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学者姓名：唐点平
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Abstract ：
The volumetric density of the metal atomic site is decisive to the operating efficiency of the photosynthetic nanoreactor, yet its rational design and synthesis remain a grand challenge. Herein, we report a shell-regulating approach to enhance the volumetric density of Co atomic sites onto/into multishell ZnxCd1-xS for greatly improving CO2 photoreduction activity. We first establish a quantitative relation between the number of shell layers, specific surface areas, and volumetric density of atomic sites on multishell ZnxCd1-xS and conclude a positive relation between photosynthetic performance and the number of shell layers. The triple-shell ZnxCd1-xS-Co-1 achieves the highest CO yield rate of 7629.7 mu mol g(-1) h(-1), superior to those of the double-shell ZnxCd1-xS-Co-1 (5882.2 mu mol g(-1) h(-1)) and single-shell ZnxCd1-xS-Co-1 (4724.2 mu mol g(-1) h(-1)). Density functional theory calculations suggest that high-density Co atomic sites can promote the mobility of photogenerated electrons and enhance the adsorption of Co(bpy)(3)(2+) to increase CO2 activation (CO2 -> CO2* -> COOH* -> CO* -> CO) via the S-Co-bpy interaction, thereby enhancing the efficiency of photocatalytic CO2 reduction.
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| GB/T 7714 | Zeng, Ruijin , Liu, Tongyu , Qiu, Minghao et al. High-Volumetric Density Atomic Cobalt on Multishell Zn x Cd1-x S Boosts Photocatalytic CO2 Reduction [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (14) : 9721-9727 . |
| MLA | Zeng, Ruijin et al. "High-Volumetric Density Atomic Cobalt on Multishell Zn x Cd1-x S Boosts Photocatalytic CO2 Reduction" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146 . 14 (2024) : 9721-9727 . |
| APA | Zeng, Ruijin , Liu, Tongyu , Qiu, Minghao , Tan, Hao , Gu, Yu , Ye, Na et al. High-Volumetric Density Atomic Cobalt on Multishell Zn x Cd1-x S Boosts Photocatalytic CO2 Reduction . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (14) , 9721-9727 . |
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Background: Measurement of endogenous cellular hydrogen peroxide (H2O2) can provide information on cellular status, and help to understand cellular metabolism and signaling processes, thus contributing to elucidation of disease mechanisms and new diagnostics/therapeutic approaches. Results: In this work, Pt–Cd bimetallic nanozyme was successfully prepared via the solvothermal synthetic method for sensitive detection of H2O2. The synthesized Pt–Cd bimetallic nanozyme could exhibited good electrochemical activity. Then, the materials were analyzed for the electrochemical properties and catalytic properties of H2O2 by cyclic voltammetry and chronoamperometry, respectively. Results indicated that the synthesized nanozyme had superior sensitivity (295 μA⸳mM−1⸳cm−2) and selectivity toward H2O2 with a detection limit of 0.21 μM. Further, the Pt–Cd bimetallic nanozyme displayed good electrochemical properties compared to platinum catalysts alone. The application was extended to determine the produced H2O2 from human hepatocellular carcinoma cells (HepG2) and normal hepatocyte (LO2) samples after ascorbic acid stimulation, thus enabling the early warning of cellular carcinogenesis. Significance: This strategy promises simple, rapid, inexpensive and effective electrochemical sensing and provides a new pathway for the synthesis of bimetallic nanozymes to construct an electrochemical sensor for the sensitive detection of H2O2. © 2024 Elsevier B.V.
Keyword ：
Enzyme-free electrochemical sensor Enzyme-free electrochemical sensor Hepatocellular carcinoma cells Hepatocellular carcinoma cells Intracellularly-originated hydrogen peroxide Intracellularly-originated hydrogen peroxide Pt–Cd bimetallic nanozyme Pt–Cd bimetallic nanozyme
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| GB/T 7714 | Xu, M. , Yu, Z. , Wei, Q. et al. Probing trace of intracellularly-originated hydrogen peroxide based Pt–Cd bimetallic nanozyme on an enzyme-free electrochemical sensor [J]. | Analytica Chimica Acta , 2024 , 1324 . |
| MLA | Xu, M. et al. "Probing trace of intracellularly-originated hydrogen peroxide based Pt–Cd bimetallic nanozyme on an enzyme-free electrochemical sensor" . | Analytica Chimica Acta 1324 (2024) . |
| APA | Xu, M. , Yu, Z. , Wei, Q. , Tang, D. . Probing trace of intracellularly-originated hydrogen peroxide based Pt–Cd bimetallic nanozyme on an enzyme-free electrochemical sensor . | Analytica Chimica Acta , 2024 , 1324 . |
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Polymetallic high -entropy nanosulfide with controlled morphology can provide high stability and sensitivity for photoelectrochemical (PEC) immunoassays due to their fascinating cocktail effect and highly customizable electrochemical properties. Most currently available methods require extremely high temperatures to homogeneously mix the different components, which further limits their large-scale synthesis. Herein, a high -entropy nanosulfide (ZnCdCuAgCo) x S with cocktail effect was prepared by mild cation exchange reactions. Initially, (ZnCdCuAgCo) x S was an excellent semiconductor that functioned as a photovoltaic material to be loaded on the electrode surface because of the synergistic effect between different metals. A sandwich -type immunoreaction has been performed in 96 -well microtiter plate, linking with the detection antibody modified with glucose oxidase-loaded gold nanoparticles. In the presence of prostate -specific antigen (PSA), enzymatically produced H 2 O 2 consumed electrons on the conduction band of (ZnCdCuAgCo) x S to generate H 2 O, leading to a decrease in the photocurrent of the system. The PEC immunoassay based on (ZnCdCuAgCo) x S displayed high sensitivity for PSA with a linear range of 0.03 -10 ng mL -1 and a low detection limit of 9.62 pg mL -1 . More importantly, the results of clinical serum specimens obtained by this PEC immunoassay are in great agreement with those of the enzyme -linked immunosorbent assay.
Keyword ：
Cation exchange reaction Cation exchange reaction Cocktail effect Cocktail effect High -entropy nanosulfide (ZnCdCuAgCo) x S High -entropy nanosulfide (ZnCdCuAgCo) x S Photoelectrochemical immunoassay Photoelectrochemical immunoassay Prostate -specific antigen Prostate -specific antigen
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| GB/T 7714 | Wan, Xinyu , Tang, Dianyong , Wang, Haiyang et al. High-entropy (ZnCdCuAgCo) x S-triggered cocktail effect with cation-exchange reaction for in-situ amplified photoelectrochemical immunoassay [J]. | SENSORS AND ACTUATORS B-CHEMICAL , 2024 , 412 . |
| MLA | Wan, Xinyu et al. "High-entropy (ZnCdCuAgCo) x S-triggered cocktail effect with cation-exchange reaction for in-situ amplified photoelectrochemical immunoassay" . | SENSORS AND ACTUATORS B-CHEMICAL 412 (2024) . |
| APA | Wan, Xinyu , Tang, Dianyong , Wang, Haiyang , Wang, Xin , Tang, Dianping . High-entropy (ZnCdCuAgCo) x S-triggered cocktail effect with cation-exchange reaction for in-situ amplified photoelectrochemical immunoassay . | SENSORS AND ACTUATORS B-CHEMICAL , 2024 , 412 . |
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A colorimetric and photothermal dual-mode detection method based on beta-NiOOH nanozyme-3,3 ',5,5 '-tetramethylbenzidine (TMB) system was established for chloramphenicol (CAP) content in fruit juice. Herein, a novel nanozyme beta-NiOOH with high oxidase-like activity can directly and effectively catalyze the oxidation of colorless TMB to blue color TMB oxidation (oxTMB) without the presence of H2O2. Using a competition-type immunoassay, the oxTMB can induce not only an increase in the absorption peak intensity but also a photothermal effect under 808 nm laser irradiation, achieving dual-mode detection of CAP. The increase of absorbance at 652 nm and the increase of temperature generated by photothermal conversion are linearly correlated with the CAP content. Under the optimal conditions, the dual-mode detection shows a low limit of 0.0056 ng mL-1 for the colorimetric method, and 0.0016 ng mL-1 for the photothermal method. Moreover, the developed colorimetric and photothermal dual-mode immunobiosensor was successfully used to detect CAP in fruit juice with an acceptable recovery rate between 93.387% and 118.514%. This method has good repeatability, specificity, and accuracy, and provides an efficient approach for real-time detection of CAP in food safety analysis and detection platforms. A colorimetric and photothermal dual-mode detection method based on beta-NiOOH nanozyme-3,3 ',5,5 '-tetramethylbenzidine system was established for chloramphenicol content in fruit juice.
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| GB/T 7714 | Lian, Yuxing , Zheng, Mengqin , Li, Suhua et al. A colorimetric and photothermal dual-mode immunobiosensor for chloramphenicol based on the β-NiOOH nanozyme-3,3′,5,5′-tetramethylbenzidine system [J]. | NEW JOURNAL OF CHEMISTRY , 2024 , 48 (16) : 7340-7346 . |
| MLA | Lian, Yuxing et al. "A colorimetric and photothermal dual-mode immunobiosensor for chloramphenicol based on the β-NiOOH nanozyme-3,3′,5,5′-tetramethylbenzidine system" . | NEW JOURNAL OF CHEMISTRY 48 . 16 (2024) : 7340-7346 . |
| APA | Lian, Yuxing , Zheng, Mengqin , Li, Suhua , Lai, Wenqiang , Tang, Dianping , Lin, Youxiu . A colorimetric and photothermal dual-mode immunobiosensor for chloramphenicol based on the β-NiOOH nanozyme-3,3′,5,5′-tetramethylbenzidine system . | NEW JOURNAL OF CHEMISTRY , 2024 , 48 (16) , 7340-7346 . |
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Early detection of cancer has a profound impact on patient survival and treatment outcomes considering high treatment success rates and reduced treatment complexity. Here, we developed a portable photoelectrochemical (PEC) immune platform for sensitive testing of alpha-fetoprotein (AFP) based on Pt nanocluster (Pt NCs) loaded defective -state g-C3N4 photon -electron transducers. The broad forbidden band structure of g-C3N4 was optimized by the nitrogen doping strategy and additional homogeneous porous structure was introduced to further enhance the photon utilization. In addition, the in -situ growth of Pt NCs provided efficient electron transfer catalytic sites for sacrificial agents, which were used to further improve the sensitivity of the sensor. Efficient photoelectric conversion under a hand-held flashlight was determined by the geometry of the transducer and the energy band design, and the portable design of the PEC sensor was realized. The developed sensing platform exhibited a wide linear response range (0.1-50 ng mL-1) and low limit of detection (0.043 ng mL-1) for AFP under optimum conditions. This work provides a new idea for designing portable PEC biosensing platforms to meet the current mainstream POC testing needs.
Keyword ：
Alpha-fetoprotein Alpha-fetoprotein Micro-electro-mechanical-system Micro-electro-mechanical-system Photoelectrochemical immunoassay Photoelectrochemical immunoassay Platinum nanoclusters Platinum nanoclusters
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| GB/T 7714 | Lou, Fangming , Wang, Shaojie , Han, Bo et al. Portable photoelectrochemical immunoassay with micro-electro-mechanical-system for alpha-fetoprotein in hepatocellular carcinoma [J]. | ANALYTICA CHIMICA ACTA , 2024 , 1298 . |
| MLA | Lou, Fangming et al. "Portable photoelectrochemical immunoassay with micro-electro-mechanical-system for alpha-fetoprotein in hepatocellular carcinoma" . | ANALYTICA CHIMICA ACTA 1298 (2024) . |
| APA | Lou, Fangming , Wang, Shaojie , Han, Bo , Li, Qunfang , Tang, Dianping . Portable photoelectrochemical immunoassay with micro-electro-mechanical-system for alpha-fetoprotein in hepatocellular carcinoma . | ANALYTICA CHIMICA ACTA , 2024 , 1298 . |
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Carcinoembryonic antigen (CEA), a vital biomarker, plays a significant role in the early diagnosis and prognostic estimation of malignant tumors. In this study, a split-type photoelectrochemical immunoassay for the sensitive quantification of CEA has been successfully developed based on the target-induced in situ formation of a Z-type heterojunction. First, gold nanoparticle-decorated ZnIn2S4 (AuNPs/ZnIn2S4) composites were synthesized and used for the fabrication of photoelectrodes. Then, the detection antibody labeled with Ag nanoparticles was formed and applied for the biorecognition of CEA and subsequent liberation of Ag+ ions to induce the in situ formation of Ag2S/AuNPs/ZnIn2S4, a Z-type heterojunction, on the photoelectrode. The Z-type Ag2S/AuNPs/ZnIn2S4 heterojunction with effectively promoted separation of photogenerated charge carriers could lead to a markedly enhanced photocurrent response and highly sensitive quantification of CEA. Moreover, the three-dimensional spatial structure of ZnIn2S4 provides abundant active sites for the reaction and exhibits non-enzymatic properties, which are conducive to the further improvement of the analytical performance of CEA. The developed split-type photoelectrochemical immunoassay with good sensitivity, satisfactory selectivity, reliable stability, wide dynamic linear range (0.01-20 ng mL(-1)), and low detection limit (7.3 pg mL(-1)) offers valuable insights into the development of novel PEC biosensing models for the detection of tumor biomarkers and holds potential application value in the field of disease diagnosis.
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| GB/T 7714 | Zhang, Jianhui , Tan, Meirong , Chen, Qian et al. Split-type photoelectrochemical immunoassay for sensitive quantification of carcinoembryonic antigen based on target-induced in situ formation of Z-type heterojunction [J]. | ANALYTICAL METHODS , 2024 , 16 (13) : 1901-1907 . |
| MLA | Zhang, Jianhui et al. "Split-type photoelectrochemical immunoassay for sensitive quantification of carcinoembryonic antigen based on target-induced in situ formation of Z-type heterojunction" . | ANALYTICAL METHODS 16 . 13 (2024) : 1901-1907 . |
| APA | Zhang, Jianhui , Tan, Meirong , Chen, Qian , Zhang, Kangyao , Zhou, Qian , Lai, Wenqiang et al. Split-type photoelectrochemical immunoassay for sensitive quantification of carcinoembryonic antigen based on target-induced in situ formation of Z-type heterojunction . | ANALYTICAL METHODS , 2024 , 16 (13) , 1901-1907 . |
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Different from prevalent approaches such as immunological recognition, complementary base pairing, or enzymatic regulation in current photoelectrochemical (PEC) sensing, this study reported an excited-state intramolecular proton transfer (ESIPT)-driven photon-gating PEC sensor. The sensor is developed for the detection of CO-releasing molecule-3 (CORM-3) by modifying an ESIPT-switched organic fluorescent probe molecule (NDAA) onto the surface of a p-type semiconductor (BiOI). The NDAA can be excited and exhibit strong green fluorescence after responding with CORM-3, resulting in an electrode-interface photon competitive absorption effect due to the switch on ESIPT and considerably reducing the photocurrent signal. The experimental results revealed that the as-developed PEC sensor achieved good analytical performance with high selectivity and sensitivity, with a linear range of 0.01-1000 mu M and a lower detection limit of 6.5 nM. This work demonstrates the great potential of the organic fluorescent probe molecule family in advancing PEC analysis. It is anticipated that our findings will stimulate the creation of diverse functional probes possessing distinctive characteristics for inventive PEC sensors.
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| GB/T 7714 | Gao, Yuan , Tang, Juan , Zhou, Qian et al. Excited-State Intramolecular Proton Transfer-Driven Photon-Gating for Photoelectrochemical Sensing of CO-Releasing Molecule-3 [J]. | ANALYTICAL CHEMISTRY , 2024 , 96 (12) : 5014-5021 . |
| MLA | Gao, Yuan et al. "Excited-State Intramolecular Proton Transfer-Driven Photon-Gating for Photoelectrochemical Sensing of CO-Releasing Molecule-3" . | ANALYTICAL CHEMISTRY 96 . 12 (2024) : 5014-5021 . |
| APA | Gao, Yuan , Tang, Juan , Zhou, Qian , Yu, Zhichao , Wu, Di , Tang, Dianping . Excited-State Intramolecular Proton Transfer-Driven Photon-Gating for Photoelectrochemical Sensing of CO-Releasing Molecule-3 . | ANALYTICAL CHEMISTRY , 2024 , 96 (12) , 5014-5021 . |
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A colorimetric immunoassay was built for determination of carcinoembryonic antigen (CEA) based on papain-based colorimetric catalytic sensing system through the use of glucose oxidase (GOx). In the presence of GOx, glucose was catalytically oxidized to produce H 2 O 2 . Through the assistance of papain (as a peroxide mimetic enzyme), the signal came from the oxidative color development of 3,3 ',5,5 '-tetramethylbenzidine (TMB, from colorless to blue) catalyzed by the generated H 2 O 2 . Herein, a sandwich -type immunoassay was built based on GOx as labels. As the concentration of CEA increased, more GOx-labeled antibodies specifically associate with target, which leaded to more H 2 O 2 generation. Immediately following this, more TMB were oxidized with the addition of papain. Accordingly, the absorbance increased further. As a result, the concentration of CEA is positively correlated with the change in absorbance of the solution. Under optimal conditions, the CEA concentration was linear in the range of 0.05 -20.0 ng/mL, and the limit of detection (LOD) reached 37 pg/mL. The papain-based colorimetric immunoassay also exhibited satisfactory repeatability, stability, and selectivity.
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| GB/T 7714 | Li, Xiaoqin , Lu, Xiaoxue , Zhang, Linyu et al. A papain-based colorimetric catalytic sensing system for immunoassay detection of carcinoembryonic antigen [J]. | SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY , 2024 , 315 . |
| MLA | Li, Xiaoqin et al. "A papain-based colorimetric catalytic sensing system for immunoassay detection of carcinoembryonic antigen" . | SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY 315 (2024) . |
| APA | Li, Xiaoqin , Lu, Xiaoxue , Zhang, Linyu , Cai, Zhixiong , Tang, Dianping , Lai, Wenqiang . A papain-based colorimetric catalytic sensing system for immunoassay detection of carcinoembryonic antigen . | SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY , 2024 , 315 . |
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Pressure and temperature, as common physical parameters, are important for monitoring human health. In contrast, single-mode monitoring is prone to causing experimental errors. Herein, we innovatively designed a dual-mode flexible sensing platform based on a platinum/zinc-meso-tetrakis(4-carboxyphenyl)porphyrin (Pt/Zn-TCPP) nanozyme for the quantitative monitoring of carcinoembryonic antigen (CEA) in biological fluids with pressure and temperature readouts. The Pt/Zn-TCPP nanozyme with catalytic and photothermal efficiencies was synthesized by means of integrating photosensitizers into porous materials. The flexible sensing system after the antigen-antibody reaction recognized the pressure using a flexible skin-like pressure sensor with a digital multimeter readout, whereas the temperature was acquired via the photoheat conversion system of the Pt/Zn-TCPP nanozyme under 808 nm near-infrared (NIR) irradiation using a portable NIR imaging camera on a smartphone. Meanwhile, the dual-mode flexible sensing system was carried out on a homemade three-dimensional (3D)-printed device. Results revealed that the developed dual-mode immunosensing platform could exhibit good pressure and temperature responses within the dynamic range of 0.5-100 ng mL-1 CEA with the detection limits of 0.24 and 0.13 ng mL-1, respectively. In addition, the pressure and temperature were sensed simultaneously without crosstalk interference. Importantly, the dual-mode flexible immunosensing system can effectively avoid false alarms during the measurement, thus providing great potential for simple and low-cost development for point-of-care testing.
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| GB/T 7714 | Wu, Di , Tang, Juan , Yu, Zhichao et al. Pt/Zn-TCPP Nanozyme-Based Flexible Immunoassay for Dual-Mode Pressure-Temperature Monitoring of Low-Abundance Proteins [J]. | ANALYTICAL CHEMISTRY , 2024 . |
| MLA | Wu, Di et al. "Pt/Zn-TCPP Nanozyme-Based Flexible Immunoassay for Dual-Mode Pressure-Temperature Monitoring of Low-Abundance Proteins" . | ANALYTICAL CHEMISTRY (2024) . |
| APA | Wu, Di , Tang, Juan , Yu, Zhichao , Gao, Yuan , Zeng, Yongyi , Tang, Dianping et al. Pt/Zn-TCPP Nanozyme-Based Flexible Immunoassay for Dual-Mode Pressure-Temperature Monitoring of Low-Abundance Proteins . | ANALYTICAL CHEMISTRY , 2024 . |
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Single-atom nanozyme-based catalytic therapy is of great interest in the field of tumor catalytic therapy; however, their development suffers from the low affinity of nanozymes to the substrates (H2O2 or O-2), leading to deficient catalytic activity in the tumor microenvironment. Herein, we report a new strategy for precisely tuning the d-band center of dual-atomic sites to enhance the affinity of metal atomic sites and substrates on a class of edge-rich N-doped porous carbon dual-atomic sites Fe-Mn (Fe1Mn1-NCe) for greatly boosting multiple-enzyme-like catalytic activities. The as-made Fe1Mn1-NCe achieved a much higher catalytic efficiency (K-cat/K-m = 4.01 x 10(5) S-1M-1) than Fe-1-NCe (K-cat/K-m = 2.41 x 10(4) S-1 center dot M-1) with an outstanding stability of over 90% activity retention after 1 year, which is the best among the reported dual-atom nanozymes. Theoretical calculations reveal that the synergetic effect of Mn upshifts the d-band center of Fe from -1.113 to -0.564 eV and enhances the adsorption capacity for the substrate, thus accelerating the dissociation of H2O2 and weakening the O-O bond on O-2. We further demonstrated that the superior enzyme-like catalytic activity of Fe1Mn1-NCe combined with photothermal therapy could effectively inhibit tumor growth in vivo, with an inhibition rate of up to 95.74%, which is the highest value among the dual-atom artificial enzyme therapies reported so far.
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| GB/T 7714 | Zeng, Ruijin , Gao, Qian , Xiao, Limei et al. Precise Tuning of the D-Band Center of Dual-Atomic Enzymes for Catalytic Therapy [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (14) : 10023-10031 . |
| MLA | Zeng, Ruijin et al. "Precise Tuning of the D-Band Center of Dual-Atomic Enzymes for Catalytic Therapy" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146 . 14 (2024) : 10023-10031 . |
| APA | Zeng, Ruijin , Gao, Qian , Xiao, Limei , Wang, Weijun , Gu, Yu , Huang, Hengshuo et al. Precise Tuning of the D-Band Center of Dual-Atomic Enzymes for Catalytic Therapy . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (14) , 10023-10031 . |
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