ANALYST
·
2021
·Vol. 146
·期 17
·5403-5412
·
IF 4.616
Shiying Zhou,Xianfeng Wang,Liuyi Jiang,Human Sun,Danqun Huo,Changjun Hou
Two different electrochemical sensors (Hemin-G4/Au/GCE and Hemin-G4/Au/ITO) were developed and applied to explore the electrocatalytic capacity of H2O2 reduction. Due to the excellent catalytic activity of Hemin-G4 and high conductivity of gold nanoparticles, both electrodes show excellent electrochemical performances towards H2O2 with a low LOD (0.67 μM for Hemin-G4/Au/GCE and 0.65 μM for Hemin-G4/Au/ITO), rapid response (<4 s), and high selectivity and sensitivity (314.33 μA mM−1 cm−2 for Hemin-G4/Au/GCE and 322.22 μA mM−1 cm−2 for Hemin-G4/Au/ITO). The two electrodes allow sensitive capture of H2O2 produced by A549 cells. Compared with the conventional method of detection in cell suspensions, an ITO electrode with a large specific surface area and good biocompatibility can provide a promising platform for cell adhesion, so as to realize real-time and in situ detection of extracellular H2O2. The experimental results show that A549 cells can adhere to the surface of the Hemin-G4/Au/ITO electrode and grow well. This is benefitted from the three-dimensional structure of the Hemin-G4/Au hydrogel, which provides a suitable microenvironment for cell adhesion and growth. Furthermore, the in situ detection shows a faster response time than that of in-solution detection. This is because the H2O2 generated by the cells can be directly captured by the ITO electrode, which avoids diffusion from the solution to the electrode. These results indicate that the self-supporting hydrogel modified ITO electrode has great application prospects in basic biomedical research and continuous dynamic surveillance of diseases.
研究领域:
电化学
·
生物传感器
·
生物医学工程
·
细胞生物学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Qiang Zhou,Xinyu Wang,Tao Xing,Mingqing Wang,Mingbo Wu,Wenting Wu
Hydrogen peroxide (H 2 O 2 ) is widely used as an oxidant for photocatalytic oxidation of methane to value-added chemicals under mild conditions, but suffers from low utilization efficiency. Herein, we propose a comprehensive strategy for the proper amount of hydroxyl radicals (•OH) generation from H 2 O 2 by regulating the Pd/Au molar ratios and the total Au-Pd contents loaded on In 2 O 3 . For the photocatalytic oxidation of methane at ambient temperature, the yield and selectivity of CH 3 OH over the optimized 1.0% AuPd 0.5 /In 2 O 3 catalyst were as high as 2187.0 μmol g −1 h −1 and 94.0% respectively, exceeding most reported literatures. Mechanism investigations revealed that the formation of Au-Pd alloys may contribute to the homolytic cleavage of H 2 O 2 into •OH radicals and improve the selectivity of •OH generation. This work provides some guidance for the delicate design of photocatalysts to manipulate selective H 2 O 2 activation and efficient photocatalytic methane oxidation.
研究领域:
化学
·
催化
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Wenxin Sun,Yanan Zhou,Ming Liu,Yina Tian,Hua Zou,Xiaoguang Duan,Hao Jia,Guoshuai Liu
Dual-atomic catalysts (DACs) demonstrated remarkable potential in addressing key challenges in electro-Fenton (EF) processes. In this study, we synthesized an EF DACs comprising both CoN 4 and FeN 4 sites, which was achieved a high H 2 O 2 generation rate (1.68 mM −1 h −1 ) and 100 % bisphenol A degradation efficiency via successive two-electron oxygen reduction and one-electron Fenton reactions (2e − ORR + 1e − Fenton). Our findings indicated that the single-atom nitrogen coordination of CoN 4 and FeN 4 sites plays crucial roles in regulating the adsorption of key intermediates of *OOH and *H 2 O 2 . The bimetallic sites independently regulated the binding energies of *OOH on CoN 4 (pyrrole-type) for favorable H 2 O 2 generation and its subsequent activation on adjacent FeN 4 (pyridine-type). Thus, the dual-site engineering addresses the trade-off of in situ H 2 O 2 generation-activation in EF chemistry, realizing high electron utilization efficiency and fast pollutant degradation toward efficient and sustainable water treatment.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Hong-Mei Chai,Jia-Ling Yan,Gang-Qiang Zhang,Jia-Xing Wang,Yi-Xia Ren,Lou-Jun Gao
When a multicarboxylate aromatic ligand, 3,5-di(2′,4′-dicarboxylphenyl)benzoic acid (H5L), was employed, five structurally similar lanthanide metal–organic frameworks (Ln-MOFs), {[Pr10L6(OH)3Cl(H2O)6]·4C2H8N}n (1), {[Nd10L6(OH)4 (H2O)9]·4C2H8N}n (2), {[Gd10L6(OH)4(H2O)3]·4C2H8N}n (3), {[Ho10L6(OH)4 (H2O)3]·4C2H8N}n (4) and {[Er10L6(OH)4(H2O)6]·4C2H8N}n (5), were synthesized and characterized. Single-crystal X-ray structural analyses disclosed that all five Ln-MOFs crystallize in the trigonal R3 space group. They have three-dimensional mesoporous structure featuring the coexistence of binuclear and tetranuclear species as inorganic building units. The mesoporous structure of 3 was verified by the gas adsorption experiment of N2. Fluorescence analysis showed that 3 can selectively detect Fe3+, Cr2O72–, and H2O2; furthermore, it can be used for the electrochemical detection of trinitrophenol. With the merit of an excellent highly sensitive detection performance, 3 has unpredictable application prospects in future research fields.
研究领域:
材料科学
·
分析化学
✓ 已验证
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 33
·15721-15730
·
IF 3.3
Wanyu Song,Peng Sun,Jihong Zhou,Xu Han,Qijun Dai,Fang Chai
The Keggin phosphotungstic acid (PW12) embedded metal–organic framework copper benzene-1,3,5-tricarboxylate (CuBTC), CuBTC@PW12, was fabricated by a facile hydrothermal synthesis technique. With a unique tetrakaidecahedron structure and multiple active sites, the obtained CuBTC@PW12 exhibited peroxidase-mimicking activity, which promoted a novel strategy for qualitative and quantitative detection of hydrogen peroxide (H2O2) and sequential sensing of ascorbic acid (AA) via colorimetric evolution. Notably, with the advantages of strong redox performance of POMs and the unique porous structure of metal organic frameworks (MOFs), as peroxidase mimics, CuBTC@PW12 achieved highly selective and sensitive detection of H2O2via oxidizing TMB to a blue oxidation product (ox-TMB), with a limit of detection of 2.67 μM within the 0.01 to 1.0 mM scale. Concomitantly, the AA can be monitored consecutively by reducing the ox-TMB with fading blue color quantitatively with a limit of detection at 0.15 μM in the range of 0.01–0.10 μM. The recoveries for the determination of AA in human serum were obtained at 94.63–105%. These results manifested that CuBTC@PW12 could be used as a peroxide-mimetic enzyme for the continuous detection of H2O2 and AA with the advantages of simplicity, efficiency, sensitivity and accuracy.
研究领域:
材料科学
·
分析化学
·
生物医学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Cui Wang,Mengli Zhang,Lipeng Bai,Panpan Gai,Feng Li
The peroxidase (POD)-like nanozyme typically requires the addition of exogenous H2O2. To address the limitation, previous work mainly adopted a cascade strategy for H2O2 production. Herein, we propose a new light-driven self-cascade strategy to construct POD-like nanozymes without exogenous H2O2. The model nanozyme resorcinol–formaldehyde resin-Fe3+ (RF-Fe3+) is synthesized with the hydroxyl-rich photocatalytic material RF as the carrier to in situ chelate metal oxides, which can simultaneously achieve the functions of in situ H2O2 generation under irradiation and substrate oxidation via POD-like behavior. Notably, RF-Fe3+ exhibits high affinity to H2O2, attributed to the excellent adsorption ability and hydroxyl-rich feature of RF. Furthermore, the dual photoelectrode-assisted photofuel cell was further constructed with a high-power density of 120 ± 5 μW cm–2 based on the RF-Fe3+ photocathode. This work not only demonstrates the new self-cascade strategy of in situ generation of catalysis substrates but also provides an opportunity to extend the catalytical field.
研究领域:
纳米技术
·
催化
·
光化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Ke Han,Hongming Su,Liang Zhang,Chaofeng Huang,Jie Cui,Fengxiang Chen,Ye Tian,Li Mi
Peroxygenase-catalyzed oxidation reactions rely on H2O2 as co-substrate. However, due to the poor robustness of peroxygenases toward H2O2, it is necessary to fabricate more efficient systems for stoichiometric in situ H2O2 production. Herein, a MoS2 nanosheet supported on the hydrophobic titanium dioxide (TiO2) film of a carbon paper (CP) (MoS2/TiO2/CP) surface was utilized to fix peroxygenase and construct a photocatalysis triphasic nanobioreactor. One side of the reactor was in contact with the analytical solution, while the opposing side was directly exposed to the gas phase. In particular, the generated electrons by photoinduction can reduce atmospheric O2 at the interface for H2O2 self-supply, and the levels of generated H2O2 could be regulated by the O2 concentration from the gas phase at the interface to further regulate peroxygenase catalytic activity. Compared with the conventional diphase interface, the catalytic efficiency of peroxygenase in the as-prepared reactor increased up to 35-fold. The product of benzene-containing substances catalyzed by triphasic nanobioreactors can be further proven by liquid chromatography/mass spectra (HPLC/MS). The above results indicated that the developed system has a potential application in biocatalysis and biosynthesis.
研究领域:
生物催化
·
纳米技术
·
酶促反应
·
光催化系统
·
生物化学工程
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2024
·Vol. 14
·期 12
·895
·
IF 3.8
Kuangjun Li,Yuting Li,Rong Feng,Jing Wu
Chemiluminescence (CL) is regarded as a better method for the detection of reactive oxygen species (ROS). However, the weak CL intensity prevents its further application. Many nanomaterials have been developed to enhance CL intensity, and mixed-ligand MOFs incorporating additional metals or organic ligands exhibit high efficiency in catalyzing. In this work, one kind of bimetallic mixed-ligand metal–organic framework (Ni-Co m-MOF) was synthesized using solvothermal methods. The material was morphologically characterized and demonstrated to be a dense and spherical flower-like structure. The addition of Ni-Co m-MOFs significantly enhanced the CL intensity of the luminol-H2O2system by nearly 2,000-fold. The enhancement was found through further research as hydrogen peroxide was catalyzed to create hydroxyl radicals, etc., which reacted more easily with luminol. Herein, significant enhancement of the CL system by Ni-Co m-MOFs was identified, which provides ideas for improving the sensitivity and signal-to-noise ratio development of CL detectors.
研究领域:
分析化学
·
纳米材料科学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL BIOCHEMISTRY
·
2017
·
IF 2.334
Zhonghua Xue,Xiaofen Wang,Honghong Rao,Xiuhui Liu,Xiaoquan Lu
Many strategies have been explored for selectively and sensitively detecting cysteine in different samples. Here, a novel colorimetric sensor based on self-assembly nanostructures of Fe 3+ -H 2 O 2 /Tetramethylbenzidine system with dual-level logic gate function and colorimetric determination of cysteine were firstly explored. The proposed Fe 3+ -H 2 O 2 -TMB system provides a sensitive optical signal due to the selectively reductive ability of cysteine to the oxidized TMB and thus could be successfully applied to the construction of instant on-site visual detection method with a paper based test strip for cysteine determination in a sample solution as well as for a dual-level logic gate fabrication.
研究领域:
分析化学
·
生物传感
·
医学检测
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2016
·
IF 4.758
Fengmin Qiao,Qingqing Qi,Zhenzhen Wang,Ke Xu,Shiyun Ai
Manganese selenide (MnSe) nanoparticles as nanocatalysts may present enhanced peroxidase-like catalysis if loaded on conductive graphite carbon nitride (g-C 3 N 4 ) supports. In this work, MnSe nanoparticles were successfully loaded on the surface of polymeric g-C 3 N 4 as a cocatalyst through a thermal condensation method by calcinating the mixture of pure MnSe, dicyandiamide and cyanuric acid . The morphology and composition of thus-prepared MnSe loaded doped graphite phase carbon nitride nanosheets (MnSe-g-C 3 N 4 ) were characterized by transmission electron microscopy (TEM), high resolution TEM , X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectra and X-ray photoelectron spectroscopy (XPS). Structural analyses revealed that the MnSe-g-C 3 N 4 nanoparticles are composed of ultrathin nanosheets with 20 nm lateral diameter. Compared with original MnSe and g-C 3 N 4 , the prepared MnSe-g-C 3 N 4 nanosheets could achieve higher aqueous stability and, especially, much stronger peroxidase-like catalysis, presumably resulting from the synergetic effects of conductive carbon nitride and lamellate MnSe nanocatalysts effectively loaded. Significantly, MnSe-g-C 3 N 4 nanosheets were proved to be novel peroxidase mimetics which could quickly catalyze oxidation of the peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H 2 O 2 , producing a blue colored solution. Kinetic analysis indicates that the catalytic behavior satisfy typical Michaelis–Menten kinetics and follows a ping-pong mechanism. Colorimetric detections of H 2 O 2 and glucose using the MnSe-g-C 3 N 4 nanosheets were conducted with high detection sensitivities, demonstrating the feasibility of practical sensing applications. It is therefore believed that our findings in this study could open up the possibility of utilizing MnSe-g-C 3 N 4 nanosheets as enzymatic mimics in diagnostics and biotechnology fields.
研究领域:
材料科学
·
纳米技术
·
分析化学
·
生物传感器
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Mengying Luo,Yinnan Song,Niaz Ali Khan,Wanru Wei,Ying Lu,Qinghua Zhao,Haiqing Jiang,Mufang Li,Dong Wang
H 2 O 2 sensor is widely used in biomedicine, environmental governance and food processing. However, it is limited by the complex preparation processes and high cost of raw materials. In this work, we develop a facile, simple and cost-effective method to fabricate H 2 O 2 sensor based on a screen-printed electrode via in-situ growth method. The copper was first electrodeposited on the working electrode of screen-printed electrode (SPE) as a sacrificial layer, subsequently, the SPE was immersed in horseradish peroxidase (HRP) containing phosphate buffer saline (PBS). The Cu ions formed by oxidation of the copper layer combined with HRP and phosphate ions to construct HRP-Cu 3 (PO 4 ) 2 hybrid nanoflowers on its surface. The fabrication process is straightforward, without complex reaction conditions and dangerous drugs, which is conducive to mass production. This sensor showed a good linear response to H 2 O 2 with a detection limit of 1.8 μM and a sensitivity of 263.3 μA∙mM −1 ∙cm −2 . Additionally, it possessed excellent selectivity and long-time stability. The performance of this sensor was investigated in various beverages such as milk, beer, and juice, showing reliable detection of H 2 O 2 which highlights the potential practical applications of the sensor.
研究领域:
生物医学工程
·
分析化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Zenan Li,Jiacheng Li,Jiaxuan Wang,Luhan Li,Weijie Yuan,Tianyang Zhang,Jian Shen,Yurong Ma,Zhenglong Fan,Fan Liao,Hui Huang,Yang Liu,Zhenhui Kang
Understanding photocatalytic processes of nanoclusters at the nanoscale remains a challenge. Here, we synthesized two kinds of gold nanoclusters stabilized by thiol ligands (AuNCs) and carbon dots (AuCDs) to study their interfacial kinetics in photocatalytic H 2 O 2 production. Three operando testing methods, including transient photovoltage (TPV), transient potential scanning (TPS) and photo-induced current (TPC), are used to investigate the influence of carbon dots (CDs) on catalytic processes. While AuNCs and AuCDs show similar O 2 adsorption abilities, AuCDs exhibit a lower reaction rate due to less surface effective photoelectrons. The AuNCs utilize their own ligands to consume photo-generated holes while the presence of CDs in AuCDs changes this way and providing stable catalytic sites for water oxidation reaction. Additionally, with the addition of CDs, the oxygen reduction reaction pathway changes from a two-step one electron process to a one-step two electron process. This work provides new insights for understanding the photocatalytic processes.
研究领域:
材料科学
·
纳米技术
·
光化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）