{"title":"Selective CO2-to-HCOOH Electroreduction on Graphdiyne-Supported Bimetallic Single-Cluster Catalysts","authors":"Bin Chen, Ya-Fei Jiang, Hai Xiao, Jun Li","doi":"10.1021/acscatal.4c00858","DOIUrl":null,"url":null,"abstract":"The oxophilic elements may stabilize the O-intermediate in electrochemical CO<sub>2</sub> reduction reaction (eCO<sub>2</sub>RR), yet their applications for formic acid (HCOOH) production may be limited by the Sabatier principle. Here we explore the bimetallic M<sub>1</sub>Ti<sub>3</sub> (M = Ni, Pd, Pt, Cu, Ag, Au) single-cluster catalysts (SCCs) anchored on graphdiyne (GDY) for eCO<sub>2</sub>RR to produce HCOOH. First-principles calculations show that the M<sub>1</sub>Ti<sub>3</sub>/GDY SCCs prefer to activate and hydrogenate CO<sub>2</sub> to the *OCHO intermediate (*denotes the active site of the catalyst) due to the oxophilic Ti sites, while the M<sub>1</sub> site plays a key role in suppressing the adsorption of *H and tuning the adsorption of *OCHO and *HCOOH for the HCOOH production, which is attributed to the modulation of Ti–O bonding strength by the M<sub>1</sub> atom. We predict that the Au<sub>1</sub>Ti<sub>3</sub>/GDY SCC is an efficient electrocatalyst for the selective eCO<sub>2</sub>RR to produce HCOOH. The directions for further improvements for the selective eCO<sub>2</sub>RR to produce HCOOH are discussed.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":11.3000,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.4c00858","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 oxophilic elements may stabilize the O-intermediate in electrochemical CO2 reduction reaction (eCO2RR), yet their applications for formic acid (HCOOH) production may be limited by the Sabatier principle. Here we explore the bimetallic M1Ti3 (M = Ni, Pd, Pt, Cu, Ag, Au) single-cluster catalysts (SCCs) anchored on graphdiyne (GDY) for eCO2RR to produce HCOOH. First-principles calculations show that the M1Ti3/GDY SCCs prefer to activate and hydrogenate CO2 to the *OCHO intermediate (*denotes the active site of the catalyst) due to the oxophilic Ti sites, while the M1 site plays a key role in suppressing the adsorption of *H and tuning the adsorption of *OCHO and *HCOOH for the HCOOH production, which is attributed to the modulation of Ti–O bonding strength by the M1 atom. We predict that the Au1Ti3/GDY SCC is an efficient electrocatalyst for the selective eCO2RR to produce HCOOH. The directions for further improvements for the selective eCO2RR to produce HCOOH are discussed.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.