{"title":"Activity trends of Pd clusters supported on C2N for oxygen evolution and reduction reactions","authors":"Longkun Huang, Min Li, Hui Wang, Long Zhang","doi":"10.1063/5.0196323","DOIUrl":null,"url":null,"abstract":"Developing highly efficient electrocatalysts for the oxygen evolution reaction (OER) and reduction reaction (ORR) is crucial for future renewable energy technology. Here, we use first-principles calculations combined with genetic algorithm to determine the structures of various Pd clusters supported on experimentally available C2N monolayer and evaluate the OER and ORR performance. Our findings show that the activity of the supported Pd clusters is closely linked to the local geometrical and electronic structure of the active site. Furthermore, we establish the activity trends of the clusters based on the adsorption free energies of intermediates. In particular, C2N supported Pd7 and Pd8 clusters exhibit outstanding OER activity with low overpotentials. We identify a volcano relation for the OER on the clusters, suggesting that the high activity of the cluster is related to the moderate adsorption strength of intermediates. Mechanistic analysis indicates that the second water formation is the potential-determining step for ORR on the clusters due to the strong adsorption of *OH. Additionally, we identify a linear scaling relationship between the ORR overpotentials and adsorption free energies of *OH, demonstrating that reducing the adsorption strength of reaction intermediates on Pd clusters can improve the activity. This work unravels the activity trends of cluster catalysts and provides strategies for the rational design of highly efficient single-cluster catalysts for OER and ORR.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"176 1","pages":""},"PeriodicalIF":3.5000,"publicationDate":"2024-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Physics Letters","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1063/5.0196323","RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"PHYSICS, APPLIED","Score":null,"Total":0}
引用次数: 0
Abstract
Developing highly efficient electrocatalysts for the oxygen evolution reaction (OER) and reduction reaction (ORR) is crucial for future renewable energy technology. Here, we use first-principles calculations combined with genetic algorithm to determine the structures of various Pd clusters supported on experimentally available C2N monolayer and evaluate the OER and ORR performance. Our findings show that the activity of the supported Pd clusters is closely linked to the local geometrical and electronic structure of the active site. Furthermore, we establish the activity trends of the clusters based on the adsorption free energies of intermediates. In particular, C2N supported Pd7 and Pd8 clusters exhibit outstanding OER activity with low overpotentials. We identify a volcano relation for the OER on the clusters, suggesting that the high activity of the cluster is related to the moderate adsorption strength of intermediates. Mechanistic analysis indicates that the second water formation is the potential-determining step for ORR on the clusters due to the strong adsorption of *OH. Additionally, we identify a linear scaling relationship between the ORR overpotentials and adsorption free energies of *OH, demonstrating that reducing the adsorption strength of reaction intermediates on Pd clusters can improve the activity. This work unravels the activity trends of cluster catalysts and provides strategies for the rational design of highly efficient single-cluster catalysts for OER and ORR.
期刊介绍:
Applied Physics Letters (APL) features concise, up-to-date reports on significant new findings in applied physics. Emphasizing rapid dissemination of key data and new physical insights, APL offers prompt publication of new experimental and theoretical papers reporting applications of physics phenomena to all branches of science, engineering, and modern technology.
In addition to regular articles, the journal also publishes invited Fast Track, Perspectives, and in-depth Editorials which report on cutting-edge areas in applied physics.
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Fast Track articles are invited original research articles that report results that are particularly novel and important or provide a significant advancement in an emerging field. Because of the urgency and scientific importance of the work, the peer review process is accelerated. If, during the review process, it becomes apparent that the paper does not meet the Fast Track criterion, it is returned to a normal track.