Pan Guo, Bo Liu, Fengdi Tu, Yunkun Dai, Ziyu Zhang, Yunfei Xia, Miao Ma, Yunlong Zhang, Lei Zhao and Zhenbo Wang
{"title":"通过改变酸性氧还原双活性位点上的氧吸附构型和反应途径来打破萨巴蒂尔顶点","authors":"Pan Guo, Bo Liu, Fengdi Tu, Yunkun Dai, Ziyu Zhang, Yunfei Xia, Miao Ma, Yunlong Zhang, Lei Zhao and Zhenbo Wang","doi":"10.1039/D4EE00823E","DOIUrl":null,"url":null,"abstract":"<p >Single-atom catalysts are promising alternatives to platinum-based catalysts for the oxygen reduction reaction (ORR). However, the ORR process with multiple-step proton-coupled electron transfer occurring on a single-active site follows the linear scaling relation, making it difficult to break through Sabatier's limitation. Herein, we switch the ORR process from a sluggish associative pathway to a favorable dissociative one by constructing diatomic active sites with a Pt-like adsorption configuration, enabling the thermodynamic limit potential to break through Sabatier's vertex. Theoretical calculations and <em>in situ</em> characterization fully corroborate the Pt-like adsorption configuration of O<small><sub>2</sub></small> on Ru–Fe dual sites, which renders the direct cleavage of O–O bonds and avoids the formation of *OOH intermediates, thus boosting the ORR kinetics. Consequently, the well-designed Ru and Fe co-doped catalysts with dual active sites (Ru, Fe-NC DAS) deliver extraordinary ORR catalytic performance, as manifested by the high half-wave potential of 0.843 V in an acid medium and a record-breaking peak power density of 1.152 W cm<small><sup>−2</sup></small> in H<small><sub>2</sub></small>/O<small><sub>2</sub></small> fuel cells, ranking at the top level of non-Pt catalysts reported so far. This work provides a new approach for designing highly efficient atomically dispersed catalysts and steering the corresponding catalytic reaction mechanisms.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 9","pages":" 3077-3087"},"PeriodicalIF":30.8000,"publicationDate":"2024-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Breaking Sabatier's vertex via switching the oxygen adsorption configuration and reaction pathway on dual active sites for acidic oxygen reduction†\",\"authors\":\"Pan Guo, Bo Liu, Fengdi Tu, Yunkun Dai, Ziyu Zhang, Yunfei Xia, Miao Ma, Yunlong Zhang, Lei Zhao and Zhenbo Wang\",\"doi\":\"10.1039/D4EE00823E\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Single-atom catalysts are promising alternatives to platinum-based catalysts for the oxygen reduction reaction (ORR). However, the ORR process with multiple-step proton-coupled electron transfer occurring on a single-active site follows the linear scaling relation, making it difficult to break through Sabatier's limitation. Herein, we switch the ORR process from a sluggish associative pathway to a favorable dissociative one by constructing diatomic active sites with a Pt-like adsorption configuration, enabling the thermodynamic limit potential to break through Sabatier's vertex. Theoretical calculations and <em>in situ</em> characterization fully corroborate the Pt-like adsorption configuration of O<small><sub>2</sub></small> on Ru–Fe dual sites, which renders the direct cleavage of O–O bonds and avoids the formation of *OOH intermediates, thus boosting the ORR kinetics. Consequently, the well-designed Ru and Fe co-doped catalysts with dual active sites (Ru, Fe-NC DAS) deliver extraordinary ORR catalytic performance, as manifested by the high half-wave potential of 0.843 V in an acid medium and a record-breaking peak power density of 1.152 W cm<small><sup>−2</sup></small> in H<small><sub>2</sub></small>/O<small><sub>2</sub></small> fuel cells, ranking at the top level of non-Pt catalysts reported so far. This work provides a new approach for designing highly efficient atomically dispersed catalysts and steering the corresponding catalytic reaction mechanisms.</p>\",\"PeriodicalId\":72,\"journal\":{\"name\":\"Energy & Environmental Science\",\"volume\":\" 9\",\"pages\":\" 3077-3087\"},\"PeriodicalIF\":30.8000,\"publicationDate\":\"2024-03-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Energy & Environmental Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/ee/d4ee00823e\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy & Environmental Science","FirstCategoryId":"88","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/ee/d4ee00823e","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Breaking Sabatier's vertex via switching the oxygen adsorption configuration and reaction pathway on dual active sites for acidic oxygen reduction†
Single-atom catalysts are promising alternatives to platinum-based catalysts for the oxygen reduction reaction (ORR). However, the ORR process with multiple-step proton-coupled electron transfer occurring on a single-active site follows the linear scaling relation, making it difficult to break through Sabatier's limitation. Herein, we switch the ORR process from a sluggish associative pathway to a favorable dissociative one by constructing diatomic active sites with a Pt-like adsorption configuration, enabling the thermodynamic limit potential to break through Sabatier's vertex. Theoretical calculations and in situ characterization fully corroborate the Pt-like adsorption configuration of O2 on Ru–Fe dual sites, which renders the direct cleavage of O–O bonds and avoids the formation of *OOH intermediates, thus boosting the ORR kinetics. Consequently, the well-designed Ru and Fe co-doped catalysts with dual active sites (Ru, Fe-NC DAS) deliver extraordinary ORR catalytic performance, as manifested by the high half-wave potential of 0.843 V in an acid medium and a record-breaking peak power density of 1.152 W cm−2 in H2/O2 fuel cells, ranking at the top level of non-Pt catalysts reported so far. This work provides a new approach for designing highly efficient atomically dispersed catalysts and steering the corresponding catalytic reaction mechanisms.
期刊介绍:
Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences."
Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).