通过制备Ni3N-MoN来稳定*OH中间体,用于可扩展的5-羟甲基糠醛电氧化

IF 3.5 3区 工程技术 Q2 ENGINEERING, CHEMICAL AIChE Journal Pub Date : 2024-12-13 DOI:10.1002/aic.18690
Shaowei Yang, Ying Guo, Jie Yang, Runze Gao, Zhibei Liao, Haidong Shen, Haoxi Wang, Lifeng Jiang, Buxing Han, Qiuyu Zhang, Hepeng Zhang
{"title":"通过制备Ni3N-MoN来稳定*OH中间体,用于可扩展的5-羟甲基糠醛电氧化","authors":"Shaowei Yang, Ying Guo, Jie Yang, Runze Gao, Zhibei Liao, Haidong Shen, Haoxi Wang, Lifeng Jiang, Buxing Han, Qiuyu Zhang, Hepeng Zhang","doi":"10.1002/aic.18690","DOIUrl":null,"url":null,"abstract":"Achieving large-scale coupling of organic electrooxidation and the hydrogen evolution reaction, while understanding the competition between organic electrooxidation and oxygen evolution reaction (OER), is a significant challenge. In this study, using Ni<sub>3</sub>N-MoN/NF, an efficient heterojunction electrocatalyst as both anode and cathode in a 50 cm<sup>2</sup> continuous flow reactor, we achieved a total current of ~20 A at 2.6 V. This resulted in the highest single-pass 5-hydroxymethylfurfural conversion efficiency (0.049 mmol cm<sup>−2</sup> min<sup>−1</sup>) and gram-level production of 2,5-furandicarboxylic acid. Theoretical studies revealed that MoN accelerated *OH formation and increased its deprotonation energy barrier, leading to *OH accumulation, effectively promoting organic electrooxidation and inhibiting OER. We anticipate that our foundation in understanding the reaction mechanism and catalyst design strategy can be extended to a wider range of anodic oxidation reactions.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"41 1","pages":""},"PeriodicalIF":3.5000,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Stabilizing *OH intermediate by fabricating Ni3N-MoN for scalable 5-hydroxymethylfurfural electrooxidation\",\"authors\":\"Shaowei Yang, Ying Guo, Jie Yang, Runze Gao, Zhibei Liao, Haidong Shen, Haoxi Wang, Lifeng Jiang, Buxing Han, Qiuyu Zhang, Hepeng Zhang\",\"doi\":\"10.1002/aic.18690\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Achieving large-scale coupling of organic electrooxidation and the hydrogen evolution reaction, while understanding the competition between organic electrooxidation and oxygen evolution reaction (OER), is a significant challenge. In this study, using Ni<sub>3</sub>N-MoN/NF, an efficient heterojunction electrocatalyst as both anode and cathode in a 50 cm<sup>2</sup> continuous flow reactor, we achieved a total current of ~20 A at 2.6 V. This resulted in the highest single-pass 5-hydroxymethylfurfural conversion efficiency (0.049 mmol cm<sup>−2</sup> min<sup>−1</sup>) and gram-level production of 2,5-furandicarboxylic acid. Theoretical studies revealed that MoN accelerated *OH formation and increased its deprotonation energy barrier, leading to *OH accumulation, effectively promoting organic electrooxidation and inhibiting OER. We anticipate that our foundation in understanding the reaction mechanism and catalyst design strategy can be extended to a wider range of anodic oxidation reactions.\",\"PeriodicalId\":120,\"journal\":{\"name\":\"AIChE Journal\",\"volume\":\"41 1\",\"pages\":\"\"},\"PeriodicalIF\":3.5000,\"publicationDate\":\"2024-12-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"AIChE Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1002/aic.18690\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"AIChE Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1002/aic.18690","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0

摘要

实现有机电氧化和析氢反应的大规模耦合,同时理解有机电氧化和析氧反应(OER)之间的竞争是一个重大挑战。在本研究中,采用高效异质结电催化剂Ni3N-MoN/NF作为阳极和阴极,在50 cm2的连续流反应器中,我们在2.6 V下获得了~20 a的总电流。这导致了最高的单道5-羟甲基糠醛转化效率(0.049 mmol cm−2 min−1)和克级2,5-呋喃二羧酸的生产。理论研究表明,MoN加速*OH的形成,增加其去质子能垒,导致*OH积聚,有效促进有机电氧化,抑制OER。我们期望我们在了解反应机理和催化剂设计策略方面的基础可以扩展到更广泛的阳极氧化反应。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
Stabilizing *OH intermediate by fabricating Ni3N-MoN for scalable 5-hydroxymethylfurfural electrooxidation
Achieving large-scale coupling of organic electrooxidation and the hydrogen evolution reaction, while understanding the competition between organic electrooxidation and oxygen evolution reaction (OER), is a significant challenge. In this study, using Ni3N-MoN/NF, an efficient heterojunction electrocatalyst as both anode and cathode in a 50 cm2 continuous flow reactor, we achieved a total current of ~20 A at 2.6 V. This resulted in the highest single-pass 5-hydroxymethylfurfural conversion efficiency (0.049 mmol cm−2 min−1) and gram-level production of 2,5-furandicarboxylic acid. Theoretical studies revealed that MoN accelerated *OH formation and increased its deprotonation energy barrier, leading to *OH accumulation, effectively promoting organic electrooxidation and inhibiting OER. We anticipate that our foundation in understanding the reaction mechanism and catalyst design strategy can be extended to a wider range of anodic oxidation reactions.
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
AIChE Journal
AIChE Journal 工程技术-工程:化工
CiteScore
7.10
自引率
10.80%
发文量
411
审稿时长
3.6 months
期刊介绍: The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.
期刊最新文献
New strategy for predicting liquid–liquid equilibrium near critical point using global renormalization group theory Integration of Pt/Fe-silicalite-1 and acidic zeolite as a bifunctional catalyst for boosting ethane dehydroaromatization Magnetic particle capture in high-gradient magnetic separation: A theoretical and experimental study Synergistic plasmon resonance hybridization of iron-dispersed MoO3−x/MXene for enhanced nitrogen photothermal reduction Machine learning potential model for accelerating quantum chemistry-driven property prediction and molecular design
×
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
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 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 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1