Co-reporter:Xiao Deng, Yishan Fang, Sha Lin, Qian Cheng, Qingyun Liu, and Xiaomei Zhang
ACS Applied Materials & Interfaces 2017 Volume 9(Issue 4) pp:
Publication Date(Web):January 9, 2017
DOI:10.1021/acsami.6b15637
Herein, we synthesized a cost-effective iron porphyrin (FePor)-based covalent organic polymer (COP), FePor-TFPA-COP, through an easy aromatic substitution reaction between pyrrole and tris(4-formylphenyl)amine (TFPA). The triangular pyramid-shaped, N-centric structure of TFPA facilitated the formation of FePor-TFPA-COP with three-dimensional porous structure, larger surface area, and abundant surface catalytically active sites. FePor-TFPA-COP exhibited strong intrinsic peroxidase activity toward a classical peroxidase substrate, 3,3′,5,5′-tetramethylbenzidine (TMB), in the presence of H2O2. Compared with horseradish peroxidase (HRP), FePor-TFPA-COP exhibited several advantages such as easy storage, high sensitivity, and prominently chemical and catalytic stability under the harsh conditions, which guaranteed the accuracy and reliability of measurements. Utilizing the excellent catalytic activity, a FePor-TFPA-COP-based colorimetric immunoassay was first established for α-fetoprotein (AFP) detection and showed high sensitivity, stability, and acceptable reproducibility. The linear response range for AFP was 5 pg/mL to 100 ng/mL and the detection limitation was 1 pg/mL. The routine provided a brilliant biomimetic catalyst to develop the nonenzyme immunoassay. More importantly, the high chemical and catalytic stability and sensitivity facilitated future practical applications under various conditions.Keywords: biomimetic catalyst; colorimetric immunoassay; peroxidase-like enzyme; porous organic frameworks; porphyrin;
Co-reporter:Lifang Sun, Yanyuan Ding, Yanling Jiang, Qingyun Liu
Sensors and Actuators B: Chemical 2017 Volume 239() pp:848-856
Publication Date(Web):February 2017
DOI:10.1016/j.snb.2016.08.094
•Well-dispersed CeO2-MMT nanocomposites were prepared by a facile “one-step” method.•CeO2-MMT nanocomposites possess superior intrinsic peroxidase-like activity.•CeO2-MMT nanocomposites provide a platform for the sensitive colorimetric detection of H2O2.•The catalytic mechanism of CeO2-MMT nanocomposites is due to the generated hydroxyl radicals from decomposition of H2O2.An efficient novel colorimetric sensor for H2O2 based on peroxidase-like CeO2-montmorillonite (MMT) nanocomposites that were successfully prepared by a facile one-pot approach, was realized. In comparison with other nanomaterials as peroxidase mimics, the catalytic reaction by the well-dispersed CeO2-MMT nanocomposites was in accordance with typical Michaelis–Menten kinetics, which exhibited a higher affinity to 3,3′,5,5′-tetramethylbenzidine (TMB) and H2O2, bringing about a superior peroxidase-like activity (a distinct blue color change was observed rapidly within 30 s, by the naked eye.) than that of pure CeO2 nanoparticles, MMT and their hybrid materials, respectively. Under the optimized conditions, CeO2-MMT nanocomposites were used to establish a colorimetric biosensor for the detection of H2O2 in a relative wide range of 9 × 10−6 M to 5 × 10−4 M with a lower detection limit of 7.8 × 10−6 M. The sensor was successfully applied in H2O2 detection in milk samples.
Co-reporter:Yanan Ding, Miaomiao Chen, Kaili Wu, Mingxing Chen, Lifang Sun, Zhenxue Liu, Zhiqiang Shi, Qingyun Liu
Materials Science and Engineering: C 2017 Volume 80(Volume 80) pp:
Publication Date(Web):1 November 2017
DOI:10.1016/j.msec.2017.06.020
•PDI-Co3O4 nanocomposites were confirmed to possess the excellent peroxidase-like activity.•The catalytic activity of PDI-Co3O4 nanocomposites was much higher than that of pure Co3O4 nanoparticles.•The catalytic mechanism of PDI-Co3O4 nanocomposites is from the electron transfer between H2O2 and TMB.•PDI-Co3O4 nanocomposites provide a platform for the sensitive colorimetric detection of H2O2 and glucose.N,N′-di-caboxy methyl perylene diimides (PDI), as one of the most promising functional materials in optional chemosensing, was first used to combine with Co3O4 nanoparticles through a facile two-step hydrothermal method and obtain the PDI functionalized Co3O4 nanocomposites (PDI-Co3O4 NCs). PDI-Co3O4 NCs were characterized by a series of technical analysis including transmission electron microscope (TEM), X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FT-IR), respectively. The experimental results indicated that the as-prepared PDI-Co3O4 NCs possessed the higher peroxidase-like activity than that of Co3O4 nanoparticles without PDI, and could rapidly catalyze oxidation reaction of the chromogenic substrate TMB in the presence of H2O2 to a blue product (oxTMB) observed by the naked eye. The improved catalytic activity of PDI-Co3O4 NCs for colorimetric reactions could be attributed to the synergistic effects of PDI and Co3O4 nanoparticles. On the basis of these experimental results, a convenient colorimetric system based on PDI-Co3O4 as enzyme mimic that is highly sensitive and selective was developed for glucose detection. Meanwhile, the electron transfer between H2O2 and TMB was responsible for the oxidation of TMB. The present work demonstrates a general strategy for the design of organic molecules functionalized oxide for different applications, such as nanocatalysts, biosensors and nanomedicine.Download high-res image (76KB)Download full-size image
Co-reporter:Yanan Ding, Miaomiao Chen, Kaili Wu, Mingxing Chen, Lifang Sun, Zhenxue Liu, Zhiqiang Shi, Qingyun Liu
Materials Science and Engineering: C 2017 Volume 80(Volume 80) pp:
Publication Date(Web):1 November 2017
DOI:10.1016/j.msec.2017.06.020
•PDI-Co3O4 nanocomposites were confirmed to possess the excellent peroxidase-like activity.•The catalytic activity of PDI-Co3O4 nanocomposites was much higher than that of pure Co3O4 nanoparticles.•The catalytic mechanism of PDI-Co3O4 nanocomposites is from the electron transfer between H2O2 and TMB.•PDI-Co3O4 nanocomposites provide a platform for the sensitive colorimetric detection of H2O2 and glucose.N,N′-di-caboxy methyl perylene diimides (PDI), as one of the most promising functional materials in optional chemosensing, was first used to combine with Co3O4 nanoparticles through a facile two-step hydrothermal method and obtain the PDI functionalized Co3O4 nanocomposites (PDI-Co3O4 NCs). PDI-Co3O4 NCs were characterized by a series of technical analysis including transmission electron microscope (TEM), X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FT-IR), respectively. The experimental results indicated that the as-prepared PDI-Co3O4 NCs possessed the higher peroxidase-like activity than that of Co3O4 nanoparticles without PDI, and could rapidly catalyze oxidation reaction of the chromogenic substrate TMB in the presence of H2O2 to a blue product (oxTMB) observed by the naked eye. The improved catalytic activity of PDI-Co3O4 NCs for colorimetric reactions could be attributed to the synergistic effects of PDI and Co3O4 nanoparticles. On the basis of these experimental results, a convenient colorimetric system based on PDI-Co3O4 as enzyme mimic that is highly sensitive and selective was developed for glucose detection. Meanwhile, the electron transfer between H2O2 and TMB was responsible for the oxidation of TMB. The present work demonstrates a general strategy for the design of organic molecules functionalized oxide for different applications, such as nanocatalysts, biosensors and nanomedicine.Download high-res image (76KB)Download full-size image
Co-reporter:Miaomiao Chen;Yanan Ding;Yan Gao;Xixi Zhu;Peng Wang;Zhiqiang Shi;Qingyun Liu
RSC Advances (2011-Present) 2017 vol. 7(Issue 41) pp:25220-25228
Publication Date(Web):2017/05/10
DOI:10.1039/C7RA04463A
Nanomaterial-based enzyme mimics (nanoenzymes) are a new forefront of chemical research at present. N,N′-Di-carboxy methyl perylene diimide (PDI) functionalized CuO nanobelts with pores (PDI–CuO nanobelts), which were prepared via a facile method and characterized using various analytical techniques, were demonstrated for the first time to possess higher intrinsic peroxidase-like activity towards classical colorimetric substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of hydrogen peroxide (H2O2), compared with that of pure CuO nanobelts without PDI modification. The underlying reaction mechanism was elucidated by catalyzing the decomposition of H2O2 and generating hydroxyl radicals (˙OH). The improved catalytic activity of PDI–CuO nanobelts for colorimetric reactions could be ascribed to the synergistic effects of CuO and PDI nanobelts. Moreover, the proposed PDI–CuO biosensor platform exhibited a more sensitive response to H2O2 with a low limit of detection (LOD) of 2.38 μM. This convenient sensing platform was further extended to detect glucose in combination with the specificity of glucose oxidase (GOx) for the oxidation of glucose and generation of H2O2. The linear range for glucose detection was from 2 μM to 50 μM with a low detection limit of 0.65 μM. Therefore, besides high sensitivity and selectivity, this colorimetric system also holds considerable potential for biological process research.
Co-reporter:Miaomiao Chen;Lifang Sun;Yanan Ding;Zhiqiang Shi;Qingyun Liu
New Journal of Chemistry (1998-Present) 2017 vol. 41(Issue 13) pp:5853-5862
Publication Date(Web):2017/06/26
DOI:10.1039/C7NJ00292K
In the present study, for the first time, N,N′-di-carboxymethyl perylene diimides (PDI) have been employed to functionalize Fe3O4 nanoparticles via a facile route. The as-prepared PDI–Fe3O4 nanocomposites have been developed as a novel enzyme mimetic and have demonstrated superior peroxidase-like activity to catalyze the oxidation of the peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2 than that of pure Fe3O4 nanoparticles as well as other reported Fe-based peroxidase mimics. In addition, kinetic analysis has revealed that the catalytic reaction was in agreement with the typical Michaelis–Menten kinetics, and the PDI–Fe3O4 nanocomposites displayed a higher affinity towards substrates such as H2O2 and TMB. Moreover, fluorescence data have indicated that the catalytic behavior can be assessed by the electron transfer ability between H2O2 and TMB. Based on the advantages of PDI–Fe3O4 nanocomposites, such as better dispersity, easy separation, enhanced catalytic activity, sensitivity and selectivity for colorimetric detection of glucose, a colorimetric sensor was designed and used for the rapid detection of H2O2 and glucose in a short time.
Co-reporter:Yanyuan Ding, Lifang Sun, Yanling Jiang, Shunxiang Liu, Mingxing Chen, Miaomiao Chen, Yanan Ding, Qingyun Liu
Materials Science and Engineering: C 2016 Volume 67() pp:188-194
Publication Date(Web):1 October 2016
DOI:10.1016/j.msec.2016.05.057
•ZnS nanocomposites deposited on MMT was synthesized by a facile one step method.•MMT-ZnS nanocomposites possess excellent intrinsic peroxidase-like activity and show highly catalytic activity.•A sensitive colorimetric sensor for H2O2 is provided based on MMT-ZnS nanocomposites.•The catalytic mechanism is from the generation of hydroxyl radical (OH) decomposed from H2O2.In this paper, ZnS nanoparticles deposited on montmorillonite (ZnS-MMT) were prepared by a facile method at room temperature and characterized by powder X-ray diffraction (XRD), Energy-dispersive X-ray Detector (EDX) and transmission electron microscope (TEM), respectively. Significantly, the as-prepared ZnS-MMT nanocomposites have been proven to possess intrinsic peroxidase-like activity that can rapidly catalyze the reaction of peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2 and produce a blue color product in less than 30 seconds, which provides a sensitive colorimetric sensor to detect H2O2. Due to the synergistic effects between montmorillonite and ZnS nanoparticles, the obtained ZnS-MMT nanocomposites exhibit higher catalytic activity than that of MMT or ZnS alone. The catalytic behaviors of the ZnS-MMT nanocomposites showed a typical Michaelis–Menten kinetics. The catalytic activity and the catalytic mechanism were investigated using the procedures of steady-state kinetics and hydroxyl radical detection. ESR data revealed that the peroxidase-like activity of ZnS-MMT originated from the generation of OH radicals.
Co-reporter:Qingyun Liu, Yanling Jiang, Leyou Zhang, Xinpei Zhou, Xintian Lv, Yanyuan Ding, Lifang Sun, Pengpeng Chen, Hailiang Yin
Materials Science and Engineering: C 2016 Volume 65() pp:109-115
Publication Date(Web):1 August 2016
DOI:10.1016/j.msec.2016.04.007
•Ag2S – montmorillonites (MMT) was synthesized by a facile one step method.•The as-prepared Ag2S-MMT nanocomposites firstly demonstrate to possess intrinsic peroxidase-like activity.•Ag2S-MMT nanocomposites showed highly catalytic activity.•Ag2S-MMT could rapidly catalytically oxidize substrates TMB in the presence of H2O2 in 1 min.•The catalytic mechanism is from the generation of hydroxyl radical (·OH) decomposed from H2O2.Nanocomposites based on silver sulfide (Ag2S) and Ca-montmorillonite (Ca2 +-MMT) were synthesized by a simple hydrothermal method. The nanocomposites were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM) and Fourier transform infrared spectra (FTIR). The as-prepared Ag2S-MMT nanocomposites were firstly demonstrated to possess intrinsic peroxidase-like activity and could rapidly catalytically oxidize the substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2 to produce a blue product which can be seen by the naked eye in only one minute. The experimental results revealed that the Ag2S-MMT nanocomposites exhibit higher thermal durance. Based on the TMB–H2O2 catalyzed color reaction, the Ag2S-MMT nanocomposites were exploited as a new type of biosensor for detection and estimation of H2O2 through a simple, cheap and selective colorimetric method.
Co-reporter:Jiechao Ge;Qingyan Jia;Weimin Liu;Liang Guo;Qingyun Liu;Minhuan Lan;Hongyan Zhang;Xiangmin Meng;Pengfei Wang
Advanced Materials 2015 Volume 27( Issue 28) pp:4169-4177
Publication Date(Web):
DOI:10.1002/adma.201500323
Co-reporter:Qingyun Liu, Leyou Zhang, Hui Li, Qingyan Jia, Yanling Jiang, Yanting Yang, Renren Zhu
Materials Science and Engineering: C 2015 Volume 55() pp:193-200
Publication Date(Web):1 October 2015
DOI:10.1016/j.msec.2015.05.028
•Porphyrin-functionalized γ-Fe2O3 nanoparticles were prepared by one-pot method.•The porphyrin-γ-Fe2O3 nanocomposites were found to possess intrinsic peroxidase-like activity.•The reaction provides a simple, sensitive and selective method for colorimetric detection of H2O2 and glucose.•The catalase-mimic activity of the porphyrin-γ-Fe2O3 nanocomposites is from the electron transfer mechanism.Meso-tetrakis(4-carboxyphenyl)-porphyrin-functionalized γ-Fe2O3 nanoparticles (H2TCPP-γ-Fe2O3) were successfully prepared by one-pot method under hydrothermal conditions and were found to possess intrinsic peroxidase-like activity. The H2TCPP-γ-Fe2O3 nanocomposites can catalytically oxidize peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2 to produce a blue color reaction, which can be easily observed by the naked eye. Furthermore, kinetic studies indicate that the H2TCPP-γ-Fe2O3 nanocomposites have an even higher affinity to TMB than that of the natural enzyme, horseradish peroxidase (HRP). On the basis of the high activity, the reaction provides a simple, sensitive and selective method for colorimetric detection of H2O2 over a range of 10–100 μM with a minimum detection limit of 1.73 μM. Moreover, H2TCPP-γ-Fe2O3/glucose oxidase (GOx)/TMB system provides a novel colorimetric sensor for glucose and shows good response toward glucose detection over a range of 5–25 μM with a minimum detection limit of 2.54 μM. The results indicated that it is a simple, cheap, convenient, highly selective, sensitive and easy handling colorimetric assay. Results of a fluorescent probe suggest that the catalase-mimic activity of the H2TCPP-γ-Fe2O3 nanocomposites effectively catalyze the decomposition of H2O2 into H2O and O2.5,10,15,20-Tetrakis(4-carboxyl phenyl)-porphyrin (H2TCPP)-γ-Fe2O3 nanocomposites were demonstrated to possess intrinsic peroxidase-like activity and showed a higher catalytic activity, compared to that of γ-Fe2O3 nanoparticles alone.
Co-reporter:Qingyun Liu, Renren Zhu, Yanling Jiang, Leyou Zhang, Hailiang Yin, Shunxiang Liu, Qingyan Jia, Pengpeng Chen
Materials Science and Engineering: B 2015 Volume 198() pp:57-61
Publication Date(Web):August 2015
DOI:10.1016/j.mseb.2015.03.017
•Por-Co3O4 NPs were first prepared via a facile one-pot hydrothermal method.•The yield of porphyrin-Co3O4 nanoparticles is more than 90%.•FT-IR reveals the coordination interaction between porphyin molecules and Co3O4.•Ethanol and the appropriate temperature are necessary in this experiment.Porphyrin functionalized Co3O4 nanoparticles were first prepared via a facile one-pot hydrothermal method. The functionalized nanoparticles were characterized by X-ray diffraction and transmission electron microscopy. Fourier transform infrared spectra revealed the coordination interaction between porphyrin molecules and Co3O4. The high yield of prophyrin functionalized Co3O4 nanoparticles is more than 90%. The phase, morphology and size of as-prepared nanoparticles were dramatically affected by the ratio of solvents, temperature and porphyrins with different substituents, respectively. Experimental results revealed that ethanol and the appropriate temperature were necessary for the formation of single-phase Co3O4. Furthermore, a probable growth mechanism of the formation of porphyrin functionalized Co3O4 nanoparticles was proposed.Porphyrins functionalized Co3O4 nanoparticles were prepared firstly via a facile one-step method. The high yield of prophyrin functionalized Co3O4 nanoparticles is more than 90%.
Co-reporter:Qingyun Liu, Yanting Yang, Hui Li, Renren Zhu, Qian Shao, Shanguang Yang, Jingjing Xu
Biosensors and Bioelectronics 2015 Volume 64() pp:147-153
Publication Date(Web):15 February 2015
DOI:10.1016/j.bios.2014.08.062
•H2TCPP functionalized NiO nanocomposites was prepared by a facile method.•H2TCPP-NiO nanocomposites possess excellent intrinsic peroxidase-like activity.•H2TCPP-NiO nanocomposites showed higher catalytic activity than that of pure NiO NPs.•A sensitive colorimetric sensor for glucose is fabricated based on H2TCPP-NiO nanocomposites.•The generation of hydroxyl radical (·OH) decomposed from H2O2 is contributed to efficient catalytic oxidation of TMB.NiO nanoparticles (NPs) and 5,10,15,20-tetrakis(4-carboxyl pheyl)-porphyrin (H2TCPP) functionalized NiO nanoparticles (H2TCPP-NiO nanocomposites) have been prepared by a facile method and characterized by powder X-ray diffraction (XRD), transmission electron microscope (TEM) and Fourier transform infrared spectra (FTIR), respectively. NiO NPs and H2TCPP-NiO nanocomposites have been proven to function as peroxidase mimetics that can catalyze the reaction of peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2 to produce a blue color reaction. Kinetic analysis indicated that the catalytic behavior was in accord with typical Michaelis–Menten kinetics. And these nanoparticles also exhibited strong affinity for the substrates of 3,3,5,5-tetramethylbiphenyl dihydrochloride (TMB). Experimental results showed that H2TCPP-NiO NPs exhibited a high sensitivity and a low detection limit towards H2O2 (8.0×10−6 M). The H2TCPP-NiO NPs/glucose oxidase (GOx)/TMB system provides a novel colorimetric sensor for glucose and shows good response toward glucose detection over arrange of 0.05–0.50 mM with a limit of detection 2.0×10−5 M. Fluorescence probe experiments demonstrated that the peroxidase-like activity of H2TCPP-NiO NPs originated from the generation of OH radical. Thus it may provide great potential applications in biomedicine, biotechnology and environmental chemistry.
Co-reporter:Qing-Yun Liu, Qing-Yan Jia, Ji-Qin Zhu, Qian Shao, Jun-Feng Fan, Dong-Mei Wang, Yan-Sheng Yin
Chinese Chemical Letters 2014 Volume 25(Issue 5) pp:752-756
Publication Date(Web):May 2014
DOI:10.1016/j.cclet.2013.12.023
meso-Tetrakis(4-aminophenyl)porphyrin (TAPP) can self-assemble into nanostructures with different morphologies by a phase-transfer method. The morphologies (nanospheres, nanorods and nanothorns) of porphyrin nanoaggregates could be easily tuned just by changing the concentration of porphyrin in a proper solvent at room temperature. HRTEM images revealed the formation of highly ordered supramolecular arrays of TAPP, i.e., superlattice of TAPP molecules in nanoaggregates, which agreed well with the size of one molecule of TAPP. UV–vis absorption spectra showed an obvious red shift of the Soret band of TAPP, indicating the formation of J-aggregates of TAPP in nanoaggregates.Highly ordered supramolecular arrays of meso-tetrakis(4-aminophenyl)porphyrin (TAPP) in the formed nanoaggregates, i.e., superlattice of TAPP molecules, which agreed well with the size of one molecule of TAPP.
Co-reporter:Qingyun Liu, Hui Li, Qingru Zhao, Renren Zhu, Yanting Yang, Qingyan Jia, Bing Bian, Linhai Zhuo
Materials Science and Engineering: C 2014 Volume 41() pp:142-151
Publication Date(Web):1 August 2014
DOI:10.1016/j.msec.2014.04.038
•H2TCPP-Fe3O4 nanocomposites exhibite ultra-high peroxidase-like activity.•A novel colorimetric sensor for glucose with a lower detection limit is provided.•The catalase-mimic activity of the H2TCPP-Fe3O4 nanocomposites originates from OH · .•H2TCPP-Fe3O4 nanocomposites show high sensitivity, selectivity and high stability.5,10,15,20-Tetrakis(4-carboxyphenyl)-porphyrin-functionalized Fe3O4 nanocomposites (H2TCPP-Fe3O4) were successfully prepared by a simple two-step method. These nanocomposites exhibited ultra-high peroxidase-like activity compared with pure Fe3O4 nanoparticles. Colorless peroxidase substrate 3,3,5,5-tetramethylbenzidine (TMB) was changed by H2O2 to its blue oxidized state. Kinetic studies indicated that the H2TCPP-Fe3O4 nanocomposites exhibited enhanced affinity toward H2O2 with a higher catalytic activity than Fe3O4 nanoparticles alone. Results of a fluorescent probe suggested that the catalase-mimic activity of the H2TCPP-Fe3O4 nanocomposites effectively catalyzed the decomposition of H2O2 into hydroxyl radicals. A simple, sensitive, and selective visual and colorimetric method with TMB as the substrate was designed to detect glucose when combined with glucose oxidase. This colorimetric method can be used for colorimetric detection of H2O2 with a minimum detection limit of 1.07 × 10− 6 M and a dynamic range of 5 × 10− 6 mol · L− 1 to 8 × 10− 5 mol · L− 1. This method can also be used to detect glucose at a minimum detection limit of 2.21 × 10− 6 M and a dynamic range of 25 × 10− 6 mol · L− 1 to 5 × 10− 6 mol · L− 1. Furthermore, the robustness of the nanocomposites makes them suitable for a wide range of applications in biomedicine and environmental chemistry fields.5,10,15,20-tetrakis(4-carboxyl phenyl)-porphyrin (H2TCPP)-Fe3O4 nanocomposites were demonstrated to possess intrinsic peroxidase-like activity and a higher catalytic activity, compared to that of Fe3O4 NPs alone.
Co-reporter:Hangyue Zhou; Qingyun Liu; Weimin Liu; Jiechao Ge;Dr. Minhuan Lan; Chao Wang; Jianxin Geng; Pengfei Wang
Chemistry – An Asian Journal 2014 Volume 9( Issue 3) pp:811-818
Publication Date(Web):
DOI:10.1002/asia.201301428
Abstract
Volvox-like CdxZn1−xS solid solutions with a cubic zinc blend structure were synthesized through a template-free ethylene glycol process. Cd(Ac)2⋅2 H2O, Zn(Ac)2⋅2 H2O, and thiourea are used as the starting materials and dissolved in ethylene glycol. These reaction precursors and solvent not only contributed to control over the formation of the volvox-like spherical geometry, but also exerted vigorous domination for existence of cubic-phase CdxZn1−xS nanostructures. As-prepared volvox-like CdxZn1−xS nanospheres have a diameter of around 100 nm with extensional shells. These samples show excellent photocatalytic H2 evolution activity from water splitting under visible-light irradiation without any cocatalyst or scaffolding, owing to their tunable band gap, cubic zinc blend structure, and unique hierarchical porous structure with a high surface area (as high as 95.2 m2 g−1).
Co-reporter:Qingyun Liu, Renren Zhu, Hui Du, Hui Li, Yanting Yang, Qingyan Jia, Bing Bian
Materials Science and Engineering: C 2014 Volume 43() pp:321-329
Publication Date(Web):1 October 2014
DOI:10.1016/j.msec.2014.07.032
•H2TCPP-Co3O4 nanocomposites was synthesized by a facile two step method.•H2TCPP-Co3O4 nanocomposites possess excellent intrinsic peroxidase-like activity.•H2TCPP-Co3O4 nanocomposites showed higher catalytic activity than pure Co3O4 NPs.•A sensitive colorimetric sensor for glucose is provided based on our nanomaterials.•The hydroxyl radical decomposed from H2O2 is contributed to efficient catalytic.5,10,15,20-Tetrakis(4-carboxyl pheyl)-porphyrin (H2TCPP) functionalized chain-like Co3O4 nanoparticles (NPs) were prepared by a facile two-step method. The H2TCPP–Co3O4 nanocomposites were demonstrated to display enhanced peroxidase-like activity than that of pure Co3O4 nanoparticles without modification with H2TCPP molecules, catalyzing oxidation of peroxidase substrate 3,3′,5,5′-tetramethyl-benzidine (TMB) in the presence of H2O2 to produce a blue color reaction. Furthermore, H2TCPP–Co3O4 nanocomposites showed typical Michaelis–Menten kinetics and higher affinity to H2O2 and TMB than that of pure Co3O4 NPs alone. Based on H2TCPP–Co3O4 nanocomposites, a simple, sensitive and selective colorimetric method with TMB as the substrate for the detection of H2O2 and glucose was successfully established. This colorimetric method can be used for the colorimetric detection of H2O2 with a low detection limit of 4 × 10− 7 mol·L− 1 and a dynamic range of 1 × 10− 6 mol·L− 1 to 75 × 10− 6 mol·L− 1. This method was designed to detect glucose when combined with glucose oxidase at a low detection limit of 8.6 × 10− 7 mol·L− 1 and a dynamic range of 1 × 10− 6 mol·L− 1 to 10 × 10− 6 mol·L− 1. Results of a fluorescent probe suggested that the peroxidase-mimic activity of the H2TCPP–Co3O4 nanocomposites effectively catalyzed the decomposition of H2O2 into [OH] radicals.5,10,15,20-Tetrakis(4-carboxyl phenyl)-porphyrin functionalized Co3O4 nanocomposites (H2TCPP–Co3O4 NCs) were demonstrated to exhibit more excellent intrinsic peroxidase-like activity with higher catalytic activity than that of pure Co3O4 NPs and the sensitive detection limit for glucose determination was as low as 8.6 × 10− 7 M.
Co-reporter:Qingyun Liu, Qingyan Jia, Renren Zhu, Qian Shao, Dongmei Wang, Peng Cui, Jiechao Ge
Materials Science and Engineering: C 2014 Volume 42() pp:177-184
Publication Date(Web):1 September 2014
DOI:10.1016/j.msec.2014.05.019
•H2TCPP–CdS nanocomposites were synthesized by a facile one step under mild condition.•H2TCPP–CdS nanocomposites possess excellent intrinsic peroxidase-like activity.•A sensitive and selective colorimetric sensor for glucose is provided based on H2TCPP–CdS nanocomposites.•The generation of hydroxyl radical (·OH) decomposed from H2O2 is contributed to efficient catalytic.Here, we describe the design of a novel mimic peroxidase, nanocomposites composed by 5,10,15,20-tetrakis(4-carboxyl phenyl)-porphyrin (H2TCPP) and cadmium sulfide (CdS). The H2TCPP–CdS nanocomposites can catalyze oxidation of substrate 3,3,5,5-tetramethylbenzidine (TMB) in the presence of H2O2 and form a blue product which can be seen by the naked eye in 5 min. The mechanism of the catalytic reaction originated from the generation of hydroxyl radical (·OH), which is a powerful oxidizing agent to oxidize TMB to produce a blue product. Then, we developed a colorimetric method that is highly sensitive and selective to detect glucose, combined with glucose oxidase (GOx). The proposed method allowed the detection of H2O2 concentration in the range of 4 × 10− 6–1.4 × 10− 5 M and glucose in the range of 1.875 × 10− 5–1 × 10− 4 M with detectable H2O2 concentration as low as 4.6 × 10− 7 M and glucose as low as 7.02 × 10− 6 M, respectively. The results provided the theoretical basis of practical application in glucose detecting and peroxidase mimetic enzymes.5,10,15,20-tetrakis(4-carboxyl phenyl)-porphyrin (H2TCPP)–CdS nanohybrids were demonstrated to possess intrinsic peroxidase-like activity and used for a glucose colorimetric sensor.
Co-reporter:Qingyun Liu, Renren Zhu, Yanling Jiang, Qingyan Jia, Shanguang Yang, Qian Shao, Dongmei Wang, Peng Cui
Materials Science and Engineering: B 2014 Volume 188() pp:106-113
Publication Date(Web):October 2014
DOI:10.1016/j.mseb.2014.05.002
•H2TCPP-CdS NCs were prepared by a facile one-step method under mild conditions.•H2TCPP-CdS NCs exhibited the high photocatalytic degradation activity toward RhB.•The photocatalytic activity of H2TCPP-CdS NCs irradiated by solar light is higher than when irradiated by UV light.•H2TCPP-CdS NCs exhibited good stability and reutilization.The 5,10,15,20-tetrakis (4-carboxyl phenyl)-porphyrin-functionalized CdS nanocomposites (H2TCPP-CdS NCs) were successfully prepared by a facile one-step method under mild conditions and were extensively characterized by X-ray diffraction, transmission electron microscopy, Fourier transform infrared spectroscopy, UV–vis diffuse reflectance. Rhodamine B (RhB) dye, a common industrial pollutant, was used as a model pollutant to study its photocatalytic activity under exposure to solar light. The results showed that the as-prepared H2TCPP-CdS NCs exhibited enhanced photocatalytic activity for the degradation of RhB dissolved in water under exposure to solar light. The degradation efficiency of RhB catalyzed by the H2TCPP-CdS NCs under exposure to solar light is higher than when exposed to UV light. The degradation and decolorization of RhB were influenced by different amounts of porphyrin in preparation of H2TCPP-CdS NCs, the amount of catalyst, and the initial concentration of dye solution and pH. Moreover, the recycling experiments confirmed the relative stability and reutilization of the catalyst.5,10,15,20-tetrakis(4-carboxyl phenyl)-porphyrin functionalized CdS nanocomposites (H2TCPP-CdS NCs) were prepared by a facile method under mild conditions and were demonstrated to exhibit higher photocatalytic degradation activity toward Rhodamine B (RhB) irradiated by solar light than that irradiated by UV light. It is clear that the intense red color of the starting solution gradually disappears with increasingly longer exposure time.
Co-reporter:Qingyun Liu, Hangyue Zhou, Jiqin Zhu, Yanting Yang, Xiaodong Liu, Dongmei Wang, Xiaomei Zhang, Linhai Zhuo
Materials Science and Engineering: C 2013 Volume 33(Issue 8) pp:4944-4951
Publication Date(Web):1 December 2013
DOI:10.1016/j.msec.2013.08.015
•Temperature dependent aggregates of H2TCPP can be fabricated by self-assembly method.•The aggregate properties transformed from H to J aggregates with different speed.•A possible explanation for the formation of nanoaggregates has been proposed.•Fluorescence spectra revealed a greater fluorescence quenching of nanoaggregates.Various nanostructures of 5,10,15,20-tetrakis(4-carboxyl phenyl)-porphyrin (H2TCPP) can be easily synthesized by a surfactant-assisted self-assembly (SAS) method at different temperatures. When the DMF solution of porphyrin monomer was injected into cetyltimethylammonium bromide (CTAB) aqueous solution by a syringe, diverse H2TCPP nanostructures dependent on the different temperatures, including hollow nanospheres, solid nanospheres and nanospheres with holes, were successfully obtained. As a result, the suitable concentration of the CTAB aqueous solution used to form nanostructues of porphyrin ranges from 0.15 to 0.2 mM. The various morphologies of porphyrin nanostructures were characterized by transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM) and scanning electron microscopy (SEM). UV–vis adsorption spectra showed that the micro-/nano-aggregate properties of porphyrin transformed from H-aggretates to J-aggregates during the process of self-assembly of porphyrin at different temperatures. Fluorescence spectra revealed a greater fluorescence quenching of various micro-/nano-aggregatess of porphyrin formed at different temperatures in aqueous solution, compared to the DMF solution of porphyrin monomer.Temperature dependent morphologies of nanoaggregates of 5,10,15,20-tetra(4-carboxyl phenyl)-porphyrin (H2TCPP) can be easily prepared by a surfactant-assisted self-assembly method.