ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Juan Li,Jinggao Wu,Chang Ming Li
Dual hetero paired single atomic catalyst (DHAC, CoCu@CN) was one-pot synthesized by a facile green method and applied as a nanozyme for the detection of H 2 O 2 . Both experimental results and theoretical calculations discover that the hetero-paired DAC realizes stronger adsorption energy and a bridge adsorption of H 2 O 2 for simultaneous 2-electron transfer, thereby offering much higher electrocatalytic activity and larger catalytic current than that of single Co atom and single Cu catalyst alone toward H 2 O 2 reduction. The CoCu@CN H 2 O 2 sensor demonstrates a wide linear detection range (0.654–7379.454 μM) and low limit of detection (LOD) of H 2 O 2 (0.047 μM), and is used successfully to in-site detect intracellular H 2 O 2 released from living cells, ensuring its practical applications in life science and medical diagnosis. This work not only discloses a scientific insight for the enhancement mechanism of the dual single heteroatomic catalyst, but also demonstrates an avenue to synthesize more efficient dual single heteroatomic catalyst for potential broad applications in energy conversion and/or sensing applications.
研究领域:
生物化学
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材料科学
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医学诊断
✓ 已验证
产品关联
DOI
高影响因子
Analytical Methods
·
2025
·
IF 2.6
Xiulei Xiong,Haihua Shen,Songnan Liu,Fei Rong,Jian Dong
To detect H2O2 and redox potential of an acute wound simultaneously, a SERS-active microneedle was fabricated by integrating H2O2 and redox potential SERS probes in two grooves of an acupuncture needle, respectively. When the SERS-active microneedle was inserted into tissues, an acute wound formed and the two SERS probes were brought into the wound to sense H2O2 and redox potential of the wound. The feasibility of the SERS-active microneedle was evaluated ex vivo and in vivo. Both sugar deficiency and sugar excess induce the increases of H2O2 and redox potential in most tissues. Short-term physiological disturbances eventually returned to normal levels in healthy organisms, and abnormal sugar intakes disrupt the normal physiological environment and induce stress response in all tissues. The SERS-active microneedle for detection of H2O2 and redox potential would become a powerful tool, used for collecting physiological signals in different tissues to elucidate the mechanisms of wound healing and redox-related diseases.
研究领域:
生物医学工程
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分析化学
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病理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wenxuan Zhou,Xiaoyong Mo,Cham Wah Cheung,Edmund C.M. Tse
At present, over 95 % of H 2 O 2 is produced via the anthraquinone process that requires large infrastructure, generates organic pollution, and poses safety issues. Electrochemical H 2 O 2 generation through oxygen reduction can serve as an alternative, reliable, and decentralized production method if affordable and high-performance electrocatalysts can be developed. Herein, a two-step process is used to prepare an Fe-based complex as a non-precious metal electrocatalyst to facilitate oxygen reduction reaction (ORR) and produce an alkaline H 2 O 2 solution. The Fe complex of benzene-1,3,5-tricarboxylate (FeBTC) is first synthesized using a hydrothermal method and then activated via a pulsed laser treatment process that is optimized via the Taguchi method. The pulse-laser-treated FeBTC (PL-FeBTC) lowers the H 2 O 2 electrosynthesis overpotential by 50 mV at −0.1 mA/cm 2 and exhibits a 25 % increase in H 2 O 2 product selectivity at 0.4 V vs. RHE. The experimental results indicate that the O 2 -to-H 2 O 2 turnover frequency and electrocatalytic yield of the Fe-based metal–organic framework are enhanced simultaneously through solid-to-solid pulsed laser conversion. Through a series of X-ray photoelectron spectroscopy, elemental analysis, Raman spectroscopy, X-ray absorption spectroscopy, and control atmospheric experiments, the origin of the improvement in catalytic performance is rationalized through the formation of an oxo-bridge across the di–Fe active site via an oxygen-doping mechanism, thus providing a systematic laser methodology for precise structure-performance tuning. Beyond H 2 O 2 generation, this study further lays the foundation for the development of cost-effective and scalable electrocatalysts that are central to other commodity manufacturing and sustainable resourcification processes.
研究领域:
材料科学
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电化学
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催化
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可持续化学
✓ 已验证
DOI
高影响因子
APPLIED CLAY SCIENCE
·
2021
·
IF 5.467
Ping Chen,Hui Zhong,Xiao-rong Li,Meisheng Li,Shouyong Zhou
Nanomaterials with intrinsic enzyme-like activities have attracted extensive research interest as promising alternatives to natural biological enzymes due to their advantages of low cost and high stability. Many artificial enzyme mimics have been successfully applied in the fields of sensing, environmental treatment, and oncotherapy. Herein, novel [email protected] 3 O 4 nanocomposites ( [email protected] 3 O 4 NCs) were fabricated by modifying Pal with Co 3 O 4 nanoparticles through a facile hydrothermal method . The obtained [email protected] 3 O 4 nanocomposites as nanozymes displayed enhanced peroxidase-like activity, which can catalyze the oxidation of 3,3,5,5-tetramethylbenzidine (TMB) in the presence of hydrogen peroxide (H 2 O 2 ) to obtain colored products. Kinetic assay indicated that the [email protected] 3 O 4 peroxidase mimics showed a higher affinity towards TMB than that of natural horseradish peroxidase (HRP). Moreover, a sensitive and selective sensor for colorimetric determination of H 2 O 2 and ascorbic acid (AA) was successfully constructed by using [email protected] 3 O 4 nanocomposites as peroxidase mimics. Furthermore, the proposed assay for sensing of AA in model samples was evaluated with satisfactory results, demonstrating the potential applications in complex biological systems.
研究领域:
生物传感
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纳米材料科学
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医学诊断
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2021
·
IF 7.46
Xin Xu,Peng Luo,Huan Yang,Shuang Pan,Hui Liu,Xiaoli Hu
This paper reports a facile approach for fabricating metal–adenosine triphosphate (ATP) nanoparticles (NPs) by the self-assembly of ATP and metal ions under moderate conditions. Here, Cu-ATP NPs only showed laccase-like activity, but the Fe 3+ -doped Cu-ATP NPs could exhibit peroxidase-like activity, resulting in a decrease in laccase-like activity. Mn 2+ ions functioned as a regulator to balance the enzyme-like activities of CuFe-ATP NPs, endowing the CuMnFe-ATP NPs with both strong laccase- and peroxidase-like activities. Surprisingly, the CuMnFe-ATP NPs also exhibited catalase-like activity under neutral conditions, improving the efficiency of phenol oxidation. X-ray photoelectron spectroscopy (XPS) analysis confirmed that the mixed valence states of the metals in the CuMnFe-ATP NPs accounted for the high catalytic efficiency; also, the large surface area and intrinsic porosity of the NPs were of great importance. The kinetic studies results indicated that the CuMnFe-ATP NPs exhibited rather strong affinities to 3,3,5′,5′-tetramethylbenzidine (TMB) and 2, 4-dichlorophenol (2,4-DP). On the basis of peroxidase-mimic activity, the CuMnFe-ATP NP system was employed to establish a facile colorimetric biosensing method for H 2 O 2 determination, and the detection limit of H 2 O 2 was 0.047 μmol⋅L −1 . These results prove that the enzyme-like activities of Cu-ATP NPs can be modulated via simple metal doping, which may extend to other nanozymes.
研究领域:
生物化学
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纳米生物学
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 41
·期 14
·6700-6708
·
IF 3.269
Huimin Zhao,Yaxi Li,Bing Tan,Yaobin Zhang,Xiaochi Chen,Xie Quan
To improve the peroxidase-like activity of molybdenum dichalcogenides (MoS2), surface modification, such as combing with monometallic or bimetallic nanoparticles, is of great and widespread interest. However, only a few studies have been reported on the modification of MoS2 with non-metallic materials. Herein, we report a study on the peroxidase-like activity of novel PEGylated MoS2 (PEG-MoS2) nanosheets prepared using a simple liquid-phase exfoliation and pegylation process. Compared to the undecorated MoS2 nanosheets, PEG-MoS2 nanosheets have improved water dispersiblity and stability, which are beneficial for improving the peroxidase-like activity, as well as the catalysis velocity and affinity for TMB or H2O2. Based on PEGylated MoS2, we successfully established a new platform for the colorimetric detection of H2O2 with a limit of detection (LOD) of 1.18 μM, which is comparable to that of the majority of the reported enzyme mimics of inorganic graphene analogues. More importantly, the as-prepared PEG-MoS2 nanosheets are environmentally friendly, water dispersible, low cytotoxic, and easily prepared, which indicate that PEG-MoS2 is a type of promising enzyme mimics and extremely likely to be applied in cell-based assay systems without any adverse reactions.
研究领域:
生物化学
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纳米医学
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Bolong Zhao,Yulong Ma,Yonggang Sun,Guangsuo Yu,Juan Zhang,Li Zhu,Min Xu,Lei Wang,Duoning Zhao,Wenxin Ji,Yuanyuan Li,Yongsheng Ren
The traditional H 2 O 2 oxidation treating high-salt industrial wastewater is confronted with challenges, because of the inhibition of Cl - on oxidant radical. Thus, a non-radical pathway for H 2 O 2 removal of organic pollutants is optional. Herein, an innovative cobalt nitrogen-doped carbon (Co-N 5 -C) catalyst was constructed with an atomically dispersed asymmetrical high-density of Co-N 5 sites and highly active intermediate Co-OH groups, achieving highly selective converting H 2 O 2 to 1 O 2 through three steps electron transfer pathways. The oxidation of tetracycline by ¹O₂ accounted for 95.6 % of the total removal. H 2 O 2 is initially activated at the Co-N 5 site, which generates the active intermediate Co-OH groups. This Co-OH group then further activates H 2 O 2 , leading to the production of •O 2 - /•OOH. The newly produced •O 2 - /•OOH are instantaneously captured by neighboring Co-OH groups and subsequently converted into 1 O 2 . These adjacent catalytic sites could effectively capture and stabilize the short-lived radicals through the distance effect. and the intermediate Co-OH group in the reaction significantly reduces the energy barrier for H 2 O 2 conversion to •O 2 - /•OOH and 1 O 2 conversion by 0.26 eV and 11.12 eV, respectively. The efficiency of tetracycline degradation at 96 % even with the Cl - concentration as high as 7000 mg/L.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yulun Nie,Xiaofei Sun,Miao Wang,Xike Tian,Chao Yang,Chu Dai
UV-H 2 O 2 is the most widely used oxidizing system with established effectiveness and a high level of technical development for practical application. However, little attention was paid on the effect of suspended particles in natural water on organic contaminants removal via UV-H 2 O 2 technique. In this study, this effect of suspended particles to enhance the contaminant degradation was explored using silica/alumina-based oxides (MCM-41 and Al@MCM-41) as the representative. The results showed that MCM-41 had no effect on OFX degradation compared with UV-H 2 O 2 . While the degradation efficiency and reaction rate were greatly enhanced at a pH range of 3.0–9.0 especially at acidic pH values (3.0–5.0) in the presence of Al@MCM-41. The probe experiments proved that OFX adsorption followed by surface reaction process played an important role to enhance the performance of UV-H 2 O 2 . Based on the characterization results, the positive effect of suspended particles was not related to their surface area and pore size distribution, but dependent on the chemical composition and surface acid-base property. The suspended particles can provide an active surface composed of acid and base sites. The base site can create a local basic micro-environment by producing more • OH et al. While the dissociated acid sites in Al@MCM-41 with a negative charged surface favor OFX adsorption and then reaction with produced ROS . Our findings suggest that the enhanced performance of UVA-H 2 O 2 induced by suspended particles should be concerned.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Pin Wang,Lingjun Bu,Yangtao Wu,Wangchi Ma,Shumin Zhu,Shiqing Zhou
The study investigated the degradation kinetic and transformation mechanism of ibuprofen (IBP) in UV/H 2 O 2 process from both experimental and theoretical aspects. Impacts of H 2 O 2 dosage, solution pH, quenching agent, and concentration of nitrite (NO 2 − ) on IBP degradation in UV/H 2 O 2 process were evaluated. Both experimental results and theoretical calculations indicated that • OH played an important role in the degradation of IBP and its transformation products . The second-order rate constants of • OH and • NO 2 with IBP were calculated as 3.93 × 10 9 M −1 s −1 and 5.59 × 10 −3 M −1 s −1 , based on the transition state theory, which explained the phenomenon that addition of NO 2 − inhibited IBP degradation. Further, according to the results of ultra-high-resolution mass and density functional theory calculations, mechanisms of a detailed degradation pathway for IBP were clarified. Namely, the detailed mechanistic formation pathways for hydroxylated and keto-based products were proposed. Then, possible active sites of the keto-based products, as well as the corresponding subsequent products were predicted by Condensed Fukui Function. Our study can broaden the knowledge of the reactions of emerging contaminants with • OH, and provide theoretical foundation for the optimization of UV/H 2 O 2 process.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 1
·450-459
·
IF 3.049
Zhikai Wei,Peng Li,Muhammad Hassan,Pu Wang,Cong Xu,Long-Fei Ren,Yiliang He
Photovoltaic wastewater contains a large amount of thiourea that cannot be directly treated by biological methods because of its biotoxicity. In this study, a novel O3/H2O2 + BiPO4/UV synergy technique was used as a pre-treatment process to degrade thiourea. The effects of H2O2 and catalyst loading were investigated, and the transformation pathway of thiourea was predicted based on the intermediates detected by UPLC-Vion-IMS-QToF. The synergy technique degraded 89.14% thiourea within only 30 min, and complete degradation occurred after 150 min. The TOC removal of O3/H2O2 + BiPO4/UV was 1.8, 1.5, and 1.9 times that of O3/H2O2 and BiPO4/UV/H2O2 single processes and O3/H2O2 + UV process, respectively, which was due to the synergy between H2O2 residues and BiPO4. In addition, thiourea was mainly degraded by ·OH into thiourea dioxide and melamine (polymerized by other intermediates) and then further degraded into biuret and methyl carbamate by the holes of BiPO4, followed by complete mineralization into H2O and CO2. These results confirm that the O3/H2O2 + BiPO4/UV synergy technique is a promising option for the degradation of thiourea.
研究领域:
环境工程
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水处理
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Haopeng Jiang,Xiaohui Yu,Jinhe Li,Lele Wang,Weikang Wang,Chunxia Wu,Liyong Tang,Qinqin Liu
Herein, a NH 2 -MIL-125(Ti)@Ag@AgCl (NM@Ag@AgCl) stacked core–shell heterojunction with Z-scheme carrier transfer mechanism was developed to fulfil the goal of synchronous reactions of CO 2 reduction and H 2 O oxidation. In detail, the NM@Ag@AgCl was obtained by in-situ loading the AgCl as the shell-inorganic semiconductor on the octahedral NM as the core-organic semiconductor, followed by in-situ transforming part of the AgCl shell into the plasmonic Ag nanoparticles using a photo-reduction method. As a result, the interface effects of core–shell architecture majorized by the Ag electronic mediator can favor the transmission of photogenerated carriers and reduce electron transport resistance; while the plasmonic Ag mediated Z-scheme mode with a giant internal electronic field provided a strong driving force to recombine the carriers with weak redox ability, reserving the carrier with strong redox ability on the NH 2 -MIL-125-core and AgCl-shell for the simultaneous reactions. The CO and H 2 O 2 yields of the optimal NM@Ag@AgCl were 6.02 and 5.43 μmol⋅g −1 ⋅h −1 , which were 3.31 and 4.02 times that of the NM, respectively. This study furnishes a novel thread for the design of core–shell organic–inorganic heterojunction with high interfacial charge transfer for realizing the simultaneous reactions.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2025
·
IF 4.6
Ting Zhang,Ruipeng Hou,Rong Wu,Chen Zhang,Yindi Yu,Wenlong Yang,Shunhang Wei
Limited by rapid carrier recombination, the photocatalytic hydrogen peroxide (H 2 O 2 ) generation performance of Zn 2 In 2 S 5 is far from practical application. Herein, Zn 2 In 2 S 5 /In 2 S 3 S-scheme heterostructures were constructed by employing a one-step hydrothermal strategy that precisely adjusted the Zn:In precursor ratio. Thanks to the band structures with sufficiently redox ability of In 2 S 3 and Zn 2 In 2 S 5 , as well as enhanced carrier separation and transfer efficiency, the optimal Zn 2 In 2 S 5 /In 2 S 3 heterostructures (ZIS/In 2 S 3 -1:4) achieved a sacrificial-agent-free H 2 O 2 production rate of 339.5 μM h −1 under AM 1.5 irradiation, which approximately 1.7 times higher than that of pristine Zn 2 In 2 S 5 . Meanwhile, it also exhibited good H 2 O 2 evolution rate under visible-light irradiation and reusability. Its apparent quantum yield (AQY) at 380 nm, 420 nm, and 450 nm reached to 1.32 %, 1.11 %, and 0.63 %, respectively. In addition, the introduction of In 2 S 3 inhibited H 2 O 2 decomposition and enhanced the selectivity of H 2 O 2 production. In the photocatalytic process, superoxide radicals and holes were the key reactive substances, thereby H 2 O 2 was generated via a two-step single-electron O 2 reduction reaction process and one-step two-electron water oxidation reaction process. The construction strategy of the Zn 2 In 2 S 5 /In 2 S 3 S-scheme heterostructures is expected to provide a new perspective for the design of photocatalysts for efficient H 2 O 2 synthesis.
研究领域:
材料科学
·
光催化
·
能源化学
·
纳米材料
·
环境功能材料
✓ 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）