{"title":"调节氧化途径机制,实现可持续酸性水氧化","authors":"Xuejie Cao, Hongye Qin, Jinyang Zhang, Xiaojie Chen, Lifang Jiao","doi":"10.1021/jacs.4c12942","DOIUrl":null,"url":null,"abstract":"The advancement of acid-stable oxygen evolution reaction (OER) electrocatalysts is crucial for efficient hydrogen production through proton exchange membrane (PEM) water electrolysis. Unfortunately, the activity of electrocatalysts is constrained by a linear scaling relationship in the adsorbed evolution mechanism, while the lattice-oxygen-mediated mechanism undermines stability. Here, we propose a heterogeneous dual-site oxide pathway mechanism (OPM) that avoids these limitations through direct dioxygen radical coupling. A combination of Lewis acid (Cr) and Ru to form solid solution oxides (Cr<sub><i>x</i></sub>Ru<sub>1–<i>x</i></sub>O<sub>2</sub>) promotes OH adsorption and shortens the dual-site distance, which facilitates the formation of *O radical and promotes the coupling of dioxygen radical, thereby altering the OER mechanism to a Cr–Ru dual-site OPM. The Cr<sub>0.6</sub>Ru<sub>0.4</sub>O<sub>2</sub> catalyst demonstrates a lower overpotential than that of RuO<sub>2</sub> and maintains stable operation for over 350 h in a PEM water electrolyzer at 300 mA cm<sup>–2</sup>. This mechanism regulation strategy paves the way for an optimal catalytic pathway, essential for large-scale green hydrogen production.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"19 1","pages":""},"PeriodicalIF":14.4000,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Regulation of Oxide Pathway Mechanism for Sustainable Acidic Water Oxidation\",\"authors\":\"Xuejie Cao, Hongye Qin, Jinyang Zhang, Xiaojie Chen, Lifang Jiao\",\"doi\":\"10.1021/jacs.4c12942\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The advancement of acid-stable oxygen evolution reaction (OER) electrocatalysts is crucial for efficient hydrogen production through proton exchange membrane (PEM) water electrolysis. Unfortunately, the activity of electrocatalysts is constrained by a linear scaling relationship in the adsorbed evolution mechanism, while the lattice-oxygen-mediated mechanism undermines stability. Here, we propose a heterogeneous dual-site oxide pathway mechanism (OPM) that avoids these limitations through direct dioxygen radical coupling. A combination of Lewis acid (Cr) and Ru to form solid solution oxides (Cr<sub><i>x</i></sub>Ru<sub>1–<i>x</i></sub>O<sub>2</sub>) promotes OH adsorption and shortens the dual-site distance, which facilitates the formation of *O radical and promotes the coupling of dioxygen radical, thereby altering the OER mechanism to a Cr–Ru dual-site OPM. The Cr<sub>0.6</sub>Ru<sub>0.4</sub>O<sub>2</sub> catalyst demonstrates a lower overpotential than that of RuO<sub>2</sub> and maintains stable operation for over 350 h in a PEM water electrolyzer at 300 mA cm<sup>–2</sup>. This mechanism regulation strategy paves the way for an optimal catalytic pathway, essential for large-scale green hydrogen production.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"19 1\",\"pages\":\"\"},\"PeriodicalIF\":14.4000,\"publicationDate\":\"2024-11-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jacs.4c12942\",\"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":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c12942","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Regulation of Oxide Pathway Mechanism for Sustainable Acidic Water Oxidation
The advancement of acid-stable oxygen evolution reaction (OER) electrocatalysts is crucial for efficient hydrogen production through proton exchange membrane (PEM) water electrolysis. Unfortunately, the activity of electrocatalysts is constrained by a linear scaling relationship in the adsorbed evolution mechanism, while the lattice-oxygen-mediated mechanism undermines stability. Here, we propose a heterogeneous dual-site oxide pathway mechanism (OPM) that avoids these limitations through direct dioxygen radical coupling. A combination of Lewis acid (Cr) and Ru to form solid solution oxides (CrxRu1–xO2) promotes OH adsorption and shortens the dual-site distance, which facilitates the formation of *O radical and promotes the coupling of dioxygen radical, thereby altering the OER mechanism to a Cr–Ru dual-site OPM. The Cr0.6Ru0.4O2 catalyst demonstrates a lower overpotential than that of RuO2 and maintains stable operation for over 350 h in a PEM water electrolyzer at 300 mA cm–2. This mechanism regulation strategy paves the way for an optimal catalytic pathway, essential for large-scale green hydrogen production.
期刊介绍:
The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.