{"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}
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.
期刊介绍:
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