{"title":"Revisiting the universal principle for the rational design of single-atom electrocatalysts","authors":"Haoxiang Xu, Daojian Cheng, Dapeng Cao, Xiao Cheng Zeng","doi":"10.1038/s41929-023-01106-z","DOIUrl":null,"url":null,"abstract":"The notion of descriptors has been widely used for assessing structure–activity relationships for many types of heterogenous catalytic reaction, as well as in searching for highly active single-atom catalysts (SACs). Here, with the aid of a machine-learning model for identifying key intrinsic properties of SACs, we revisit our previous descriptor φ [ , 339–348 (2018) ] and present φ′ to correlate the activity of graphene-based SACs for the oxygen reduction reaction, oxygen evolution reaction and hydrogen evolution reaction. The descriptor φ′ not only captures the activity trend among experimentally reported SACs, but can also help with the search for SACs to replace precious-metal-based commercial catalysts (for example Pt/C and IrO2), including Fe-pyridine/pyrrole-4N for the oxygen reduction reaction and Co-pyridine/pyrrole-4N for the oxygen evolution reaction (discovered in previous experimental studies). More importantly, we show that the descriptor φ′ can be broadly applicable to correlate SACs embedded in small-, mid- and large-sized macrocyclic complexes, so long as the active metal centre has the same local coordination environment. In 2018 a descriptor was put forward to correlate the activity of various electrocatalytic reactions on carbon-based single-atom catalysts, but some data the work was based on were later found to be incorrect. This work revisits and amends the original 2018 study while presenting a modified version of the φ descriptor.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":42.8000,"publicationDate":"2024-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.nature.com/articles/s41929-023-01106-z","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The notion of descriptors has been widely used for assessing structure–activity relationships for many types of heterogenous catalytic reaction, as well as in searching for highly active single-atom catalysts (SACs). Here, with the aid of a machine-learning model for identifying key intrinsic properties of SACs, we revisit our previous descriptor φ [ , 339–348 (2018) ] and present φ′ to correlate the activity of graphene-based SACs for the oxygen reduction reaction, oxygen evolution reaction and hydrogen evolution reaction. The descriptor φ′ not only captures the activity trend among experimentally reported SACs, but can also help with the search for SACs to replace precious-metal-based commercial catalysts (for example Pt/C and IrO2), including Fe-pyridine/pyrrole-4N for the oxygen reduction reaction and Co-pyridine/pyrrole-4N for the oxygen evolution reaction (discovered in previous experimental studies). More importantly, we show that the descriptor φ′ can be broadly applicable to correlate SACs embedded in small-, mid- and large-sized macrocyclic complexes, so long as the active metal centre has the same local coordination environment. In 2018 a descriptor was put forward to correlate the activity of various electrocatalytic reactions on carbon-based single-atom catalysts, but some data the work was based on were later found to be incorrect. This work revisits and amends the original 2018 study while presenting a modified version of the φ descriptor.
期刊介绍:
Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry.
Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.