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Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production
Peng, Wei1; Liu, Jiaxin1; Liu, Xiaoqing1; Wang, Liqun2; Yin, Lichang3; Tan, Haotian1; Hou, Feng1; Liang, Ji1
通讯作者Wang, Liqun(wlxywlq@mail.tjnu.edu.cn) ; Yin, Lichang(lcyin@imr.ac.cn) ; Hou, Feng(houf@tju.edu.cn) ; Liang, Ji(liangji@tju.edu.cn)
2023-07-22
发表期刊NATURE COMMUNICATIONS
卷号14期号:1页码:11
摘要Electrocatalytic hydrogen peroxide (H2O2) production via the two-electron oxygen reduction reaction is a promising alternative to the energy-intensive and high-pollution anthraquinone oxidation process. However, developing advanced electrocatalysts with high H2O2 yield, selectivity, and durability is still challenging, because of the limited quantity and easy passivation of active sites on typical metal-containing catalysts, especially for the state-of-the-art single-atom ones. To address this, we report a graphene/mesoporous carbon composite for high-rate and high-efficiency 2e- oxygen reduction catalysis. The coordination of pyrrolic-N sites -modulates the adsorption configuration of the *OOH species to provide a kinetically favorable pathway for H2O2 production. Consequently, the H2O2 yield approaches 30 mol g-1 h-1 with a Faradaic efficiency of 80% and excellent durability, yielding a high H2O2 concentration of 7.2 g L-1. This strategy of manipulating the adsorption configuration of reactants with multiple non-metal active sites provides a strategy to design efficient and durable metal-free electrocatalyst for 2e- oxygen reduction. A graphene/mesoporous carbon composite presents rapid and efficient H2O2 electrosynthesis capability by two-electron oxygen reduction catalysis which is facilitated by the presence of multiple pyrrolic nitrogen dopants within the material.
资助者National Natural Science Foundation of China (National Science Foundation of China) ; National Natural Science Foundation of China ; Tianjin University International Education Program for Outstanding Doctoral Thesis
DOI10.1038/s41467-023-40118-y
收录类别SCI
语种英语
资助项目National Natural Science Foundation of China (National Science Foundation of China)[22179093] ; National Natural Science Foundation of China[C2-2021-004] ; Tianjin University International Education Program for Outstanding Doctoral Thesis
WOS研究方向Science & Technology - Other Topics
WOS类目Multidisciplinary Sciences
WOS记录号WOS:001111938400006
出版者NATURE PORTFOLIO
引用统计
被引频次:144[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/182989
专题中国科学院金属研究所
通讯作者Wang, Liqun; Yin, Lichang; Hou, Feng; Liang, Ji
作者单位1.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin 300072, Peoples R China
2.Tianjin Normal Univ, Coll Phys & Mat Sci, Appl Phys Dept, Tianjin 300387, Peoples R China
3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China
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GB/T 7714
Peng, Wei,Liu, Jiaxin,Liu, Xiaoqing,et al. Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production[J]. NATURE COMMUNICATIONS,2023,14(1):11.
APA Peng, Wei.,Liu, Jiaxin.,Liu, Xiaoqing.,Wang, Liqun.,Yin, Lichang.,...&Liang, Ji.(2023).Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production.NATURE COMMUNICATIONS,14(1),11.
MLA Peng, Wei,et al."Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production".NATURE COMMUNICATIONS 14.1(2023):11.
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