用软界面分子介质催化工业过氧化氢生产。

IF 20.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Dawei Xi, Yuheng Wu, Yuli Li, Zifei Yan, Richard Y Liu, Michael J Aziz
{"title":"用软界面分子介质催化工业过氧化氢生产。","authors":"Dawei Xi, Yuheng Wu, Yuli Li, Zifei Yan, Richard Y Liu, Michael J Aziz","doi":"10.1038/s41557-025-01940-7","DOIUrl":null,"url":null,"abstract":"<p><p>Hydrogen peroxide is manufactured industrially via the anthraquinone autoxidation process-a typical thermocatalytic non-aqueous method. Despite a high interest in using renewable electricity to drive such processes, electrifying non-aqueous syntheses remains a substantial challenge. Here we present a multi-phase electrochemical anthraquinone autoxidation process that leverages an aqueous-non-aqueous interfacial proton-coupled electron transfer method facilitated by heterogeneous molecular mediation. This design enables the reduction of aqueous anthraquinones with high efficiency at high current densities, using only carbon electrodes. The method operates with high selectivity through a quinhydrone intermediate and prevents the over-reduction of aromatics during thermocatalytic hydrogenation. This approach combines the benefits of aqueous electrochemistry with those of the traditional non-aqueous process to achieve high current density electrochemistry with rapid kinetics and mass transport, while avoiding unwanted electrolyte in the hydrogen peroxide product. This strategy bridges aqueous electrochemistry with non-aqueous chemistry and establishes a framework for the electrification and decentralization of other non-aqueous chemical processes.</p>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":20.2000,"publicationDate":"2025-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Electrifying industrial hydrogen peroxide production via soft interfacial molecular mediation.\",\"authors\":\"Dawei Xi, Yuheng Wu, Yuli Li, Zifei Yan, Richard Y Liu, Michael J Aziz\",\"doi\":\"10.1038/s41557-025-01940-7\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Hydrogen peroxide is manufactured industrially via the anthraquinone autoxidation process-a typical thermocatalytic non-aqueous method. Despite a high interest in using renewable electricity to drive such processes, electrifying non-aqueous syntheses remains a substantial challenge. Here we present a multi-phase electrochemical anthraquinone autoxidation process that leverages an aqueous-non-aqueous interfacial proton-coupled electron transfer method facilitated by heterogeneous molecular mediation. This design enables the reduction of aqueous anthraquinones with high efficiency at high current densities, using only carbon electrodes. The method operates with high selectivity through a quinhydrone intermediate and prevents the over-reduction of aromatics during thermocatalytic hydrogenation. This approach combines the benefits of aqueous electrochemistry with those of the traditional non-aqueous process to achieve high current density electrochemistry with rapid kinetics and mass transport, while avoiding unwanted electrolyte in the hydrogen peroxide product. This strategy bridges aqueous electrochemistry with non-aqueous chemistry and establishes a framework for the electrification and decentralization of other non-aqueous chemical processes.</p>\",\"PeriodicalId\":18909,\"journal\":{\"name\":\"Nature chemistry\",\"volume\":\" \",\"pages\":\"\"},\"PeriodicalIF\":20.2000,\"publicationDate\":\"2025-09-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1038/s41557-025-01940-7\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature chemistry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1038/s41557-025-01940-7","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

摘要

过氧化氢的工业生产是通过蒽醌自氧化法-一种典型的热催化非水法。尽管人们对使用可再生电力来推动这一过程非常感兴趣,但非水合成的电气化仍然是一个重大挑战。在这里,我们提出了一种多相电化学蒽醌自氧化过程,该过程利用非均相分子中介促进的水-非水界面质子耦合电子传递方法。这种设计能够在高电流密度下高效地还原含水蒽醌,仅使用碳电极。该方法通过醌醌中间体具有高选择性,并且在热催化加氢过程中防止了芳烃的过度还原。这种方法结合了水电化学和传统非水工艺的优点,实现了具有快速动力学和质量传递的高电流密度电化学,同时避免了过氧化氢产物中不需要的电解质。该策略将水电化学与非水化学连接起来,并为其他非水化学过程的电气化和分散化建立了框架。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Electrifying industrial hydrogen peroxide production via soft interfacial molecular mediation.

Hydrogen peroxide is manufactured industrially via the anthraquinone autoxidation process-a typical thermocatalytic non-aqueous method. Despite a high interest in using renewable electricity to drive such processes, electrifying non-aqueous syntheses remains a substantial challenge. Here we present a multi-phase electrochemical anthraquinone autoxidation process that leverages an aqueous-non-aqueous interfacial proton-coupled electron transfer method facilitated by heterogeneous molecular mediation. This design enables the reduction of aqueous anthraquinones with high efficiency at high current densities, using only carbon electrodes. The method operates with high selectivity through a quinhydrone intermediate and prevents the over-reduction of aromatics during thermocatalytic hydrogenation. This approach combines the benefits of aqueous electrochemistry with those of the traditional non-aqueous process to achieve high current density electrochemistry with rapid kinetics and mass transport, while avoiding unwanted electrolyte in the hydrogen peroxide product. This strategy bridges aqueous electrochemistry with non-aqueous chemistry and establishes a framework for the electrification and decentralization of other non-aqueous chemical processes.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Nature chemistry
Nature chemistry 化学-化学综合
CiteScore
29.60
自引率
1.40%
发文量
226
审稿时长
1.7 months
期刊介绍: Nature Chemistry is a monthly journal that publishes groundbreaking and significant research in all areas of chemistry. It covers traditional subjects such as analytical, inorganic, organic, and physical chemistry, as well as a wide range of other topics including catalysis, computational and theoretical chemistry, and environmental chemistry. The journal also features interdisciplinary research at the interface of chemistry with biology, materials science, nanotechnology, and physics. Manuscripts detailing such multidisciplinary work are encouraged, as long as the central theme pertains to chemistry. Aside from primary research, Nature Chemistry publishes review articles, news and views, research highlights from other journals, commentaries, book reviews, correspondence, and analysis of the broader chemical landscape. It also addresses crucial issues related to education, funding, policy, intellectual property, and the societal impact of chemistry. Nature Chemistry is dedicated to ensuring the highest standards of original research through a fair and rigorous review process. It offers authors maximum visibility for their papers, access to a broad readership, exceptional copy editing and production standards, rapid publication, and independence from academic societies and other vested interests. Overall, Nature Chemistry aims to be the authoritative voice of the global chemical community.
×
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:604180095
Book学术官方微信