{"title":"高通量筛选用于高活性和选择性二氧化碳还原反应的 1 T-TMD 单原子催化剂:计算和机器学习见解","authors":"Shen Xi , Peng Zhao , Cheng He , Wenxue Zhang","doi":"10.1016/j.jcat.2024.115610","DOIUrl":null,"url":null,"abstract":"<div><p>The study of transition metals and various possible surface compositions has sparked great interest in low-cost materials, which exhibit high activity and selectivity in catalysis. While various single-atom catalysts loaded on transition metal dichalcogenide (TMD) substrates with excellent CO<sub>2</sub> reduction performance have been identified, the relationship between catalytic activity and the intrinsic properties of TMD single-atom catalysts remains unclear. Hence, a high-throughput first-principle computational approach is proposed to screen 24 transition metals anchored on 8 TMD monolayers to determine their catalytic activity in CO<sub>2</sub>RR. The results show that Fe@CoS<sub>2</sub>, Pt@TiTe<sub>2</sub> and Co@CoS<sub>2</sub> exhibit exceptional performances with low CO<sub>2</sub>RR limiting-potentials of −0.045 eV, 0.75 eV, and 0.54 eV, respectively, showcasing selective pathways towards formic acid (HCOOH), methane (CH<sub>4</sub>), and methanol (CH<sub>3</sub>OH). Employing the Sure Independence Screening and Sparsifying Operator method(SISSO), key descriptors linking the performance of single-atom catalysts with their intrinsic features are identified, providing insights for the discovery of superior CO<sub>2</sub>RR catalysts. Moreover, it was observed that a feature of the anchored single atom, the difference between covalent radius and atomic radius (CR-R), is associated with multiple crucial reaction steps, exhibiting a strong linear relationship with the charge transfer of *COOH. This work not only identifies promising CO<sub>2</sub>RR catalysts but also establishes a predictive framework for screening catalysts based on their intrinsic properties, paving the way for future advancements in CO<sub>2</sub> reduction research.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":6.5000,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"High-throughput screening of single-atom catalysts on 1 T-TMD for highly active and selective CO2 reduction reaction: Computational and machine learning insights\",\"authors\":\"Shen Xi , Peng Zhao , Cheng He , Wenxue Zhang\",\"doi\":\"10.1016/j.jcat.2024.115610\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The study of transition metals and various possible surface compositions has sparked great interest in low-cost materials, which exhibit high activity and selectivity in catalysis. While various single-atom catalysts loaded on transition metal dichalcogenide (TMD) substrates with excellent CO<sub>2</sub> reduction performance have been identified, the relationship between catalytic activity and the intrinsic properties of TMD single-atom catalysts remains unclear. Hence, a high-throughput first-principle computational approach is proposed to screen 24 transition metals anchored on 8 TMD monolayers to determine their catalytic activity in CO<sub>2</sub>RR. The results show that Fe@CoS<sub>2</sub>, Pt@TiTe<sub>2</sub> and Co@CoS<sub>2</sub> exhibit exceptional performances with low CO<sub>2</sub>RR limiting-potentials of −0.045 eV, 0.75 eV, and 0.54 eV, respectively, showcasing selective pathways towards formic acid (HCOOH), methane (CH<sub>4</sub>), and methanol (CH<sub>3</sub>OH). Employing the Sure Independence Screening and Sparsifying Operator method(SISSO), key descriptors linking the performance of single-atom catalysts with their intrinsic features are identified, providing insights for the discovery of superior CO<sub>2</sub>RR catalysts. Moreover, it was observed that a feature of the anchored single atom, the difference between covalent radius and atomic radius (CR-R), is associated with multiple crucial reaction steps, exhibiting a strong linear relationship with the charge transfer of *COOH. This work not only identifies promising CO<sub>2</sub>RR catalysts but also establishes a predictive framework for screening catalysts based on their intrinsic properties, paving the way for future advancements in CO<sub>2</sub> reduction research.</p></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-06-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021951724003233\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021951724003233","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
High-throughput screening of single-atom catalysts on 1 T-TMD for highly active and selective CO2 reduction reaction: Computational and machine learning insights
The study of transition metals and various possible surface compositions has sparked great interest in low-cost materials, which exhibit high activity and selectivity in catalysis. While various single-atom catalysts loaded on transition metal dichalcogenide (TMD) substrates with excellent CO2 reduction performance have been identified, the relationship between catalytic activity and the intrinsic properties of TMD single-atom catalysts remains unclear. Hence, a high-throughput first-principle computational approach is proposed to screen 24 transition metals anchored on 8 TMD monolayers to determine their catalytic activity in CO2RR. The results show that Fe@CoS2, Pt@TiTe2 and Co@CoS2 exhibit exceptional performances with low CO2RR limiting-potentials of −0.045 eV, 0.75 eV, and 0.54 eV, respectively, showcasing selective pathways towards formic acid (HCOOH), methane (CH4), and methanol (CH3OH). Employing the Sure Independence Screening and Sparsifying Operator method(SISSO), key descriptors linking the performance of single-atom catalysts with their intrinsic features are identified, providing insights for the discovery of superior CO2RR catalysts. Moreover, it was observed that a feature of the anchored single atom, the difference between covalent radius and atomic radius (CR-R), is associated with multiple crucial reaction steps, exhibiting a strong linear relationship with the charge transfer of *COOH. This work not only identifies promising CO2RR catalysts but also establishes a predictive framework for screening catalysts based on their intrinsic properties, paving the way for future advancements in CO2 reduction research.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.