RSC Advances
·
2022
·Vol. 12
·期 32
·20838-20849
·
IF 4.036
Hanzhang Ye,Yongli Ding,Tingting Liu,Jiani Li,Qi Wang,Yuhao Li,Jingjing Gu,Zhanen Zhang,Xuedong Wang
Traditional bimetallic sulfide-based nanomaterials often have a small specific surface area (SSA), low dispersion, and poor conductivity, thereby limiting their wide applications in the nanozyme-catalytic field. To address the above issues, we herein integrated NiCo2S4 with N,S-rGO to fabricate a nanocomposite (NiCo2S4@N,S-rGO), which showed a stronger peroxidase–mimetic activity than its pristine components. The SSA (155.8 m2 g−1) of NiCo2S4@N,S-rGO increased by ∼2-fold compared to NiCo2S4 with a pore size of 7–9 nm, thus providing more active sites and charge transfer channels. Based on the Michaelis–Menten equation, the affinity of this nanocomposite increased 40% and 1.1∼10.6-fold compared with NiCo2S4 with N,S-rGO, respectively, highlighting the significant enhancement of the peroxidase-like activity. The enhanced activity of this nanocomposite is derived from the joint participation of ˙OH, ˙O2−, and photogenerated holes (h+), and was dominated by h+. To sum up, N,S-codoping, rich S-vacancies, and multi-valence states for this nanocomposite facilitate electron transfer and accelerate reaction processes. The nanocomposite-based colorimetric sensor gave low detection limits for H2O2 (12 μM) and glucose (0.3 μM). In comparison with the results detected by a common glucose meter, this sensor provided the relative recoveries across the range of 97.4–101.8%, demonstrating its high accuracy. Moreover, it exhibited excellent selectivity for glucose assay with little interference from common co-existing macromolecules/ions, as well as high reusability (>6 times). Collectively, the newly developed colorimetric sensor yields a promising methodology for practical applications in H2O2 and glucose detection with advantages of highly visual resolution, simple operation, convenient use, and satisfactory sensitivity.
研究领域:
生物化学
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分析化学
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纳米医学
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DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Liru Song,Wenyu Wang,Jun Tang,Xu Guo,Xiantai Zhou,Qingping Ke
Selective aerobic epoxidation of allylic alcohols and olefins presents a promising solution to the modern chemical industry. However, the development of non-noble metal catalysts with superior catalytic performance for this reaction remains a significant challenge. This study introduces a plasmonic photothermal-catalytic system centered around nano LaSrCoNiO 6 (LSCNi-N) catalyst, enabling the epoxidation of cinnamyl alcohol and styrene mediated by LSPR effect under visible light illumination (>420 nm). This catalyst exhibits superior epoxidation catalytic performance, with selectivities of up to 72.3 % in a 93.4 % conversion of cinnamyl alcohol and 91.8 % selectivity of styrene oxide at almost 100 % conversion of styrene. Mechanistic studies reveal that the high selectivity derives from the in-situ photochemical formation of H 2 O 2 mediated by the localized surface plasmon resonance effect of LSCNi-N and hole scavenger effect of cinnamyl alcohol. These findings highlight the potential of designing plasmonic transition-metal oxidic catalysts to overcome challenges in selectively synthesizing fine chemicals through visible light catalysis.
研究领域:
化学工程
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材料科学
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环境化学
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DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Pengfei Gan,Yichun Sun,Yunyi Li,Wen Liu,Jiangyu Ye,Meiping Tong,Jialiang Liang
In this work, the different selectivity of SO 4 •- and • OH towards municipal solid waste incineration leachates (MSWILs) was studied by a comparative study of UV/persulfate (PS) and UV/H 2 O 2 . Results showed SO 4 •- preferentially mineralized carbon atoms of higher average oxidation state, while • OH showed a two-stage mechanism of partial oxidation and mineralization successively. Electron spin resonance (ESR) analysis showed SO 4 •- had superior selectivity towards MSWILs than • OH, and Fe(II) would significantly affect the selectivity via forming Fe-MSWILs complex. As the consequence, Fe(II) showed slightly negative effect on UV/PS, but greatly enhanced the performance of UV/H 2 O 2 /Fe(II). High concentration of Cl - affected the degradation of non-fluorescent substances by UV/PS, while SO 4 2 - and NO 3 - showed no effect. In contrast, anions showed no effect on UV/H 2 O 2 . In addition, • OH preferentially attacked large molecules, but SO 4 •- showed no selectivity. This study further revealed the selectivity of SO 4 •- and • OH in the treatment of hypersaline wastewater, and provided theoretical support for the development of targeted technology .
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Hongru Qu,Yimin Zhang,Hong Liu,Nannan Xue,Yiping Wang
In traditional methods for preparing vanadium electrolytes, challenges include lengthy processes, high costs, and difficulties in deeply separating vanadium and impurities. This study introduces an innovative approach utilizing an H 2 O 2 -NaClO efficient selective oxidative stripping system within the D2EHPA extraction process. This method was optimized at a pH of 12, with a phase ratio (O/A) of 6:1, a reaction temperature of 45 °C, and a reaction time of 8 min. The concentration of H 2 O 2 was set at 1.5 %, with a volume ratio between H 2 O 2 and NaClO of 95 % to 5 %. Under these conditions, the vanadium stripping rate in a single stage reached 95.13 %. The low concentration (1.5 %) of H 2 O 2 increased the single-stage stripping rate of vanadium by nearly 50 %, reducing H 2 O 2 usage by at least 25 %, while NaClO enhanced the stability of H 2 O 2 . The prepared electrolyte contained impurity ion concentrations of less than 10 ppm, meeting Chinese national first-class standard of Electrolyte for vanadium flow battery. The electrolyte demonstrated excellent electrochemical and charge–discharge performance, with Coulombic efficiency, voltage efficiency, and energy efficiency reaching 85.45 %, 89.58 %, and 76.55 %, respectively, achieving 95 % of the standard electrolyte’s performance. This method significantly shortens the process and reduces costs by 25.29 % compared to the traditional V 2 O 5 dissolution method. This study offers a novel approach to producing high-purity electrolytes through a shorter, cost-effective process.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Yang Yang,Wenqing Zhen,Tingting Zhao,Maoquan Wu,Shouchun Ma,Liyan Zhao,Jie Wu,Li Liu,Jiaxu Zhang,Tongjie Yao
Fenton/photo-Fenton reaction was limited by slow Fe 3+ /Fe 2+ cycle, low H 2 O 2 activation efficiency, and narrow applicable pH range. Here, Fe atoms doped MoS 2 (Fe–MoS 2 ) with abundant of low-valence Mo δ+ (0 < δ < 4) was prepared. Benefiting from the powerful reduction capacity of Mo δ+ , the rate-limiting step of Fe 3+ reduction was significantly accelerated. Nearly 100% of H 2 O 2 utilization efficiency was realized. Importantly, 90% of H 2 O 2 was effectively activated to be • OH. As a result, tetracycline degradation rate in photo-Fenton reaction catalyzed by Fe–MoS 2 was 5.8 and 4.2 times higher than those of MoS 2 and Fe–MoS 2 -Hyd (prepared by hydrothermal reaction). In comparison with MoS 2 and Fe–MoS 2 -Hyd whose efficient work range were limited in acidic condition, Fe–MoS 2 was a pH-universal catalyst (pH = 2.6–14.0) by taking advantage of the exposed Mo δ+ and photoinduced electrons, largely improving the environmental tolerance. This work simultaneously addressed three bottlenecks in Fenton/photo-Fenton reaction, and provided a new strategy for the preparation of catalysts with powerful catalytic performance and high environmental adaptability.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry C
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2025
·
IF 5.1
Yonghao Wang,Liting Ling,Zhenghao Lu,Ming Zhou,Xiaomei Zheng,Yongjing Wang
Spinel-structured materials are considered promising electrocatalysts for environmental remediation, yet their mechanisms in the electrocatalytic reduction of O2 to H2O2 and the activation of H2O2 remain poorly understood. Herein, we synthesized a novel MgFe2O4/carbon nanotube (CNT) composite via a hydrothermal method and systemically investigated its electrocatalytic performance in the degradation of phenol through the in situ electrocatalytic-reduction of O2 to H2O2 and activation to ˙OH. The composite exhibited exceptional catalytic activity, achieving 99% phenol degradation within 30 minutes under optimized conditions (MgFe2O4/CNT mass ratio of 10 : 1, applied voltage of −0.9 V, pH 3, and catalyst loading of 0.44 mg cm−2). Moreover, the total organic carbon (TOC) reached 78.6% in 90 minutes, with the catalyst maintaining 91.4% efficiency after four recycling experiments. Mechanistic studies using XPS and control experiments indicate that introducing CNTs considerably improves electron transfer and enriches active oxygen and defect degrees. Importantly, abundant defects and active oxygen species facilitate the generation of H2O2 and dominate the conversion of H2O2 into ˙OH by heterogeneous activation for MgFe2O4/CNT, while MgFe2O4 mainly depends on homogeneous activation. This work offers a significant case for the degradation of organic contaminants utilizing spinel-structured electrocatalysts.
研究领域:
环境催化
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电化学
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材料科学
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环境修复
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纳米技术
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DOI
高影响因子
FOOD AND CHEMICAL TOXICOLOGY
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2018
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IF 3.977
Qiang Chu,Lushuang Yu,Zihuan Zheng,Meng Chen,Zheng Hua,Miaojia Hang,Yonglu Li,Xixi Li,Yangyang Liu,Yunyun Yang,Xiaodong Zheng
Since flavonoids are antioxidant compounds, they could beneficially affect neurodegenerative diseases where reactive oxygen species are involved. In this study, we firstly isolated and identified fourteen compounds from the flowers of Apios americana Medik. Then, we tested whether Apios americana Medik flowers water extract (AFWE) exerts a protective effect on H 2 O 2 induced PC12 cells injure. As expected, pretreatment with AFWE inhibited cytotoxicity and DNA condensation in H 2 O 2 induced PC12 cells. Exposure of PC12 cells to H 2 O 2 resulted in reactive oxygen species accumulation and mitochondrial dysfunction, while AFWE alleviated these damages. AFWE obviously reversed the alternations as H2O2 increased Caspase-3 and decreased the ratio of Bcl-2/Bax expressions. Furthermore, autophagy in PC12 cells was further activated by AFWE, which was beneficial to resisting adversity. These results manifest that AFWE prevents H 2 O 2 induced damage via regulating autophagy.
研究领域:
神经科学
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药理学
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细胞生物学
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生物化学
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DOI
PubMed
高影响因子
Frontiers in Immunology
·
2024
·
IF 5.7
Shen Man,Dai Xianling,Ning Dongni,Xu Hanqing,Zhou Yang,Chen Gangan,Ren Zhangyin,Chen Ming,Gao Mingxuan,Bao Jing
The treatment of wound inflammation is intricately linked to the concentration of reactive oxygen species (ROS) in the wound microenvironment. Among these ROS, H2O2 serves as a critical signaling molecule and second messenger, necessitating the urgent need for its rapid real-time quantitative detection, as well as effective clearance, in the pursuit of effective wound inflammation treatment. Here, we exploited a sophisticated 3D Cu2-xSe/GO nanostructure-based nanonzymatic H2O2 electrochemical sensor, which is further decorated with evenly distributed Pt nanoparticles (Pt NPs) through electrodeposition. The obtained Cu2-xSe/GO@Pt/SPCE sensing electrode possesses a remarkable increase in specific surface derived from the three-dimensional surface constructed by GO nanosheets. Moreover, the localized surface plasma effect of the Cu2-xSe nanospheres enhances the separation of photogenerated electron-hole pairs between the interface of the Cu2-xSe NPs and the Pt NPs. This innovation enables near-infrared light-enhanced catalysis, significantly reducing the detection limit of the Cu2-xSe/GO@Pt/SPCE sensing electrode for H2O2 (from 1.45 μM to 0.53μM) under NIR light. Furthermore, this biosensor electrode enables in-situ real-time monitoring of H2O2 released by cells. The NIR-enhanced Cu2-xSe/GO@Pt/SPCE sensing electrode provide a simple-yet-effective method to achieve a detection of ROS (H2O2、-OH) with high sensitivity and efficiency. This innovation promises to revolutionize the field of wound inflammation treatment by providing clinicians with a powerful tool for accurate and rapid assessment of ROS levels, ultimately leading to improved patient outcomes.
研究领域:
生物医学工程
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分析化学
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纳米医学
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2024
·Vol. 25
·期 23
·12518
·
IF 4.9
Mingyu Jia,Jueyu Wang,Yuxuan Liu,Daizong Cui,Min Zhao
In this study, Fe3(PO4)2·8H2O magnetic nanoparticles (MNPs) were successfully extracted from the strainBurkholderia cepaciaCG-1. We subsequently characterized their composition, structure, and morphology, revealing that these nanoparticles consisted of Fe3(PO4)2·8H2O with an average diameter of 66.87 ± 0.56 nm. Our measurements indicated magnetic parameters of 151 Oe for coercivity, 2 emu/g for saturation remanence, and 16 emu/g for saturation magnetization. Our findings confirmed that these magnetic nanoparticles exhibited intrinsic peroxidase-like activity, catalyzing the oxidation of 3,3,5,5-tetramethylbenzidine (TMB) in the presence of H2O2. Compared to horseradish peroxidase (HRP), the peroxidase mimic demonstrated greater stability under various physicochemical conditions. To investigate the mechanisms underlying the peroxidase-like catalysis of Fe3(PO4)2·8H2O, we employed fluorescence spectroscopy and electron spin resonance (ESR) analysis. The results revealed that the peroxidase-like activity of Fe3(PO4)2·8H2O stemmed from the generation of hydroxyl radicals (·OH). Furthermore, we established a platform for the colorimetric detection of H2O2and glucose. Our method was capable of detecting H2O2concentrations as low as 1.0 × 10−3mmol/L. Impressively, this sensitive method was successfully applied to determine glucose levels in human serum.
研究领域:
生物化学
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纳米医学
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分析化学
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产品关联
DOI
PubMed
高影响因子
ACS ES&T Engineering
·
2024
·
IF 7.4
Xuechuan Li,Sen Lu,Nan Chen,Siyuan Chen,Hyoung-il Kim,Guan Zhang
Constructing effective cathode materials for simultaneously producing and activating H2O2 to achieve functional reduction of O2 for •OH production is crucial for the development of a heterogeneous electro-Fenton process in wastewater treatment. In this study, the active groups of the carbonaceous catalyst for electrochemical O2 reduction have been tuned and identified from the molecular level. Proton amines and pyrolysis temperature present significant influences on the polymerization process of the phenolic-formaldehyde resin, thereby altering the structure, functional groups, defects, and activity of the carbonized phenolic-formaldehyde catalyst. A graphite felt-based gas-diffusion electrode composed of the active carbonaceous catalyst, organic binder, and transition metal species has been employed in the electron-Fenton-like system to achieve highly selective H2O2 and •OH production for water decontamination. The optimized gas-diffusion electrode exhibits a high H2O2 selectivity of 87.6–92.4% at 0.2–0.4 V vs standard hydrogen electrode (SHE), a higher current efficiency of 99.1%, and a H2O2 production rate of 6.29 mg cm–2 h–1 at 10 mA cm–2, respectively. Furthermore, owing to the efficient decomposition of H2O2 into •OH by Mnn+ species, humic acid can be efficiently degraded in an electron-Fenton-like process. The electrochemical oxidation performance and energy consumption efficiency for the treatment of real landfill leachate have been evaluated. The results demonstrate that the relational design and fabrication of a high-performance gas-diffusion electrode based on regulating the active carbonaceous O2 reduction catalyst and H2O2 activation catalyst have huge potential for electrochemical wastewater treatment.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Na Zhang,Ying Liu,Zhenchen Wan,Yanting Zhang,Wenjing Xie,Peng Zhang,Man Tong,Songhu Yuan
Reactive oxygen species (ROS) production in O2-perturbed subsurface environments has been increasingly documented in recent years. However, the constraining conditions under which abiotic and/or biotic mechanisms predominate for ROS production remain ambiguous. Here, we demonstrate that the ROS production mechanism, biotic and abiotic, is determined by sediment redox properties and sediment compositions. Upon the oxygenation of 10 field sediments, the cumulative H2O2 concentrations reached up to 554 μmol/kg within 2 h. The autoclaving sterilization experiments showed that H2O2 could be produced by both biotic and abiotic processes depending on the redox conditions. However, only the abiotic process could produce significant levels of •OH, and the production yield was closely related to the sediment components, particularly sediment Fe(II) and organic matter. Fe(II) bound with organic matter led to high yields of H2O2 and •OH production. Sediment oxygenation contributed to the appearance of H2O2 in groundwater, with the abiotic mechanism producing higher instantaneous H2O2 concentrations than the biotic mechanism. These findings reveal that the redox conditions, compositions, and texture of sediments collectively control abiotic and biotic mechanisms for ROS production, which assists the identification of ROS production hotspots and the understanding of ROS distribution and utilization in the subsurface.
研究领域:
环境科学
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地球化学
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微生物学
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产品关联
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 12
·1-11
·
IF 6.408
Wang Jing,Xu Wei,Zhou Lin,Zhang Tianqi,Yang Na,Wang Min,Luo Xuemei,Jin Lu,Zhu Huaijun,Ge Weihong
The peroxidase-like activity of MXene@Fe 3 O 4 nanocomposites and the relevant colorimetric application have been investigated for the first time. According to a kinetic study, MXene@Fe 3 O 4 nanocomposites displayed higher peroxidase activity than their individual components, and the catalytic process followed a ping-pong mechanism. The improved peroxidase-like activity of the MXene@Fe 3 O 4 nanocomposites was obtained due to the synergetic impact of the Fe 3 O 4 and MXene phases, the huge ion-accessible interface, and quick electron transfer channels in the nanocomposites. In the presence of hydrogen peroxide (H 2 O 2 ), the MXene@Fe 3 O 4 nanocomposites can catalyze the reaction of the colorless substrate 3, 3, 5, 5-tetramethylbenzidine (TMB) into oxidized TMB which revealed a blue color at 652 nm. After the introduction of glutathione (GSH), the blue color was gradually fading owing to the hydroxyl radical scavenging effect of glutathione. A colorimetric detection platform based on the peroxidase-like activity of the MXene@Fe 3 O 4 nanocomposites was developed for H 2 O 2 and GSH with a detection limit of 0.4 μM and 0.5 μM, respectively. The calibration plot for glutathione detection is calculated by absorbance difference at 652 nm, which ranged from 0.5 to 10 μM with a detection limit of 0.2 μM. The recoveries of GSH with different concentrations ranged from 93.76 to 108.50% and the relative standard deviation from 0.30 to 5.96%. This work significantly extends the application of MXene@Fe 3 O 4 nanocomposites in the construction of colorimetric sensors and reveals a satisfactory result in real sample analysis. Graphical Abstract
研究领域:
纳米材料
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分析化学
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生物传感器
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催化
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产品关联
DOI
PubMed
高影响因子