CHEMOSPHERE
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2020
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IF 5.778
Jiafeng Ding,Lilai Shen,Ruopeng Yan,Shihuan Lu,Yinan Zhang,Xiaofang Zhang,Hangjun Zhang
Advanced oxidation processes (AOPs) based on the activation of hydrogen peroxide (H 2 O 2 ) and persulfate (PS) by minerals have received increasing interest for environmental remediation. Herein, H 2 O 2 and PS activation systems employing goethite as a catalyst were discovered for the rapid degradation of BPA with the generation of reactive oxidation species (ROS) and for the reduction of total organic carbon (TOC) in aqueous solutions. The morphology of goethite were characterized by XRD, SEM, BET, TEM, etc. As a result, the oxidant efficiency of the goethite/H 2 O 2 system (75.9%) was higher than that of the goethite/PS system (61.4%) after 240 min due to the restricted radical scavenging. According to the results of electron paramagnetic resonance (EPR) and radical quenching experiments, the main active ROS during the BPA degradation process were OH and SO 4 − . The two reaction systems were all pH-dependent that BPA can be effectively degraded in the goethite/PS system under acidic, neutral and weakly alkaline conditions, while the most inefficient degradation under alkaline conditions in the goethite/H 2 O 2 system. Moreover, goethite showed good structural stability in the two systems. Several reaction products were detected using LC-MS, and the mechanisms for three systems were proposed. Density functional theory (DFT) was employed to study the conceivable degradation pathways of BPA in the two processes. This work reveals novel mechanistic insights regarding H 2 O 2 and PS activation over goethite and implies the great potential application of the PS/mineral process in water and wastewater treatment .
研究领域:
环境科学
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化学工程
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水处理
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高级氧化过程
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Jiahang Liu,Yingying Chu,Xiaoyang Li,Mengying Qian,Weiming Zhang
The co-catalytic effect of hydroquinone/quinone electron shuttle has received great attention in the area of Fenton-like reaction. However, the crucial roles of phenolic or hydroquinone moieties in the chemical structures of organic pollutants have always been overlooked. In this study, we discovered that the introduction of rifampicin (RIF), a representative of rifamycin antibiotics, could trigger complete degradation of atrazine (ATZ) in the Fe(III)/H 2 O 2 system. By exploring the influences of initial Fe(III), H 2 O 2 , RIF concentrations and pH values on ATZ degradation efficiency, key components affecting metal ion valence transitions in the system were identified. Quenching experiments, probe tests and EPR analysis verified that •OH served as the primary active species, while HO 2 •/O 2 •− was also generated. Through monitoring Fe(II) concentration variations and employing mass spectrometric analyses, the oxidation pathway of RIF was elucidated: When mixed with Fe(III), the naphthohydroquinone moiety of RIF immediately acted as a direct electron donor to reduce Fe(III) to Fe(II), while itself being oxidized to RIF-Q. Upon H 2 O 2 addition, it rapidly triggered the classical Fenton reaction with Fe(II) to generate •OH, enabling ATZ degradation. Simultaneously, RIF-Q underwent further oxidative breakdown, with some degradation products retaining the capacity to continuously donate electrons to Fe(III), thereby promoting its reduction. This study provides new insights for the co-catalytic effect of pollutant-derived electron shuttles on the transition of metal ion valences.
研究领域:
环境化学
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污染物降解
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高级氧化过程
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金属离子价态转化
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有机污染物转化
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产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2025
·
IF 5.3
Yacong Yang,Ya Zhao,Fengyan Shi,Zitao Chen,Weiguang Zhao,Yue Gao,Yingchun Miao,Yuning Huo
Micromotors with autonomous motion by multiple driving forces have attracted wide attentions. In this work, we successfully constructed MnO 2 -carbon microspheres (Mn-Cs) composite micromotors with synergistic photothermal-bubbly driving effect. The uniform MnO 2 loading and the stable combination of MnO 2 with Cs in Mn-Cs composite facilitated to improve the photothermal conversion performance. The regular morphology and large specific surface area of Mn-Cs were beneficial for the in-situ photocatalytic decomposition of H 2 O 2 under light irradiation. Notably, the photothermal conversion effect of Mn-Cs could further promote the decomposition of H 2 O 2 . The low thermal conductivity of air was beneficial for expanding the temperature gradient between the micromotor surface and the environment. As a result, the speed of optimal 1.0-Mn-Cs sample under the light irradiation and addition of H 2 O 2 (75.2 μm/s) was 14.3 and 5.88 times higher than that individual light irradiation (5.27 μm/s) and addition of H 2 O 2 (12.8 μm/s), respectively. It was indicative of the great significance of synergistic photothermal-bubbly driving effect. This study provided a new strategy for developing synergistically driven micromotors to reduce chemical fuel dependence, and showed a significant prospect in green, economic and sustainable applications.
研究领域:
材料科学
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纳米技术
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化学工程
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物理化学
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产品关联
DOI
高影响因子
Energy Advances
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2024
·
IF 3.2
Kunpeng Liu,Xu Wang,Nan Wang,Ruiyong Zhang,Meinan Yang,Baorong Hou,Wolfgang Sand
Rationally designing high-efficiency catalysts for electrochemical two-electron water oxidation reaction (2e− WOR) to produce hydrogen peroxide (H2O2) is extremely important, while designing bimetallic metal–organic frameworks (MOFs) is of great significance for effective 2e− WOR. Herein, MIL-53(Fe) and different proportions of Co-doped MIL-53(Fe) were prepared by a hydrothermal method. The structural characterization and elemental analysis showed that the Co ions were successfully doped into MIL-53(Fe) to form a MIL-53(Fe/Co) bimetallic MOF, and the morphology of MIL-53(Fe/Co) became more regular after Co doping. We found that the optimized MIL-53(Fe/Co) exhibits remarkable 2e− WOR performance, which gave an overpotential of 150 mV at 1 mA cm−2. The overpotential of MIL-53(Fe/Co) was approximately 220 mV (at 1 mA cm−2) lower than that of MIL-53(Fe), which may be attributed to the change of microstructure of MIL-53(Fe) after Co doping and the synergistic effect between Fe/Co. Our work introduces a strategy for designing bimetallic MOF-based electrocatalysts, opening up new possibilities for efficient 2e− WOR systems.
研究领域:
材料科学
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电催化
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能源化学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Zhihan Yu,Dainan Zhang,Chenbing Ai,Jianjun Zhang,Quanjun Xiang
Accelerated charge migration and proton transfer to the reaction site are critical factors for improving photocatalytic efficiency. However, realizing both simultaneously is challenging because of the sluggish water (proton source) oxidation kinetics and interdependent redox reactions. Herein, we design an imide and hydrogen bond to connect carbon nitride ports of the D-π-A system with the dual-engineered linkages. The system uses an acetylene functional group and an imidazole ring as spatially separated water oxidation and oxygen reduction reaction (ORR) catalytic centers for photogenerated charge separation, respectively. The imine bond is a bridge grafted to the oxidation site to act as a hydrogen proton trap, and the hydrogen bond formed between reduction site and carbon nitride is used as the channel for instantaneous proton delivery to the reduction center. In situ characterization confirms that the linking sites protonation optimizes the pathway of ORR to H 2 O 2 and facilitates the *OOH intermediates generated. It is concluded that proton transport plays a critical role in optimizing photocatalytic H 2 O 2 production. Our work provides a strategy to improve dynamic proton transfer mechanisms.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Zhaohui Wang,Kun Li,Junling Hu,Ang Li,Yang Tang,Yanzhi Sun,Pingyu Wan,Haomin Jiang,Yongmei Chen
H 2 O 2 production in coupled electrochemical systems, where H 2 O 2 is generated through 2e-pathway of water oxidation (2e-WOR) at anode and 2e-pathway of oxygen reduction (2e-ORR) at cathode, offers an advanced alternative to the anthraquinone process. However, the efficiency of such coupled system is often hindered by the limited activity and selectivity of electrocatalysts. Herein, a dual-functional catalyst composed of amorphous TiO 2 embedded in mesoporous carbon hollow spheres (TiO x @MCHS) is reported, which exhibits exceptional electrocatalytic performance for both 2e-WOR and 2e-ORR. By employing TiO x @MCHS-loaded electrodes as both anode and cathode in a membrane-free flow cell with 4 м K 2 CO 3 /KHCO 3 as electrolyte, a rate of 108.3 µmol min −1 cm −2 and a Faradaic efficiency (FE) of ≈145% for H 2 O 2 production are achieved at a voltage of ≈2.5 V under a constant current of 240 mA (anode: 1 cm 2 , cathode: 4 cm 2 ). Experimental and computational results reveal the crucial role of low-coordinated Ti in optimizing the adsorption of intermediates involved in the two electrode reaction pathways, thereby enhancing both activity and selectivity of these processes. This work establishes a new paradigm for the development of advanced electrocatalysts and the design of novel coupled-electrolysis systems, enabling scalable and sustainable H 2 O 2 electrosynthesis.
研究领域:
材料科学
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电化学
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催化化学
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产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2024
·Vol. 171
·期 10
·107506
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IF 3.1
Chen-Yang Han,Kun-Zhi Wang,Xin Chen,Zhencheng Chen,Guo-Cheng Han,Xiao-Zhen Feng,Heinz-Bernhard Kraatz
Hydrogen peroxide (H2O2) possesses disinfectant, antiseptic, deodorizing, and cleansing properties. It is commonly used to clean wounds, ulcers, abscessed sinuses, and pus in the ear. Herein, a colorimetric-electrochemical bimodal method for the detection of hydrogen peroxide in serum was constructed, when using a platinum sheet electrode electrocatalyzes H2O2 producing hydroxyl radical, resulting in oxidising TMB and giving a color and current change. After optimaztion, cyclic voltammetry, differential pulse voltammetry and ultraviolet spectrophotometry constituting a colorimetric-electrochemical bimodal method were used to establish four linear relationships within the concentration range of 10.00–1000.00 μM. The limit of detection was found to be 3.33 μM. Additionally, the method's recoveries ranged from 98.88% to 101.10% with a relative standard deviation of no more than 3.70% when using the standard addition method in serum, which indicates its potential for practical medical testing.
研究领域:
分析化学
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医学检测
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生物化学
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产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
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2025
·
IF 2
Yali Zhao,Ziru Wang,Jinxiu Zhai,Xingjian Cao,Peilei He
Graphical The lacunary polyoxometalate ([PW 11 O 39 ] 7− , PW 11 ) can self-assemble with TBAB to form tetrakaidecahedron-like nanodices (NDs). These NDs exhibit significantly higher catalytic activity for the epoxidation of cyclooctene compared to PW 11 alone and nanospheres (NSs) formed from the non-lacunary polyoxometalate ([PW 12 O 40 ] 3− , PW 12 ). DFT studies confirm the critical role of hydroperoxo species generated at the lacunary site in facilitating oxygen transfer to cycloalkenes over PW 11 . The activation of hydrogen peroxide (H 2 O 2 ) as a terminal oxidant holds great promise for catalytic oxidation processes. However, developing an efficient catalyst for the epoxidation of bulky organic molecules with H 2 O 2 , including cyclic alkenes, remains challenging. In this research, a lacunary polyoxometalate (POM)-based tetrakaidecahedron nanodices (NDs) are synthesized by [PW 11 O 39 ] 7− (PW 11 ) clusters with tetrabutylammonium bromide (TBAB). The NDs exhibit significantly enhanced catalytic activity in the epoxidation of cyclooctene, with a yield 55.4 times greater than that of the raw PW 11 . Conversely, nanospheres (NSs) assembled from non-lacunary POM clusters of [PW 12 O 40 ] 3− (PW 12 ) under the same conditions achieve only a 2.9 % yield, highlighting the essential role of the lacunary PW 11 structure in NDs. Raman spectroscopy and density functional theory (DFT) calculations confirm that the active hydroperoxo species from H 2 O 2 activation serves as the effective epoxidizing agent. The reduced energy barrier for H 2 O 2 activation on PW 11 , relative to PW 12 , corroborates the superior activity of the NDs. Furthermore, the intermediate generated post-H 2 O 2 activation shows stronger adsorption of cyclooctene, increasing oxygen transfer to cyclooctene during the epoxidation process. This study demonstrates the exceptional performance of an assembly structure utilizing lacunary POMs for the activation of H 2 O 2 and subsequent oxidation reactions.
研究领域:
催化化学
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材料科学
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理论计算化学
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产品关联
DOI
高影响因子
Nanoscale
·
2024
·
IF 5.8
Ziyin Yang,Yaqi Kong,Chengcheng Qi
Compared with transition metals with partially occupied 3d orbitals, Zn has a filled 3d10 configuration, which severely restricts electron mobility and hence usually renders Zn2+ intrinsically inactive for electrochemical sensing. Metal single-atom catalysts are a new kind of sensing material. Owing to their unique coordination structure and high atomic utilization rate, metal single-atom catalysts show unique properties, which makes them promising for use in the field of electrochemical sensing. However, whether Zn single atoms are active sites remains to be elucidated. In this study, we prepared nitrogen-doped carbon (NC) materials by pyrolyzing ZIF-8 at high temperatures and reported that when the pyrolysis temperature was 800 °C, many Zn single atoms with Zn-N4 coordination structures remained in the NC material. Even when the pyrolysis temperature is increased to 1000 °C, a small number of Zn single atoms remain, and the coordination structure changes from Zn-N4 to Zn-N3. Furthermore, unexpectedly, both residual Zn single atoms showed electrocatalytic activity for H2O2 reduction. In particular, the electrocatalytic activity was significantly enhanced after the coordination structure was changed from Zn-N4 to Zn-N3. Density functional theory (DFT) calculations indicate that the coordination structure of Zn-N3 optimizes the adsorption and desorption strength of oxygen-containing species in the electrocatalytic reaction process, which lowers the energy barrier of the rate-determining step and increases the detection sensitivity of H2O2 nearly 4.1 times. This study revealed new properties of Zn single atoms for the electrocatalytic reduction of H2O2 and developed a strategy to increase the electrocatalytic activity of metal single-atom catalysts through coordination number regulation, which lays the foundation for the use of Zn single atoms in the field of electrochemical sensing and provides ideas for the design of new highly active sensing materials.
研究领域:
材料科学
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电化学
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催化科学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Yue An,Yiwei He,Mingtao Li,Wenying Yu,Na Tian,Yihe Zhang,Hongwei Huang
Graphitic phase carbon nitride (g-C 3 N 4 ) is considered one of the most promising catalysts for photocatalytic production of hydrogen peroxide (H 2 O 2 ) due to its green and non-polluting nature and stability. However, the conventional g-C 3 N 4 prepared by direct thermal polymerization has insufficient reaction sites due to its excessive bulk defects derived from incomplete polymerization and low specific surface area, leading to rapid carrier recombination and limited photocatalytic activity. In this work, a series of crystalline g-C 3 N 4 (CN-UxM) with large specific surface areas have been prepared by a molten salt post-treatment strategy with regulating the precursor ratio of urea to melamine . In-situ KPFM, photoelectrochemical experiment and DFT calculation results show that the sample with an optimized urea/melamine ratio of 20 (CN-U20M) has the highest charge separation and transfer efficiency derived from the internal electric field. And its H 2 O 2 production rate under simulated visible light reaches as high as 10.94 mmol∙g −1 ∙h −1 , far exceeding that of most g-C 3 N 4 -based photocatalysts in reported literatures. The present work provides an effective strategy to enhance the photocatalytic activity of g-C 3 N 4 , which is expected to be applied to other organic semiconductor catalytic systems.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Yi Kexin,Li Chao,Hu Shaogang,Yuan Xiayu,Logan Bruce E.,Yang Wulin
Hydrogen peroxide (H 2 O 2 ) can be sustainably synthesized through the electrochemical oxygen reduction reaction in a dual-chamber water electrolyzer separated by expensive ion exchange (IX) membranes. The development of an IX membrane-free electrolyzer has been limited by direct anodic degradation of the produced H 2 O 2 . Here, we devise a bubble shielding strategy by using a low-cost polytetrafluoroethylene hydrophobic porous layer (HPL) on the anode that enables numerous sites for anodically generated oxygen bubbles and significantly suppresses H 2 O 2 degradation in the electrolyte. The H 2 O 2 production increases by ~600% compared to that using non-bubble shielded anode. A high H 2 O 2 concentration of 10.05 ± 0.05 g L −1 at 40 mA cm −2 can be obtained with both HPL-coated anode and cathode. A solar-driven disinfection device equipped with HPL-coated electrodes achieves >99.9% E. coli inactivation within 60 min. This innovative approach for achieving high electrochemical H 2 O 2 concentrations in IX membrane-free electrolyzers more generally provides insights for fine tuning three-phase interfaces and could be applicable to other reactions pathways in electrochemical applications.
研究领域:
环境科学
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化学工程
·
生物学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Jianying Xi,Yong Li,Longhao Lv,Zhengshuai Tang,Fangfang Liu,Jinliang Liu
Photodynamic (PDT) and chemodynamic therapies (CDT) relying on reactive oxygen species-mediated treatments mainly face various challenges of hypoxia, endogenous hydrogen peroxide (H 2 O 2 ) deficiency, and glutathione (GSH) overexpression in the tumor microenvironment. Herein, we propose a novel strategy using a core–shell structured nanocomposite, UCNP@mSiO 2 @5-ALA-CaO 2 -Cu(UA@CC). The strategy centers on upconverting NPs and then utilizes mesoporous silica loaded with 5-aminolevulinic acid (5-ALA) to maximize the enrichment of protoporphyrin IX (Pph IX), an intra-tumor photosensitizer. Then in the acidic tumor microenvironment (TME), CaO 2 in the outer layer reacts with H 2 O to form O 2 , H 2 O 2 and Ca 2+ , and the released H 2 O 2 serves as an auxiliary “fuel” to induce acceleration of the Fenton-like (Cu 2+ ) reaction and inactivation of the antioxidant GSH enzyme, thus enhancing the tumor cells’ Catalysis. Furthermore, under the excitation of a 980 nm laser, 5-ALA-mediated PDT and Cu + -based CDT were initiated. Through interconnected processes of Ca 2+ overload, self-supply of H 2 O 2 /O 2 , and enhanced GSH depletion, an accelerated cycling strategy for combined PDT/CDT therapy was established, resulting in amplified oxidative stress and anti-tumor capabilities, which was validated in cancer cells and melanoma mouse models.
研究领域:
肿瘤学
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纳米医学
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生物化学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）