CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Haiqian Zhao,Shuaishuai Han,Jiuyang Jia,Mingqi He,Kaibo An,Ziyu Tang,Shiwei Lai,Xue Yang,Zhonghua Wang
The adsorption of carbon materials and 2e-ORR performance can be promoted by N-doping. However, the effect of different N-doping types on adsorption and 2e-ORR and their synergy is not clear, which limits the development of an electro-Fenton system. To enhance the degradation efficiency of the electro-Fenton system, it is essential to understand the mechanisms involved in regulating cathode performance. To achieve this goal, a multi-scale simulation approach was employed that integrates molecular dynamics and quantum chemical simulations. This method was utilized to fabricate carbon planes with various N-doping types. The simulation results showed pyridinic-N and pyrrolic-N showed a cooperative effect and promoted the capacity of activated carbon to adsorb tetracycline. Graphitic-N and pyridinic-N greatly improved the selectivity of 2e-ORR, which is conducive to the formation of H 2 O 2 . Experimental investigations have revealed a synergistic association between adsorption and 2e-ORR, and suboptimal performance of either process can hinder the degradation efficacy of electro-Fenton. The reason for this is that an exceptional selectivity of 2e-ORR enhances the production of ·OH, and good adsorption capability facilitates the utilization of ·OH. The MAC cathode exhibits a greater synergistic effect between adsorption and 2e-ORR owing to the suitable proportion of pyridinic-N, pyrrolic-N, and graphitic-N. Under the action of high-efficiency synergy, the degradation effect of tetracycline by the electro-Fenton cathode was 8.72%-11.64% higher than that of other modified cathodes. The outcomes of our investigation provided insights into the approach for targeted control of the performance of N-doped modified cathodes in the electro-Fenton system.
研究领域:
环境科学
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材料科学
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化学工程
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电化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jiahao Liu,Zhaorui Zhang,Zhihang Xu,Ye Zhu,Chenshuai Han,Wei Xiong,J. Paul Attfield,Jianrong Zeng,Siqi Liu,Minghui Yang
Electrocatalytic hydrogen peroxide (H 2 O 2 ) production via the 2e − oxygen reduction reaction (ORR) offers a sustainable alternative to the energy-intensive anthraquinone process. However, achieving cost-effective, long-term stable H 2 O 2 synthesis at industrial-level current densities remains a formidable challenge. Here, we demonstrate that Ni 3 N supported on Ti 3 CN MXene (Ni 3 N/MX) undergoes surface reconstruction during electrocatalysis, forming an active NiOOH layer that optimizes *O 2 and *OOH adsorption, thereby enhancing the 2e − ORR pathway. As a result, Ni 3 N/MX achieves an exceptional H 2 O 2 yield rate of 10.7 mol·h −1 ·g −1 with a Faradaic efficiency of 92.0%. The catalyst maintains continuous operation for over 100 h at 300 mA cm −2 , demonstrating outstanding durability. Furthermore, the estimated production cost of 70 wt% H 2 O 2 is as low as $0.21 kg −1 , underscoring the economic feasibility of this approach. This work highlights metal nitride reconstruction as a powerful strategy for advancing electrosynthesis of H 2 O 2 .
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ELECTROCHIMICA ACTA
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2024
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IF 5.5
Yuhui Wang,Tong Zhang,Yong Huang,Shaonan Gu,Shu Zhang,Zhi Wang,Junhao Liu,Xuzhong Gong
Precise regulation of oxygen reduction reaction (ORR) for 2e-ORR or 4e-ORR is of great importance in designing efficient catalysts for electrochemical reactions. Currently, the exact roles of the functional groups and their possible synergistic functions still remain controversial. In this work, catalysts with different combinations of N and O functional groups were prepared using graphite to regulate ORR selectivity. Meanwhile, the quantum chemical parameters of various functional group combinations in the literature were summarized by using DFT calculation, and a method was provided to explain the relationship between functional group combinations, electronic structure and ORR selectivity by HOMO orbital delocalization index (ODI H ) and Mulliken population (MP). Finally, combining the molecular level calculations, a close correlation between the molecular structures with the tendency of 2e-ORR or 4e-ORR was established. Among them, the combination of C=O, N-Graphitic and Pyridinic-Pyrrolic-Graphitic nitrogen structure promoted 4e-ORR. C-O, O=C-O, N-Pyridinic and N-Pyrrolic promoted 2e-ORR. This study has revealed the essential difference between 2e-ORR and 4e-ORR, and provided a direction for determining the structure of 2e-ORR or 4e-ORR catalysts.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Materials
·
2025
·Vol. 18
·期 8
·1786
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IF 3.2
Xu Wang,Nan Wang,Kunpeng Liu,Meinan Yang,Ruiyong Zhang,Sikandar Khan,Jinhui Pang,Jizhou Duan,Baorong Hou,Wolfgang Sand
Marine biofouling causes significant economic losses, and conventional antifouling methods are often associated with environmental pollution. Hydrogen peroxide (H2O2), as a clean energy source, has gained increasing attention in recent years. Meanwhile, electrocatalytic 2e−oxygen reduction reaction (ORR) for H2O2production has received growing interest. However, the majority of current studies are conducted on acidic or alkaline electrolytes, and research on 2e−ORR in neutral NaCl solutions remains rare. Here, a bimetallic Zn-Cd zeolitic imidazolate framework (ZnCd-ZIF) is rationally designed to achieve chloride-resistant 2e−ORR catalysis under simulated seawater conditions (pH 7.5, 3.5% Cl−). Experimental results demonstrate that the ZnCd-ZIF catalyst exhibits an exceptional H2O2selectivity of 70% at 0.3 VRHE, surpassing monometallic Zn-ZIF (60%) and Cd-ZIF (50%). Notably, H2O2production reaches 120 mmol g−1in a Cl−-containing neutral electrolyte, exhibiting strong resistance to structural corrosion and Cl−poisoning. This work not only pioneers an effective strategy for designing ORR catalysts adapted to marine environments but also advances the practical implementation of seawater-based electrochemical H2O2synthesis.
研究领域:
材料科学
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电化学
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环境科学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Fahao Ma,Shuhua Wang,Xizhuang Liang,Cong Wang,Fengxia Tong,Zeyan Wang,Peng Wang,Yuanyuan Liu,Ying Dai,Zhaoke Zheng,Baibiao Huang
Electrocatalytic synthesis of hydrogen peroxide (H 2 O 2 ) via the two-electron oxygen reduction reaction (2e − ORR) is an ideal method for the on-site H 2 O 2 production. Herein, Ni 3 B is identified as an active, selective, and stable catalyst for ORR to generate H 2 O 2 , which exhibits a high selectivity of over 90 % and an onset potential of ∼0.7 V versus the reversible hydrogen electrode (RHE). Furthermore, the mass activity of Ni 3 B is about 16.5 A g -1 at 0.52 V (RHE), which is comparable to some noble metal alloys. Our experimental results suggest that the high performance of Ni 3 B originates from the alloying process of Ni and B atoms. The density functional theory calculations reveal that the inner B atoms with high electronegativity decrease the state density of Ni-3d orbital near the Fermi level relative to Ni, which optimizes the binding energy of OOH* and makes Ni 3 B a highly efficient and stable catalyst for the two-electron ORR.
研究领域:
催化
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电化学
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材料科学
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DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 10
·4823-4832
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IF 3.5
Haihui Hu,Ke Ma,Yuandong Yang,Na Jin,Linjie Zhang,Jinjie Qian,Lili Han
Hydrogen peroxide (H2O2) electrosynthesis via the two-electron oxygen reduction reaction (2e− ORR) represents a green alternative to the energy-intensive anthraquinone process. However, the practical application of this method is limited by the lack of cost-effective and high-performance electrocatalysts. Reported here is a hybrid catalyst composed of nickel (Ni) clusters immobilized onto the surface of two-dimensional siloxene nanosheets (Ni/siloxene), which exhibits excellent efficiency and selectivity in electrocatalytic oxygen reduction to H2O2 in an alkaline medium, demonstrating a standard 2e− pathway with >95% H2O2 selectivity across a wide potential range. Experimental results disclose that the high performance of Ni/siloxene can be traced to a synergy of the Ni clusters and the oxygen-rich surface of siloxene. Density functional theory (DFT) calculations further reveal a weakened interaction between Ni/siloxene and *OOH and the consequently reduced energy barrier for the *OOH protonation toward H2O2 desorption, thus leading to a high 2e− ORR reactivity and selectivity. This work provides a valuable and practical guidance for designing high-performance 2e− ORR electrocatalysts based on the rational engineering of the metal–support interaction.
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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纳米技术
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DOI
PubMed
高影响因子
Nature Communications
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2024
·Vol. 15
·期 1
·1-12
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IF 14.7
Sun Yining,Fan Kui,Li Jinze,Wang Lei,Yang Yusen,Li Zhenhua,Shao Mingfei,Duan Xue
The electrochemical oxygen reduction reaction (ORR) to produce hydrogen peroxide (H 2 O 2 ) is appealing due to its sustainability. However, its efficiency is compromised by the competing 4e − ORR pathway. In this work, we report a hierarchical carbon nanosheet array electrode with a single-atom Ni catalyst synthesized using organic molecule-intercalated layered double hydroxides as precursors. The electrode exhibits excellent 2e − ORR performance under alkaline conditions and achieves H 2 O 2 yield rates of 0.73 mol g cat −1 h −1 in the H-cell and 5.48 mol g cat −1 h −1 in the flow cell, outperforming most reported catalysts. The experimental results show that the Ni atoms selectively adsorb O 2 , while carbon nanosheets generate reactive hydrogen species, synergistically enhancing H 2 O 2 production. Furthermore, a coupling reaction system integrating the 2e − ORR with ethylene glycol oxidation significantly enhances H 2 O 2 yield rate to 7.30 mol g cat −1 h −1 while producing valuable glycolic acid. Moreover, we convert alkaline electrolyte containing H 2 O 2 directly into the downstream product sodium perborate to reduce the separation cost further. Techno-economic analysis validates the economic viability of this system.
研究领域:
电化学
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催化
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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
PubMed
高影响因子
Science Bulletin
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2025
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IF 21.1
Ergui Luo,Jingyi Liang,Kexuan Zhang,Xian Wang,Luozhen Jiang,Tianjun Hu,Junming Zhang,Junjie Ge,Jianfeng Jia
Electrochemical two-electron oxygen reduction reaction (2e − ORR) serves as an appealing approach for green hydrogen peroxide (H 2 O 2 ) production. However, the corresponding progress in efficient non-precious metal catalysts for acidic 2e − ORR has not kept pace, with the research model being almost confined to Co-based system. Here, guided by molecular dynamics simulations, the active nature and origin of pyrolyzed Cr−N 4 catalysts for ORR are unveiled, wherein the over-strong oxygen affinity of the Cr center is counterbalanced by a spontaneous axial O-coordination. By creating an oxidation-induced electron-deficient environment, the Cr−N 4 can be flexibly tailored for selective H 2 O 2 formation. A single-atom Cr−N 4 /C(O) catalyst is developed experimentally, which rivals and even slightly outperforms its Co-based counterpart in terms of selectivity (92% versus 71%) and productivity (202 versus 145 mmol g cat −1 h −1 ) for H 2 O 2 . More encouragingly, the Cr-based catalysts exhibit minimal reactivity towards H 2 O 2 -related side reactions, with the metal component being robust against leaching. This research marks the first identification of pyrolyzed Cr−N 4 catalysts as competent for acidic two-electron O 2 reduction to H 2 O 2 . The innovative models and insights offer profound guidance for the design of future-generation catalysts for electrochemical H 2 O 2 synthesis.
研究领域:
电催化
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材料科学
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能源化学
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可持续化学
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计算化学
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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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2023
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IF 9.9
Xiangyu You,Fang Hou,Tianzhu Xie,An Cai,Hongwei He,Guozhu Li,Fengbao Zhang,Wenchao Peng,Xiaobin Fan,Yang Li
Hypothesis Electrochemical manufacture of H 2 O 2 through the two-electron oxygen reduction reaction (2e – ORR), providing prospects of the distributed production of H 2 O 2 in remote regions, is considered a promising alternative to the energy-intensive anthraquinone oxidation process . Experiments In this study, one glucose-derived oxygen-enriched porous carbon material (labeled as HGC 500 ) is developed through a porogen-free strategy integrating structural and active site modification. Findings The superhydrophilic surface and porous structure together promote the mass transfer of reactants and accessibility of active sites in the aqueous reaction, while the abundant C O species (e.g., aldehyde groups) are taken for the main active site to facilitate the 2e – ORR catalytic process. Benefiting from the above merits, the obtained HGC 500 possesses superior performance with a selectivity of 92 % and mass activity of 43.6 A g cat –1 at 0.65 V ( vs. RHE). Besides, the HGC 500 can operate steadily for 12 h with the accumulation of H 2 O 2 reaching up to 4090±71 ppm and a Faradic efficiency of 95 %. The H 2 O 2 generated from the electrocatalytic process in 3 h can degrade a variety of organic pollutants (10 ppm) in 4–20 min, displaying the potential in practical applications.
研究领域:
材料科学
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电化学
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环境科学
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催化
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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）