Vacancy‐Activated B‐Doping for Efficient 2e‐ Oxygen Reduction through Suppressing H2O2 Decomposition at High Overpotential

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Wangyang Cui, Zhiyuan Zhen, Yuanyuan Sun, Xiaofeng Liu, Jinhui Chen, Sijia Liu, Hao Ren, Yan Lin, Mingbo Wu, Zhongtao Li
{"title":"Vacancy‐Activated B‐Doping for Efficient 2e‐ Oxygen Reduction through Suppressing H2O2 Decomposition at High Overpotential","authors":"Wangyang Cui, Zhiyuan Zhen, Yuanyuan Sun, Xiaofeng Liu, Jinhui Chen, Sijia Liu, Hao Ren, Yan Lin, Mingbo Wu, Zhongtao Li","doi":"10.1002/anie.202423056","DOIUrl":null,"url":null,"abstract":"The production of hydrogen peroxide (H2O2) through two‐electron oxygen reduction reaction (2e‐ ORR) has emerged as a more environmentally friendly alternative to the traditional anthraquinone method. Although oxidized carbon catalysts have intensive developed due to their high selectivity and activity, the yield and conversion rate of H2O2 under high overpotential still limited. The produced H2O2 was rapidly consumed by the increased intensity of H2O2 reduction, which could ascribe to decomposition of peroxide radicals under high voltage in the carbon catalyst. To overcome this issue, a B doped carbon have been developed to catalyze 2e‐ ORR with high efficient through suppressing H2O2 decomposition at high potential. Thus, thermal reducing of oxygen containing groups (OCGs) on graphite could construct defects and vacancies, which in situ convert to B‐Cx subunits on the edge of graphene sheets. The introduction of B‐Cx effectively prevented the decomposition of the *O‐O bond and provided suitable adsorption capacity for *OOH, achieving excellent selectivity for the 2e‐ ORR across a wide voltage range. Finally, a remarkable H2O2 yield of 7.91 mmol cm−2 h−1 was delivered at an industrial current density of 600 mA cm−2, which could provide “green” pathway for scale‐upable synthesis H2O2.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"36 1","pages":""},"PeriodicalIF":16.1000,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Angewandte Chemie International Edition","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/anie.202423056","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

Abstract

The production of hydrogen peroxide (H2O2) through two‐electron oxygen reduction reaction (2e‐ ORR) has emerged as a more environmentally friendly alternative to the traditional anthraquinone method. Although oxidized carbon catalysts have intensive developed due to their high selectivity and activity, the yield and conversion rate of H2O2 under high overpotential still limited. The produced H2O2 was rapidly consumed by the increased intensity of H2O2 reduction, which could ascribe to decomposition of peroxide radicals under high voltage in the carbon catalyst. To overcome this issue, a B doped carbon have been developed to catalyze 2e‐ ORR with high efficient through suppressing H2O2 decomposition at high potential. Thus, thermal reducing of oxygen containing groups (OCGs) on graphite could construct defects and vacancies, which in situ convert to B‐Cx subunits on the edge of graphene sheets. The introduction of B‐Cx effectively prevented the decomposition of the *O‐O bond and provided suitable adsorption capacity for *OOH, achieving excellent selectivity for the 2e‐ ORR across a wide voltage range. Finally, a remarkable H2O2 yield of 7.91 mmol cm−2 h−1 was delivered at an industrial current density of 600 mA cm−2, which could provide “green” pathway for scale‐upable synthesis H2O2.
空位活化B掺杂抑制高过电位下H2O2分解,有效还原2e -氧
通过双电子氧还原反应(2e - ORR)生产过氧化氢(H2O2)已成为传统蒽醌方法的一种更环保的替代方法。虽然氧化碳催化剂因其高选择性和高活性而得到了广泛的发展,但在高过电位条件下H2O2的产率和转化率仍然有限。随着H2O2还原强度的增加,生成的H2O2被迅速消耗,这可能是由于碳催化剂中过氧化自由基在高压下分解所致。为了克服这一问题,研究人员开发了一种B掺杂碳,通过抑制H2O2在高电位下的分解,高效催化2e - ORR。因此,石墨上的含氧基团(ocg)的热还原可以形成缺陷和空位,这些缺陷和空位在石墨烯片的边缘原位转化为B - Cx亚基。B - Cx的引入有效地阻止了*O - O键的分解,并为*OOH提供了合适的吸附能力,在宽电压范围内实现了对2e - ORR的优异选择性。最后,在600 mA cm−2的工业电流密度下,H2O2的产率达到7.91 mmol cm−2 h−1,这为大规模合成H2O2提供了“绿色”途径。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信