for the fluorescence imaging sensing of aqueous sulfide in HeLa cells.
Co-reporter:Suying Xu, Xilin Bai, Jingwen Ma, Minmin Xu, Gaofei Hu, Tony D. James, and Leyu Wang
Analytical Chemistry 2016 Volume 88(Issue 15) pp:7853
Publication Date(Web):June 28, 2016
DOI:10.1021/acs.analchem.6b02032
The use of fluorescence probes for biomedical imaging has attracted significant attention over recent years owing to their high resolution at cellular level. The probes are available in many formats including small particle size based imaging agents which are considered to be promising candidates, due to their excellent stabilities. Yet, concerns over the potential cytotoxicity effects of inorganic luminescent particles have led to questions about their suitability for imaging applications. Exploration of alternatives inspired us to use organic fluorophores with aggregation-induced emission (AIE), prepared by functionalizing the amine group on tetraphenylethene with 3,5-bis(trifluoromethyl)phenyl isocyanate. The as-synthesized novel AIE fluorophore (TPE-F) display enhanced quantum yield and longer lifetime as compared with its counterparts (4,4′,4″,4‴-(ethene-1,1,2,2-tetrayl)tetraaniline, TPE-AM). Furthermore, the TPE-F was encapsulated into small-size organic nanoparticles (NPs; dynamic light scattering size, ∼10 nm) with polysuccinimide (PSI). The biocompatibility, excellent stability, bright fluorescence, and selective cell targeting of these NPs enable the as-prepared TPE-F NPs to be suitable for specific fluorescence cell imaging.
Co-reporter:Lili Lu, Suying Xu, Jiabin Cui and Leyu Wang
RSC Advances 2016 vol. 6(Issue 35) pp:29378-29382
Publication Date(Web):16 Mar 2016
DOI:10.1039/C6RA01567K
We present a facile one-pot wet chemical strategy for the synthesis of monodispersed W17O47 nanoneedles, of which the synthetic conditions and photothermal properties are systematically investigated. By modulating experimental conditions such as the ratio of solvent, the dose of sulfur powder and the reaction time, uniform W17O47 nanoneedles with an aspect ratio larger than 10 are obtained. These hydrophobic W17O47 nanoneedles are subsequently transferred into aqueous solution by coating with amphiphilic polyvinylpyrrolidone (PVP) for photothermal imaging applications. The results suggest that these monodispersed nanoneedles have potential for photothermal detection and photothermal therapy.
Co-reporter:Jun Xu;Jiabin Cui;Chong Guo;Zipeng Zhao;Rui Jiang; Suying Xu;Zhongbin Zhuang;Dr. Yu Huang;Dr. Leyu Wang;Dr. Yadong Li
Angewandte Chemie International Edition 2016 Volume 55( Issue 22) pp:6502-6505
Publication Date(Web):
DOI:10.1002/anie.201600686
Abstract
Increasing the active edge sites of molybdenum disulfide (MoS2) is an efficient strategy to improve the overall activity of MoS2 for the hydrogen-evolution reaction (HER). Herein, we report a strategy to synthesize the ultrasmall donut-shaped Cu7S4@MoS2 hetero-nanoframes with abundant active MoS2 edge sites as alternatives to platinum (Pt) as efficient HER electrocatalysts. These nanoframes demonstrate an ultrahigh activity with 200 mA cm−2 current density at only 206 mV overpotential using a carbon-rod counter electrode. The finding may provide guidelines for the design and synthesis of efficient and non-precious chalcogenide nanoframe catalysts.
Co-reporter:Jun Xu;Jiabin Cui;Chong Guo;Zipeng Zhao;Rui Jiang; Suying Xu;Zhongbin Zhuang;Dr. Yu Huang;Dr. Leyu Wang;Dr. Yadong Li
Angewandte Chemie 2016 Volume 128( Issue 22) pp:6612-6615
Publication Date(Web):
DOI:10.1002/ange.201600686
Abstract
Increasing the active edge sites of molybdenum disulfide (MoS2) is an efficient strategy to improve the overall activity of MoS2 for the hydrogen-evolution reaction (HER). Herein, we report a strategy to synthesize the ultrasmall donut-shaped Cu7S4@MoS2 hetero-nanoframes with abundant active MoS2 edge sites as alternatives to platinum (Pt) as efficient HER electrocatalysts. These nanoframes demonstrate an ultrahigh activity with 200 mA cm−2 current density at only 206 mV overpotential using a carbon-rod counter electrode. The finding may provide guidelines for the design and synthesis of efficient and non-precious chalcogenide nanoframe catalysts.
Co-reporter:Hongli Chen, Manli Song, Juan Tang, Gaofei Hu, Suying Xu, Zhide Guo, Nannan Li, Jiabin Cui, Xianzhong Zhang, Xiaoyuan Chen, and Leyu Wang
ACS Nano 2016 Volume 10(Issue 1) pp:1355
Publication Date(Web):January 7, 2016
DOI:10.1021/acsnano.5b06759
19F magnetic resonance imaging (MRI) is a powerful noninvasive, sensitive, and accurate molecular imaging technique for early diagnosis of diseases. The major challenge of 19F MRI is signal attenuation caused by the reduced solubility of probes with increased number of fluorine atoms and the restriction of molecular mobility. Herein, we present a versatile one-pot strategy for the fabrication of a multifunctional nanoprobe with high 19F loading (∼2.0 × 108 19F atoms per Cu1.75S nanoparticle). Due to the high 19F loading and good molecular mobility that results from the small particle size (20.8 ± 2.0 nm) and ultrathin polymer coating, this nanoprobe demonstrates ultrahigh 19F MRI signal. In vivo tests show that this multifunctional nanoprobe is suitable for 19F MRI and photothermal therapy. This versatile fabrication strategy has also been readily extended to other single-particle nanoprobes for ablation and sensitive multimodal imaging.Keywords: 19F MRI; copper sulfide nanoparticle; multifunctional nanoprobes; photothermal imaging and therapy;
Co-reporter:Yuanbao Li;Xilin Bai;Minmin Xu;Suying Xu;Gaofei Hu
Science China Materials 2016 Volume 59( Issue 4) pp:254-264
Publication Date(Web):2016 April
DOI:10.1007/s40843-016-5035-6
Drug delivery systems (DDSs) have been getting more and more attention in the field of cancer therapy with the development of nanotechnology. But remote and noninvasive controlled drug release for improving treatment efficacy and reducing side effects faces great challenge. We report a kind of “smart” nanocomposites (NCs) that is sensitive to the surrounding temperature by grafting a layer of thermosensitive polymer, poly(N-isopropylacrylamide) (pNIPAm), on the surface of single Cu7S4 nanoparticle (NP) via atomtransfer radical polymerization (ATRP). These NCs demonstrate a photothermal conversion efficiency of 25.4% under 808-nmnear infrared (NIR) light irradiation and a drug loading content of 19.4% (drug/total NCs, w/w) with a lower critical solution temperature (LCST) of ~38°C. At normal physiological temperature (37°C), only 10.8% of the loaded doxorubicin (DOX) was released at physiological pH value (pH 7.4) within 10 h. In the presence of 808-nm irradiation, due to the temperature increment as a result of photothermal effects, DOX was rapidly released.抗癌药物的靶向安全输送及远程无损控制释放是提高肿瘤治疗效率并降低毒副作用的前提, 但挑战巨大. 本文通过原子转移自由基 聚合技术在单颗粒Cu7S4光热纳米粒子表面嫁接一层温敏高分子, 从而设计了一种近红外光热控制智能纳米药物胶囊. 该载药纳米胶囊具 有较高的抗癌药物(阿霉素)负载能力(19.4%)和良好的光热转换效率(25.4%), 并具有合适的药物释放温度(~38°C). 在正常生理条件下(37°C, pH 7.4), 10 h后仅有10.8%的阿霉素释放, 但在808-nm近红外光的照射下, Cu7S4将光能转换成热, 诱导温敏高分子快速收缩, 从而导致所负载 的阿霉素被挤出而释放, 达到远程光控药物释放的目的. 与此同时, Cu7S4的光热效应还可用于肿瘤的热疗, 该复合纳米胶囊对癌症的化疗 与热疗协同疗法将显著提高癌症治疗效果.
Co-reporter:Gaofei Hu;Juan Tang;Xilin Bai;Suying Xu
Nano Research 2016 Volume 9( Issue 6) pp:1630-1638
Publication Date(Web):2016 June
DOI:10.1007/s12274-016-1057-2
Copper sulfide (Cu7S4) nanoparticles coated with an ultra-high payload (~5.0 × 107 fluorine atoms per particle) of fluorinated ligands (oleylamine functionalized 3,5-bis(trifluoromethyl)benzaldehyde, 19FOAm) exhibited a single intense 19F magnetic resonance (MR) signal and efficient near infrared photothermal performance in water medium. In vivo assessment revealed strong 19F MR signals at cancerous lesions and effective inhibition of tumor growth after photothermal treatment, indicating the great potential of these fabricated nanoprobes for simultaneous 19F MR imaging and photothermal therapy.
Co-reporter:Xilin Bai, Suying Xu, Jiali Liu, Leyu Wang
Talanta 2016 Volume 150() pp:118-124
Publication Date(Web):1 April 2016
DOI:10.1016/j.talanta.2015.08.038
•We present a versatile nanocarrier for gene delivery and upconversion luminescence tracking.•The functionalized polymer is biocompatible, biodegradable and easy to prepare.•Near-infrared irradiation allows for deep tissue penetration, promising for real-time monitoring.The real-time fluorescence tracking of gene delivery is very important as it helps to figure out how a vector enters a cell and also to follow its fate within the cell interior. Lanthanide-doped upconversion nanoparticles (UCNPs) have shown great potential in biomedical applications in virtue of their unique optical and biological properties. Herein, we report a simple and versatile strategy to fabricate a multifunctional nanocapsule for effective gene delivery and real-time luminescence tracking. The hydrophobic UCNPs were modified by positively charged amphiphilic polymer together with polyethylene glycol-poly(lactic-co-glycolic acid) (PEG–PLGA) polymer, affording biocompatible nanocapsules with high gene loading capacity and good stability. Red UC luminescence of UCNPs are able to track the delivery of nanocapsules in cells without background fluorescence interference, in the meantime, the green fluorescence of green fluorescence protein (GFP) expressed by the pDNA could subtly monitor the gene transfection efficacy. The results demonstrated that our nanocapsule has ideal biocompatibility, satisfactory gene loading capacity and great bioimaging ability, which is promising for imaging guided cell therapy and gene engineering.A biodegradable multifunctional nanocarrier was fabricated for the simultaneous gene delivery and upconversion luminescence tracking.
Co-reporter:Xilin Bai, Suying Xu, Gaofei Hu, Leyu Wang
Sensors and Actuators B: Chemical 2016 Volume 237() pp:224-229
Publication Date(Web):December 2016
DOI:10.1016/j.snb.2016.06.093
•A novel nanosensor for selective detection of 2,4,6-trinitrotolune was fabricated.•A Meisenheimer complex was formed by means of a charge transfer process from AuNPs-NH2 to TNT, which promotes the aggregation of AuNPs-NH2, thus, enhance the photothermal performance.•The proposed sensor realized on-site visual and ultra-sensitive detection of TNT based on the induced photothermal effect.The exploration of feasible, reliable sensors for the selective and sensitive detection of nitroaromatic explosives is a critical issue nowadays as mandated by homeland security concerns. Our endeavor is to develop an instant on-site visual and ultra-sensitive photothermal nanosensor for 2,4,6-trinitrotoluene (TNT) detection, which could be applied on a broad scale with high selectivity and sensitivity. The fundamental principle of our work is that TNT could effectively induce the aggregation of the cysteamine-stabilized gold nanoparticles (Au NPs) by forming the Meisenheimer complex, which further enhanced the surface plasmon resonance (SPR) properties and the photothermal effects of Au NPs. Other coexisting nitroaromatics have negligible influences on the photothermal responses. By means of the temperature enhancement and photothermal imaging technique, the presence of TNT could be readily recognized and visualized, indicating wide potential applications in analytical sensing.
Co-reporter:Jiabin Cui, Yongjia Li, Lei Liu, Lin Chen, Jun Xu, Jingwen Ma, Gang Fang, Enbo Zhu, Hao Wu, Lixia Zhao, Leyu Wang, and Yu Huang
Nano Letters 2015 Volume 15(Issue 10) pp:6295-6301
Publication Date(Web):September 7, 2015
DOI:10.1021/acs.nanolett.5b00950
We report a highly efficient photocatalyst comprised of Cu7S4@Pd heteronanostructures with plasmonic absorption in the near-infrared (NIR)-range. Our results indicated that the strong NIR plasmonic absorption of Cu7S4@Pd facilitated hot carrier transfer from Cu7S4 to Pd, which subsequently promoted the catalytic reactions on Pd metallic surface. We confirmed such enhancement mechanism could effectively boost the sunlight utilization in a wide range of photocatalytic reactions, including the Suzuki coupling reaction, hydrogenation of nitrobenzene, and oxidation of benzyl alcohol. Even under irradiation at 1500 nm with low power density (0.45 W/cm2), these heteronanostructures demonstrated excellent catalytic activities. Under solar illumination with power density as low as 40 mW/cm2, nearly 80–100% of conversion was achieved within 2 h for all three types of organic reactions. Furthermore, recycling experiments showed the Cu7S4@Pd were stable and could retain their structures and high activity after five cycles. The reported synthetic protocol can be easily extended to other Cu7S4@M (M = Pt, Ag, Au) catalysts, offering a new solution to design and fabricate highly effective photocatalysts with broad material choices for efficient conversion of solar energy to chemical energy in an environmentally friendly manner.
Co-reporter:Sheng Huang, Qian He, Suying Xu, and Leyu Wang
Analytical Chemistry 2015 Volume 87(Issue 10) pp:5451
Publication Date(Web):April 28, 2015
DOI:10.1021/acs.analchem.5b01078
We report for the first time a photothermal paper sensor for the selective and sensitive detection of 2,4,6-trinitrotoluene (TNT) down to 14 ng/cm2. In the presence of TNT, a Meisenheimer complex was formed by means of a charge transfer process from an electron-rich group in polyaniline (PANI) to an electron-deficient nitro group in TNT, which resulted in the near-infrared absorption around 800 nm. Upon irradiation with an 808 nm diode laser, the photothermal effect of the PANI/TNT complex caused the temperature increase, and the temperature difference (ΔT) was proportional to the TNT concentration, while the temperature increase was hardly observed for other nitroaromatics including 2,4-dinitrotoluene (DNT), 2,4,6-trinitrophenol (TNP), and nitrobenzene (NB), affording high selectivity toward TNT. All the tests can be conducted both in solution and on paper. Therefore, the proposed photothermal strategy not only offers a fast and convenient protocol for selective detection of TNT but also indicates great potential in practical applications, especially for airport/railway security inspection and prevention of terrorist attacks.
Co-reporter:Jiabin Cui, Suying Xu, Chang Guo, Rui Jiang, Tony D. James, and Leyu Wang
Analytical Chemistry 2015 Volume 87(Issue 22) pp:11592
Publication Date(Web):October 23, 2015
DOI:10.1021/acs.analchem.5b03652
Optical imaging of latent fingerprints (LFPs) has been widely used in forensic science and for antiterrorist applications, but it suffers from interference from autofluorescence and the substrates background color. Cu7S4 nanoparticles (NPs), with excellent photothermal properties, were synthesized using a new strategy and then fabricated into amphiphilic nanocomposites (NCs) via polymerization of allyl mercaptan coated on Cu7S4 NPs to offer good affinities toward LFPs. Here, we develop a facile and versatile photothermal LFP imaging method based on the high photothermal conversion efficiency (52.92%, 808 nm) of Cu7S4 NCs, indicating its effectiveness for imaging LFPs left on different substrates (with various background colors), which will be extremely useful for crime scene investigations. Furthermore, by fabricating Cu7S4-CdSe@ZnS NCs, a fluorescent-photothermal dual-mode imaging strategy was used to detect trinitrotoluene (TNT) in LFPs while still maintaining a complete photothermal image of LFP.
Co-reporter:Min Bai, Shuina Huang, Suying Xu, Gaofei Hu, and Leyu Wang
Analytical Chemistry 2015 Volume 87(Issue 4) pp:2383
Publication Date(Web):January 21, 2015
DOI:10.1021/ac504322s
We developed an efficient one-pot strategy for the preparation of hydrophilic amine-functionalized nanocomposites by using hydrophobic fluorescence quantum dots ZnS:Mn2+@allyl mercaptan (QDs@AM) as building blocks through novel light-induced in situ polymerization. The average size of as-prepared hydrophilic nanocomposites was ∼50 nm, which could be further tuned by varying the concentrations of the monomers. Importantly, these nanocomposites were further utilized for the facile, highly sensitive, and selective detection of nitroaromatics. The linear ranges for 2,4,6-trinitrotoluene (TNT) and 2,4,6-trinitrophenol (TNP) lie in 0.01–0.5 μg/mL and 0.05–8.0 μg/mL, respectively, barely interfered with by other nitroaromatics such as 2,4-dinitrotoluene (DNT) and nitrobenzene (NB). Moreover, the novel surface modification method developed here offered a general strategy for fabricating hydrophobic nanocomposites with hydrophilic properties and indicated various potential applications including sensing and imaging.
Co-reporter:Hongli Chen, Suying Xu, Jiabin Cui and Leyu Wang
RSC Advances 2015 vol. 5(Issue 114) pp:94375-94379
Publication Date(Web):30 Oct 2015
DOI:10.1039/C5RA20207H
We present Cu2−xS/graphene oxide nanocomposites, which exhibit excellent photocatalytic properties toward photodegradation of organic compounds by real sunlight due to the broadband absorption of Cu2−xS and good electron trapping and shuttling ability of graphene.
Co-reporter:Qian He, Sheng Huang, Suying Xu and Leyu Wang
RSC Advances 2015 vol. 5(Issue 54) pp:43148-43154
Publication Date(Web):06 May 2015
DOI:10.1039/C5RA05939A
We design a pH-responsive cocktail nanocapsule with a suitable size (around 100 nm) via the assembly of doxorubicin (DOX) modified poly(amino acid). Paclitaxel (PTX) is successfully encapsulated in the hydrophobic cavity of the nanocapsules through a non-covalent interaction between PTX and the DOX modified poly(amino acid). Guided by the surface bioconjugated Arg–Gly–Asp (RGD) moieties, a target peptide, nanocapsules are targeted to and uptaken by cancer cells. These nanocapsules are stable under normal physiological pH conditions (pH 7.4) and drug release can be triggered by the relatively low pH (5.0) in cancer cells. Moreover, the drug release can be tracked via the recovered red fluorescence of DOX due to the relief from the self-quenching state as a result of nanocapsule disruption under acidic conditions. The in vitro test results undoubtedly confirm the RGD-mediated synergetic therapeutic efficacy of these cocktail drug nanocapsules. This research paves a new way for the fabrication of smart nanocapsules for cocktail drug delivery.
Co-reporter:Yingxin Ma, Shiguo Wang, Leyu Wang
TrAC Trends in Analytical Chemistry 2015 Volume 65() pp:13-21
Publication Date(Web):February 2015
DOI:10.1016/j.trac.2014.09.007
•Nanosensors serve as powerful tool for detecting nitroaromatic explosives.•We discuss design principles of nanosensors for detection.•We summarize the challenges of designing nanosensors for practical applications.Ultrasensitive, low-cost detection of nitroaromatic explosives has attracted tremendous attention due to their great significance in homeland and international security, environmental assays, and forensics applications. Nanomaterial-based luminescence is a powerful tool in the development of highly selective analytical methods for the detection of nitroaromatic explosives. We critically examine and comment on the current diverse methodologies, principles and techniques for detection of nitroaromatic explosives based on the luminescence of nanomaterials. We provide a comprehensive discussion of the status, advancements, unparalleled challenges and future directions of this field.
Co-reporter:Suying Xu, Sheng Huang, Qian He, Leyu Wang
TrAC Trends in Analytical Chemistry 2015 Volume 66() pp:72-79
Publication Date(Web):March 2015
DOI:10.1016/j.trac.2014.11.014
•Upconversion nanophosphores show great advantages in bioimaging applications.•Synthesis methods, surface-modification strategies for upconversion nanophosphores.•Upconversion nanophosphores with ultrasmall size and high luminescence.•We summarize recent applications of upconversion nanophosphores in bioimaging.•Challenges for future developments of upconversion nanophosphores in bioimaging.Upconversion nanophosphore (UCNP)-based optical imaging is a promising technique in the field of bioimaging due to the unique optical properties of UCNPs. UCNPs can be excited by long wavelength light with low power density and have excellent biocompatibility. By carefully controlling the synthesis of UCNPs, near-infrared emission can also be obtained. Such NIR-to-NIR bioimaging probes show great advantages in terms of bioimaging, such as deep penetration and low autofluorescence. Moreover, UCNPs can also offer a platform for fabricating multifunctional nanocomposites for multi-modal imaging by incorporating magnetic resonance imaging, X-ray computed tomography and single-photon emission computerized tomography techniques. In this review, we briefly introduce the fundamental points of UCNPs, highlight the methods of synthesis and surface-modification strategies, and summarize recent progress. We also discuss the current issues faced by researchers.
Co-reporter:Jiali Liu, Lili Lu, Aiqin Li, Juan Tang, Shiguo Wang, Suying Xu, Leyu Wang
Biosensors and Bioelectronics 2015 Volume 68() pp:204-209
Publication Date(Web):15 June 2015
DOI:10.1016/j.bios.2014.12.053
•Monodispersed and water stable upconversion luminescence nanocrystals were synthesized.•Upconversion luminescence nanosensors were fabricated for the simultaneous detection of H2O2 and glucose.•This nanosensor can be used for glucose detection in complicated human serum without prepurification process.In this paper, a green upconversion photoluminescence (UCPL) system for the highly sensitive and selective detection of H2O2 and glucose in human sera was developed by utilizing the excellent optical properties of NaYF4:Yb3+/Er3+ upconversion nanoparticles (UCNPs). In the presence of H2O2, the colorless 3,3′,5,5′-tetramethylbenzidine (TMB) was oxidized into blue oxidized TMB (oxTMB) by assistance of horseradish peroxidase (HRP). And the green UCPL of UCNPs was quenched by the oxTMB linearly over the range of 100 nM–4.0 μM with a low limit of detection (LOD) of 45.0 nM for H2O2. Based on the transformation of glucose into H2O2 by means of glucose oxidase, the TMB–UCNPs–HRP system was further exploited for the highly sensitive detection of glucose in the range of 0.1–5.0 μM with a LOD of 64.0 nM in human sera independent of preconcentration and purification. The results are in good agreement with the clinical data, suggesting that this UCPL nanosensor is highly practical.
Co-reporter:Xilin Bai, Shiguo Wang, Suying Xu, Leyu Wang
TrAC Trends in Analytical Chemistry 2015 Volume 73() pp:54-63
Publication Date(Web):November 2015
DOI:10.1016/j.trac.2015.04.027
•Multifunctional nanomaterials used as luminescent trackers of drug or gene delivery.•Luminescent nanocarriers in simultaneous tracking drug or gene delivery and imaging.•Strategies for the fabricating luminescent trackers.Drug or gene delivery based on nanostructure is promising for treatments of cancers to solve a variety of issues associated with traditional therapeutic agents from poor bioavailability to systemic toxicity. For real-time monitoring of the delivery process, imaging-guided therapy has attracted growing interest in biomedical applications. Luminescent nanostructures serve as an essential tool for illuminating the pathway of drug or gene delivery in biomedical systems. Considering their crucial role in medical applications, we summarize recent progress of luminescent nanostructures as drug- or gene-delivery nanocarriers with simultaneous imaging tracking. We also discuss the design principles and the critical issues faced by multifunctional nanostructure engineering, which might provide guidance for further development in this field.
Co-reporter:Yingxin Ma, Suying Xu, Shiguo Wang, Leyu Wang
TrAC Trends in Analytical Chemistry 2015 Volume 67() pp:209-216
Publication Date(Web):April 2015
DOI:10.1016/j.trac.2015.01.012
•Luminescent molecularly-imprinted polymer nanocomposites (MIP-NCs).•MIP-NCs are nanomaterials for molecular recognition and detection.•We summarize preparation methods and recent advancements in MIP-NCs.•We discuss the challenges of future applications of MIP-NCs.Molecularly-imprinted polymer nanocomposites (MIP-NCs) have been widely employed to produce stable, robust and cheap materials with specific binding sites for recognition of target molecules such as proteins, drugs, pesticides and explosives. MIP-NCs with luminescent properties possess intrinsic capability as signal transducers with excellent molecular recognition properties. The exploration of luminescent and magnetic MIP-NCs with high-specificity affinity toward analytes has great significance for clinical diagnosis, environmental analysis and homeland security. Here, we summarize the novel approaches to fabrication of luminescent MIP-NCs and their recent applications in sensing.
Co-reporter:Jiali Liu, Lili Lu, Suying Xu, Leyu Wang
Talanta 2015 Volume 134() pp:54-59
Publication Date(Web):1 March 2015
DOI:10.1016/j.talanta.2014.10.058
•A facile one-pot strategy was developed for the synthesis of lysozyme functionalized fluorescence gold nanoclusters.•The lysozyme functionalized fluorescence gold nanoclusters demonstrate good biorecognition abilities.•This nanosensor can be used for fluorescence enhancement detection of E. coli.A facile one-pot strategy was developed for the synthesis of lysozyme functionalized fluorescence gold nanoclusters (AuNCs). The lysozymes added to reduce Au3+ ions and stabilize the AuNCs during the synthesis were coated on the AuNCs surface and retained their specific recognition ability for bacteria such as Escherichia coli (E. coli). Based on such ability, these AuNCs were specifically attached onto the surface of E. coli, which resulted in great red fluorescence enhancement. Nevertheless, the bovine serum albumin (BSA) stabilized AuNCs could not recognize E. coli and no fluorescence enhancement was observed. Upon the addition of E. coli, the red fluorescence intensity of lysozyme-AuNCs was enhanced linearly over the range of 2.4×104 −6.0×106 CFU/mL of E. coli with high sensitivity (LOD=2.0×104 CFU/mL, S/N=3). The visualization fluorescence evolution may enable the rapid and real-time detection of bacteria. This study may be extended to other functional proteins such as antibody, enzyme, and peptide functionalized nanoclusters while retaining the bioactivity of coating proteins and find wide applications in the fields of biochemistry and biomedicine.Lysozyme functionalized fluorescence gold nanoclusters with good biorecognition ability were synthesized through a facile one-pot strategy and utilized for the fluorescence enhancement detection of E. coli.
Co-reporter:Yingxin Ma, Sheng Huang, Mingliang Deng, and Leyu Wang
ACS Applied Materials & Interfaces 2014 Volume 6(Issue 10) pp:7790
Publication Date(Web):April 16, 2014
DOI:10.1021/am501053n
A highly water stable and strong upconversion (UC) luminescence NaYF4@PSI–NH nanosensor for the simultaneous and selective detection of 2,4,6-trinitrotoluene (TNT) and 2,4,6-trinitrophenol (TNP) was successfully developed. Via the 980 nm near-infrared (NIR) irradiation, these nanosensors emit strong white UC luminescence with five typical emission peaks centered at 363, 455, 475, 546, and 654 nm. The UC emission at both 363 and 546 nm was quenched by the addition of TNT; however, the ratio of luminescence intensity at 363 nm to 546 nm (I363/I546) had no change with the increase of TNT concentration. Meanwhile, only violet UC emission at 363 nm was dramatically quenched via the addition of TNP, and the I363/I546 ratio is negatively proportional to the TNP concentration in the range of 0.01–4.5 μg/mL of TNP. On the other hand, the green UC emission intensity at 546 nm is in negative proportion to the concentration of TNT. Moreover, cyclohexane, toluene, and other nitroaromatics (such as 2,4-dinitrotoluene (DNT) and nitrobenzene (NB)) have no influence on the detection. Therefore, we developed a facile method for the simultaneous and selective detection of TNT and TNP in the mixture solution of nitroaromatics independent of complicated instruments and sample pretreatment.Keywords: nanoparticles; nitroaromatic explosives; simultaneous detection; white upconversion luminescence;
Co-reporter:Min Bai, Xilin Bai, and Leyu Wang
Analytical Chemistry 2014 Volume 86(Issue 22) pp:11196
Publication Date(Web):October 21, 2014
DOI:10.1021/ac5026489
Fluorescence imaging of transduced cells and tissues is valuable in the development of gene vectors and the evaluation of gene therapy efficacy. We report here the simple and rational design of multifunctional nanocomposites (NCs) for simultaneous gene delivery and fluorescence tracking based on ZnS:Mn2+ quantum dots (QDs) and positively charged polymer coating. The positively charged imidazole in the as-synthesized amphiphilic copolymer can be used for gene loading via electrostatic interaction. While the introduced poly(ethylene glycol) (PEG) can be used to reduce the binding of plasma proteins to nanovectors and minimize clearance by the reticuloendothelial system after intravenous administration. Most importantly, these multifunctional nanovectors showed much lower cellular toxicity than the commercial polyethylenimine (PEI) transfection vectors. On the basis of the red fluorescence of QDs, we can real-time track the gene delivery in cells, and the transfection efficacy of pDNA encoding enhanced green fluorescence protein (pEGFP) was monitored via the green fluorescence of the GFP expressed by the pDNA delivered into the nuclei. Fluorescence imaging analysis confirmed that the QDs-based nanovectors delivered pDNA into HepG2 cells efficiently. These new insights and capabilities pave a new way toward nanocomposite engineering for fluorescence imaging tracking of gene therapy.
Co-reporter:Yingxin Ma, Leyu Wang
Talanta 2014 Volume 120() pp:100-105
Publication Date(Web):March 2014
DOI:10.1016/j.talanta.2013.12.009
Co-reporter:Mingliang Deng
Nano Research 2014 Volume 7( Issue 5) pp:782-793
Publication Date(Web):2014 May
DOI:10.1007/s12274-014-0439-6
Co-reporter:Mingyue An ; Jiabin Cui
The Journal of Physical Chemistry C 2014 Volume 118(Issue 6) pp:3062-3068
Publication Date(Web):January 26, 2014
DOI:10.1021/jp4092305
Nanocomposite catalysts containing both magnetite (Fe3O4) and palladium (Pd) nanoparticles with magnetic separation and recyclability were successfully fabricated via polymer encapsulation and then silica coating and applied for catalytic hydrogenation of 4-nitrophenol. Fe3O4 nanoparticles were used as not only the prerequisite of magnetic separation but also the supports to prevent the aggregation of Pd nanoparticles at high temperature. Moreover, the surfactants and polymer supports on the particle surface were removed by calcination, and thus the catalysis centers (Pd nanoparticles) were totally exposed to the reactants, which is preferable for a good catalysis efficacy. The results of catalytic hydrogenation of 4-nitrophenol demonstrated that the catalytic activity of these as-prepared nanocomposite catalysts were well maintained even after 10 repeated cycles. Unlike the noble metal nanoparticle decorated large magnetic nanosphere with residual magnetism, these as-prepared nanocomposites based on superparamagnetic nanoparticles possess many advantages including high catalytic activity, convenient magnetic separation, good dispersibility, high water stability, and excellent recyclability.
Co-reporter:Hao Li ;Dr. Leyu Wang
Chemistry – An Asian Journal 2014 Volume 9( Issue 1) pp:153-157
Publication Date(Web):
DOI:10.1002/asia.201300897
Abstract
Multicolor upconversion (UC) luminescence of NaYF4:Yb3+/Er3+ nanoparticles (NPs) was successfully tuned by simply controlling the NaF dosage. Unlike UC nanocrystals previously reported in the literature with multicolor emission obtained by varying the rare-earth dopants, the current work developed a new approach to tune the UC emission color by controlling the NaF concentration without changing the ratio and dosage of rare-earth ions. TEM and powder XRD were used to characterize the shape, size, and composition of the UC luminescent nanocrystals. The luminescence images, emission spectra, and multicolor emission mechanism of the NPs have also been demonstrated. As a result of the excellent ability of this new method to manipulate color emission, this will open up new avenues in the areas of bioprobes, light-emitting devices, color displays, lasers, and so forth. To demonstrate their biological applications, the water-stable, biocompatible, and bioconjugatable NaYF4:Yb3+/Er3+@poly(acrylic acid) NPs were synthesized by this developed strategy and applied in targeted-cell UC luminescence imaging.
Co-reporter:Shiguo Wang, Leyu Wang
TrAC Trends in Analytical Chemistry 2014 Volume 62() pp:123-134
Publication Date(Web):November 2014
DOI:10.1016/j.trac.2014.07.011
•Lanthanide-doped nanomaterials are essential for optical imaging.•Lanthanide-doped nanomaterials have excellent luminescence.•Lanthanide-doped nanomaterials can be functionalized with polymers.•Lanthanide-doped luminescent nanocomposites can be used in analytical chemistry.•Regulated and multicolor emissions of lanthanide-doped nanocomposites can be useful.Lanthanide-doped inorganic nanomaterials are a prominent class of nanocrystals with multicolor emissions that are an essential tool for optical imaging in analytical chemistry. Based on the excellent luminescence of lanthanide-doped nanomaterials, novel nanocomposites with diverse sizes (sub-10 nm) and properties, such as luminescence-plasmon, magnetism-luminescence, and upconversion (UC) and downconversion (DC) dual-mode luminescence, have been designed and prepared. These functional nanocomposites have been achieved by functionalization of lanthanide-doped nanomaterials with various types of polymers, responsive moieties, and targeting molecules. Here, we summarize the recent advancements in application of lanthanide-doped luminescence nanocomposites in analytical chemistry and highlight the challenges for future research. Precisely regulated and multicolor-emission lanthanide-doped nanocomposites will be a next thrust for applications in theranostics. Future applications of lanthanide-doped nanocomposites will benefit from such research.
Co-reporter:Hui Li, Huanjie Wang and Leyu Wang
Journal of Materials Chemistry A 2013 vol. 1(Issue 6) pp:1105-1110
Publication Date(Web):21 Nov 2012
DOI:10.1039/C2TC00359G
Via a facile one-pot strategy, polyaspartate (PASP) coated LaF3:Ce3+/Tb3+ luminescent nanocrystals have been successfully prepared. Based on the luminescence quenching of the PASP modified LaF3:Ce3+/Tb3+ nanocrystals by Fe3+, a simple and novel luminescent chemosensor for Fe3+ has been developed. High selectivity and sensitivity is observed over other cations, which is mainly attributed to the formation of a PASP–Fe3+ complex on the NP surface. The luminescence of the suspensions was gradually quenched with the addition of Fe3+ ion, with a linear range of 5 × 10−7 to 1 × 10−4 mol L−1.
Co-reporter:Mingyue An, Jiabin Cui, Qian He and Leyu Wang
Journal of Materials Chemistry A 2013 vol. 1(Issue 9) pp:1333-1339
Publication Date(Web):08 Jan 2013
DOI:10.1039/C2TB00469K
Dual-modal luminescence nanocomposites (NCs) were successfully prepared via a facile and versatile strategy by embedding the hydrophobic down-conversion (DC) fluorescence ZnS:Mn2+ quantum dots (QDs) and up-conversion (UC) luminescence NaYF4:Er3+/Yb3+ nanoparticles (NPs) into hydrophilic polymer matrixes through in situ cross-linking polymerization. Due to the enriched carboxylic groups in the polymer matrixes, the as-prepared NCs are highly water-stable and bioconjugatable with chemical and biological moieties. The results of cytotoxicity assay and dual-modal luminescence cell imaging application of DC–UC NCs indicate that the as-prepared NCs are biocompatible and applicable in biomedical fields. The current work paves the way to the fabrication of multifunctional NCs including down- and up-conversion dual-modal luminescence, luminescence–magnetism, magnetic targeted drug vehicles and magnetic recyclable catalyst NCs, and will attract wide attention from the fields of chemistry, materials, catalysis, nanotechnology, nanobiotechnology and nanomedicine.
Co-reporter:Nina Tu and Leyu Wang
Chemical Communications 2013 vol. 49(Issue 56) pp:6319-6321
Publication Date(Web):28 May 2013
DOI:10.1039/C3CC43146K
We present a novel report on a surface plasmon resonance enhanced upconversion luminescence strategy in aqueous media for highly sensitive and selective detection of 2,4,6-trinitrotoluene (TNT).
Co-reporter:Hao Li and Leyu Wang
ACS Applied Materials & Interfaces 2013 Volume 5(Issue 21) pp:10502
Publication Date(Web):October 2, 2013
DOI:10.1021/am4020605
A facile method is presented for the selective luminescence detection of trace polycyclic aromatic hydrocarbons (PAHs) based on a combination of the specific recognition of molecularly imprinted polymers (MIPs) and magnetic separation (MS). Multifunctional magnetic–luminescent MIP nanocomposites were fabricated via a one-pot emulsion strategy using polystyrene-co-methacrylic acid copolymer, hydrophobic Fe3O4 nanoparticles and luminescent LaVO4:Eu3+ nanoparticles as building blocks with a phenanthrene template. The resulting nanocomposites can be employed in a simple method for the luminescence detection of phenanthrene. Furthermore, magnetic separation of the nanocomposites from the target mixture prior to luminescence detection of phenanthrene affords significantly enhanced selectivity and sensitivity, with a 3σ limit of detection (LOD) as low as 3.64 ng/mL. Milk samples spiked with phenanthrene (5.0 μg/mL) were assayed via this method and recoveries ranging from 97.11 to 101.9% were obtained, showing that our strategy is potentially applicable for the preconcentration, recovering, and monitoring of trace PAHs in complex mixtures.Keywords: luminescence detection; magnetic separation; molecularly imprinted polymers; nanocomposites; polycyclic aromatic hydrocarbons (PAHs); selectivity;
Co-reporter:Huanjie Wang and Leyu Wang
Inorganic Chemistry 2013 Volume 52(Issue 5) pp:2439-2445
Publication Date(Web):February 18, 2013
DOI:10.1021/ic302297u
For successful biological applications of luminescent nanocrystals, surface functionalization is very essential. It is very important to develop the facile synthetic methods to gain access to obtaining water-stable and biocompatible NPs with appropriate functional groups as well as high luminescence efficiency. Herein, a green and facile one-pot hydrothermal strategy was developed for the preparation of poly(amino acid) coated LaVO4:Eu3+–PASP luminescent nanocrystals by employing the hydrolysis of polysuccinimide (PSI) to polyaspartic acid (PASP) to provide a general platform for the surface modification. Because of the enriched carboxylic groups in the PASP coating, these as-prepared nanoparticles (NPs) demonstrated good water-stability, biocompatibility, and bioconjugatability. Due to their strong red luminescence and good bioconjugatability, the antibody bioconjugated LaVO4:Eu3+–PASP NPs were successfully used as the biomarkers for cancer cell specific luminescence imaging. The results indicate that these NPs have the potential to act as luminescent probes for luminescence assay and in vitro imaging.
Co-reporter:Hui Li and Leyu Wang
Analyst 2013 vol. 138(Issue 5) pp:1589-1595
Publication Date(Web):16 Jan 2013
DOI:10.1039/C3AN36601D
Upconversion luminescence is an anti-Stokes' emission process by converting long wavelength near-infrared (NIR, 980 nm) irradiation into shorter wavelength visible light emission, which demonstrates many advantages including no autofluorescence, low damage to samples, no photobleaching, and high sensitivity. Based on the Rhodamine B thiolactone (RBT) functionalized NaYF4:15%Yb3+,5%Er3+ (UCNPs@RBT) nanocomposites, an ultrasensitive, selective, and rapid upconversion luminescence resonance energy transfer (UC-LRET) sensor has been developed for the detection of mercury ions (Hg2+) in water. Upconverting luminescence resonance energy transfer from the UCNPs to the RBT derivates occurs after the addition of Hg2+ ions into the UCNPs@RBT colloidal solution. This UC-LRET recognition of Hg2+ can be finished within 1 min and other cations have no influence on the detection of mercury ions. This newly developed sensor demonstrates high selectivity toward the mercury ions and enables ultrasensitive and rapid detection of mercury ions in water in the range of 5 nM to 10 μM with a 3σ limit of detection of 3.7 nM. This sensor can be used for a naked-eye detection of Hg2+ ions via its green upconverting luminescence response under the infrared excitation (980 nm) with the merit of no autofluorescence interference and good photostability. In addition, by dipping the hydrogel of UCNPs@RBT nanocomposites onto the filter paper, a highly selective and convenient luminescent paper sensor for Hg2+ ions was also developed.
Co-reporter:Shan Peng, Wei Yan, Leyu Wang
Materials Research Bulletin 2013 48(11) pp: 4693-4698
Publication Date(Web):
DOI:10.1016/j.materresbull.2013.08.012
Co-reporter:Jiabin Cui, Mingyue An, Leyu Wang
Talanta 2013 Volume 115() pp:512-517
Publication Date(Web):15 October 2013
DOI:10.1016/j.talanta.2013.05.069
•A facile strategy for the fabrication of composites nanosensors was developed.•Naked-eye visible luminescence turn-on detection of Hg2+ was obtained.•The detection has advantages of rapid response, good sensitivity, and high selectivity.Composite nanospheres containing dithizone, luminescent LaVO4:Eu3+ nanoparticles (NPs), and amphiphilic polymer have been composed for the rapid, selective, and visual luminescence turn-on detection of mercury ions (Hg2+) in water. Due to the absorption of dithizone, the strong red luminescence of LaVO4:Eu3+ NPs encapsulated in nanospheres was quenched noticeably. As a result, these as-prepared nanocomposites (NCs) demonstrate very weak red luminescence. However, in the presence of Hg2+, the red luminescence of nanocomposites was turned on dramatically, which can be attributed to the strong binding of mercury (II) ions by dithizone and forming a complex without absorption in the red emission range. Meanwhile, other cations have no influence on the detection of Hg2+, suggesting a good selectivity for Hg2+ sensing. Due to the high photostability and chemical stability of the nanocomposites, operation simplicity, low cost, and good selectivity, this newly developed method is highly desirable for field assay of Hg2+ in aqueous media ranging from 40.0 nM to 4.0 μM with a limit of detection of 32.0 nM and a good linearity (r=0.9980). Therefore, a facile, rapid, selective, and visual luminescence turn-on technology has been successfully developed for Hg2+ detection.
Co-reporter:Hao Li
Science Bulletin 2013 Volume 58( Issue 33) pp:4051-4056
Publication Date(Web):2013 November
DOI:10.1007/s11434-013-6023-8
Upconversion luminescence nanoparticles (UCNPs) have shown promising applications in biomedical fields as luminescent probes because of their excellent advantages such as single excitation with multicolor emission, low autofluorescence, and deep penetration. But the biological applications of such nanomaterials are still restricted due to the unfavorable surface properties. In this work, we develop a facile one-pot hydrothermal route to obtain O-carboxymethyl chitosan (OCMC)-wrapped NaYF4: Yb3+/Tm3+ /Er3+ red UCNPs which have been used for targeted cell luminescence imaging directly and efficiently. The successful coating of the UCNPs by OCMC has been confirmed by Fourier-transform infrared (FTIR) spectroscopy and dynamic light scattering (DLS) studies. Transmission electron microscopy (TEM), powder X-ray diffraction (XRD), thermogravimetric analysis (TGA), and photoluminescence (PL) spectra have been used to characterize the size, composition and emission color of the samples, respectively. Due to the good biocompatibility, water-solubility, and strong UC luminescence, these hydrophilic nanocrystals will open up new avenues in further bioapplications.
Co-reporter:Yingxin Ma, Sheng Huang, Leyu Wang
Talanta 2013 Volume 116() pp:535-540
Publication Date(Web):15 November 2013
DOI:10.1016/j.talanta.2013.07.033
•Multifunctional nanocomposites containing luminescent and magnetic nanoparticles were successfully fabricated.•With the help of magnetic separation, TNT can be selectively detected in the presence of coexisting nitroaromatics.•This multifunctional nanoplatform can be extended for other biochemical application.Rapid, sensitive and selective detection of 2,4,6-trinitrotoluene (TNT) in aqueous solution differentiating from other nitroaromatics and independent of complicated instruments is in high demand for public safety and environmental monitoring. Despite of many methods for TNT detection, it is hard to differentiate TNT from 2,4,6-trinitrophenol (TNP) due to their highly similar structures and properties. In this work, via a simple and versatile method, LaF3ːCe3+−Tb3+and Fe3O4 nanoparticle-codoped multifunctional nanospheres were prepared through self-assembly of the building blocks. The luminescence of these nanocomposites was dramatically quenched via adding nitroaromatics into the aqueous solution. After the magnetic separation, however, the interference of other nitroaromatics including 2,4,6-trinitrophenol (TNP), 2,4-dinitrotoluene (DNT), and nitrobenzene (NB) was effectively overcome due to the removal of these coexisting nitroaromatics from the surface of nanocomposites. Due to the formation of TNT−−RCONH3+, the TNT was attached to the surface of the nanocomposites and was quantitatively detected by the postexposure luminescence quenching. Meanwhile, the luminescence intensity is negatively proportional to the concentration of TNT in the range of 0.01–5.0 μg/mL with the 3σ limit of detection (LOD) of 10.2 ng/mL. Therefore, the as-developed method provides a novel strategy for rapid and selective detection of TNT in the mixture solution of nitroaromatics by postexposure luminescence quenching.
Co-reporter:Mingliang Deng, Nina Tu, Feng Bai, and Leyu Wang
Chemistry of Materials 2012 Volume 24(Issue 13) pp:2592
Publication Date(Web):June 12, 2012
DOI:10.1021/cm301285g
A facile and general strategy was successfully developed for the surface modification of kinds of hydrophobic inorganic nanomaterials with various chemical compositions, shapes, and sizes. Via this ultrasonication assistant encapsulation technology, these hydrophobic inorganic nanocrystals were successfully encapsulated into the carboxylated phospholipids and polymers micelles with one particle per micelle. The surface modified nanocrystals were characterized by transmission electron microscopy (TEM), Fourier-transform infrared (FTIR), and thermogravimetric analysis (TGA). After encapsulation, the particle size, shape, and optical and magnetic properties were effectively retained. These functionalized nanocrystals are highly water-stable and biocompatible. After being bioconjugated with the antibodies, the functionalized quantum dots (QDs) have been successfully used as biolabels for targeted cell fluorescence imaging.Keywords: cell imaging; hydrophobic nanocrystals; surface functionalization;
Co-reporter:Yingxin Ma, Hao Li and Leyu Wang
Journal of Materials Chemistry A 2012 vol. 22(Issue 36) pp:18761-18767
Publication Date(Web):27 Jul 2012
DOI:10.1039/C2JM32897F
Luminescent-magnetic multifunctional molecularly imprinted polymer (MIP) nanospheres containing luminescent LaVO4:Eu3+ nanocrystals (NCs), magnetic Fe3O4 nanoparticles (NPs), and the recognition sites of template organophosphate pesticides were successfully prepared via a facile and versatile bottom-up self-assembly strategy. Because of the photoluminescence quenching via diazinon molecules (templates) rebinding into the recognition cavities, these composite MIP nanospheres were successfully applied to the selective and direct luminescence detection of diazinon with the assistance of magnetic separation and concentration. The luminescence intensity was proportional to the concentration of diazinon in the range of 0.01–9.0 μg mL−1 with the 3σ limit of detection (LOD) of 7.1 ng mL−1. This facile and versatile strategy for the MIP nanocomposites is very easy to be extended to other inorganic/organic multifunctional composite nanospheres and will find great potential application as chemical and biological sensors in aqueous media.
Co-reporter:Yaoyao Zhao, Yingxin Ma, Hao Li, and Leyu Wang
Analytical Chemistry 2012 Volume 84(Issue 1) pp:386
Publication Date(Web):November 18, 2011
DOI:10.1021/ac202735v
Quantum dots (QDs)-based molecularly imprinted polymer (MIP) composite nanospheres were successfully prepared via a facile and versatile ultrasonication-assisted encapsulation method. Unlike the hydrogen-bond-based MIPs, these so-prepared QDs-MIP composite nanospheres, relying on the interaction including van der Waals forces and hydrophobic forces, demonstrated excellent selectivity in aqueous media. Their small particle sizes and carboxyl-enriched polymer matrixes give rise to their good dispersibility and stability in aqueous solution, and faster adsorption and desorption kinetics, which further make them extensively applicable for chemical/biological sensors in aqueous media. Based on the fluorescence quenching via template analytes (diazinon) rebinding into the recognition cavities in the polymer matrixes, the QDs-MIP nanospheres were successfully applied to the direct fluorescence quantification of diazinon, independent of extracting templates from the MIP nanospheres, as well as further complicated and time-consuming assays. This novel method can selectively and sensitively detect down to 50 ng/mL of diazinon in water, and a linear relationship has been obtained covering the concentration range of 50–600 ng/mL. The present studies provide a new and general strategy to fabricate other multifunctional (luminescent and magnetic) inorganic–organic MIP nanocomposites with highly selective recognition ability in aqueous media and are pretty desirable for biomedical/chemical sensing applications.
Co-reporter:Yingxin Ma, Hao Li, Shan Peng, and Leyu Wang
Analytical Chemistry 2012 Volume 84(Issue 19) pp:8415
Publication Date(Web):September 4, 2012
DOI:10.1021/ac302138c
Rapid, sensitive, and selective detection of explosives such as 2,4,6-trinitrotoluene (TNT) and 2,4,6-trinitrophenol (TNP), especially using a facile paper sensor, is in high demand for homeland security and public safety. Although many strategies have been successfully developed for the detection of TNT, it is not easy to differentiate the influence from TNP. Also, few methods were demonstrated for the selective detection of TNP. In this work, via a facile and versatile method, 8-hydroxyquinoline aluminum (Alq3)-based bluish green fluorescent composite nanospheres were successfully synthesized through self-assembly under vigorous stirring and ultrasonic treatment. These polymer-coated nanocomposites are not only water-stable but also highly luminescent. Based on the dramatic and selective fluorescence quenching of the nanocomposites via adding TNP into the aqueous solution, a sensitive and robust platform was developed for visual detection of TNP in the mixture of nitroaromatics including TNT, 2,4-dinitrotoluene (DNT), and nitrobenzene (NB). Meanwhile, the fluorescence intensity is proportional to the concentration of TNP in the range of 0.05–7.0 μg/mL with the 3σ limit of detection of 32.3 ng/mL. By handwriting or finger printing with TNP solution as ink on the filter paper soaked with the fluorescent nanocomposites, the bluish green fluorescence was instantly and dramatically quenched and the dark patterns were left on the paper. Therefore, a convenient and rapid paper sensor for TNP-selective detection was fabricated.
Co-reporter:Sheng Huang, Wei Yan, Gaofei Hu, and Leyu Wang
The Journal of Physical Chemistry C 2012 Volume 116(Issue 38) pp:20558-20563
Publication Date(Web):September 5, 2012
DOI:10.1021/jp305211d
By using water as an exclusive solvent, a facile one-pot strategy was developed for the preparation of hydrophilic magnetite nanofluids coated with oxidized dextran. These as-synthesized magnetic nanofluids are highly water-soluble, biocompatible, and bioconjugatible for targeted detection because of the enriched carboxylate groups in the oxidized dextran shell. These nanoparticles are less than 10 nm and demonstrate strong magnetization, low cytotoxicity, and high T2-weighted MR image signal intensity (r2 = 250.5 mM–1 s–1, 3.7 times larger than the commercial product). Also, these magnetic nanofluids are highly stable in many kinds of aqueous media; even though a strong magnet is adjoined to the nanofluids, the whole colloid solution rather than the solid particle only is drawn to the side wall of the vial. These novel properties render this magnetic nanofluid desirable for wide bioapplications including MRI, highly efficient magnetic bioseparation, targeted drug delivery, and magnetic hyperthermia.
Co-reporter:Yanyu Zhu;Yaoyao Zhao;Yingxin Ma;Mingliang Deng
Luminescence 2012 Volume 27( Issue 1) pp:74-79
Publication Date(Web):
DOI:10.1002/bio.1328
ABSTRACT
A simple general strategy was successfully developed for the preparation of magnetic–luminescent multifunctional nanocomposites by incorporating fluorescent (pyrene) and magnetic (Fe3O4) components simultaneously into a poly(styrene-co-methacrylic acid) [poly(St-co-MAA)] copolymer matrix. The nanospheres so prepared were characterized using scanning electron microscopy (SEM), powder X-ray diffraction (XRD) and Fourier transform infrared (FTIR) analysis. The prepared magnetic–fluorescent inorganic–organic nanocomposites have excellent magnetic and photoluminescent properties. They can be used in magnetic separation of trace amounts of sample, fluorescence detection and imaging applications, including magnetic resonance imaging (MRI) and fluorescence imaging. The fluorescence quenching of the nanospheres in the presence of different amounts of Cu2+ ions was also investigated. Under optimal experimental conditions, the relative fluorescence intensity of the composite nanosphere colloidal solution is proportional to the concentration of Cu2+ ions, which indicates that these multifunctional nanocomposites can be used for the magnetic separation and fluorescence detection of Cu2+ ions. Copyright © 2011 John Wiley & Sons, Ltd.
Co-reporter:Mingliang Deng;Yingxin Ma;Sheng Huang;Gaofei Hu
Nano Research 2011 Volume 4( Issue 7) pp:
Publication Date(Web):2011 July
DOI:10.1007/s12274-011-0124-y
A facile strategy using cheap and readily available precursors has been successfully developed for the synthesis of rare-earth doped hexagonal phase NaYF4 nanocrystals with uniform shape and small particle size as well as strong photoluminescence. Due to their optical properties and good biocompatibility, these multicolor nanocrystals were successfully used as a bio-tag for cancer cell imaging. This novel synthetic method should also be capable of extension to the synthesis of other fluoride nanocrystals such as YF3 and LaF3.
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Co-reporter:Leyu Wang;Yi Zhang;Yanyu Zhu
Nano Research 2010 Volume 3( Issue 5) pp:317-325
Publication Date(Web):2010 May
DOI:10.1007/s12274-010-1035-z
Co-reporter:Hui Li, Huanjie Wang and Leyu Wang
Journal of Materials Chemistry A 2013 - vol. 1(Issue 6) pp:NaN1110-1110
Publication Date(Web):2012/11/21
DOI:10.1039/C2TC00359G
Via a facile one-pot strategy, polyaspartate (PASP) coated LaF3:Ce3+/Tb3+ luminescent nanocrystals have been successfully prepared. Based on the luminescence quenching of the PASP modified LaF3:Ce3+/Tb3+ nanocrystals by Fe3+, a simple and novel luminescent chemosensor for Fe3+ has been developed. High selectivity and sensitivity is observed over other cations, which is mainly attributed to the formation of a PASP–Fe3+ complex on the NP surface. The luminescence of the suspensions was gradually quenched with the addition of Fe3+ ion, with a linear range of 5 × 10−7 to 1 × 10−4 mol L−1.
Co-reporter:Yingxin Ma, Hao Li and Leyu Wang
Journal of Materials Chemistry A 2012 - vol. 22(Issue 36) pp:NaN18767-18767
Publication Date(Web):2012/07/27
DOI:10.1039/C2JM32897F
Luminescent-magnetic multifunctional molecularly imprinted polymer (MIP) nanospheres containing luminescent LaVO4:Eu3+ nanocrystals (NCs), magnetic Fe3O4 nanoparticles (NPs), and the recognition sites of template organophosphate pesticides were successfully prepared via a facile and versatile bottom-up self-assembly strategy. Because of the photoluminescence quenching via diazinon molecules (templates) rebinding into the recognition cavities, these composite MIP nanospheres were successfully applied to the selective and direct luminescence detection of diazinon with the assistance of magnetic separation and concentration. The luminescence intensity was proportional to the concentration of diazinon in the range of 0.01–9.0 μg mL−1 with the 3σ limit of detection (LOD) of 7.1 ng mL−1. This facile and versatile strategy for the MIP nanocomposites is very easy to be extended to other inorganic/organic multifunctional composite nanospheres and will find great potential application as chemical and biological sensors in aqueous media.
Co-reporter:Mingyue An, Jiabin Cui, Qian He and Leyu Wang
Journal of Materials Chemistry A 2013 - vol. 1(Issue 9) pp:NaN1339-1339
Publication Date(Web):2013/01/08
DOI:10.1039/C2TB00469K
Dual-modal luminescence nanocomposites (NCs) were successfully prepared via a facile and versatile strategy by embedding the hydrophobic down-conversion (DC) fluorescence ZnS:Mn2+ quantum dots (QDs) and up-conversion (UC) luminescence NaYF4:Er3+/Yb3+ nanoparticles (NPs) into hydrophilic polymer matrixes through in situ cross-linking polymerization. Due to the enriched carboxylic groups in the polymer matrixes, the as-prepared NCs are highly water-stable and bioconjugatable with chemical and biological moieties. The results of cytotoxicity assay and dual-modal luminescence cell imaging application of DC–UC NCs indicate that the as-prepared NCs are biocompatible and applicable in biomedical fields. The current work paves the way to the fabrication of multifunctional NCs including down- and up-conversion dual-modal luminescence, luminescence–magnetism, magnetic targeted drug vehicles and magnetic recyclable catalyst NCs, and will attract wide attention from the fields of chemistry, materials, catalysis, nanotechnology, nanobiotechnology and nanomedicine.
Co-reporter:Nina Tu and Leyu Wang
Chemical Communications 2013 - vol. 49(Issue 56) pp:NaN6321-6321
Publication Date(Web):2013/05/28
DOI:10.1039/C3CC43146K
We present a novel report on a surface plasmon resonance enhanced upconversion luminescence strategy in aqueous media for highly sensitive and selective detection of 2,4,6-trinitrotoluene (TNT).