xploring the adsorption site coordination as a strategy to tune copper catalysts for CO2 electro-reductio

Author(s)

Verga, Lucas G. ^[1] ; Mendes, Paulo C. D. ^[1] ; Ocampo-Restrepo, Vivianne K. ^[1] ; Da Silva, Juarez L. F. ^[1]

Affiliation

^[1] Univ Sao Paulo, Sao Carlos Inst Chem, POB 780, BR-13560970 Sao Carlos, SP - Brazil

• Document type: Journal article
• Source: CATALYSIS SCIENCE & TECHNOLOGY; v. 12, n. 3, p. 869-879, FEB 7 2022.
• Web of Science Citations: 0

Abstract

The electrochemical reduction of CO2 is a promising technology to reach a carbon-neutral economy. However, among other challenges, the design of active and selective catalysts still limits such advances. Herein, we explored the atomistic engineering of the catalyst substrate as a strategy to tune Cu catalysts for CO2 reduction towards different C-1 products by using generalized coordination numbers, GCN, as a structural descriptor of catalytic properties. We observed bifurcations on reaction mechanisms and significant changes in the predicted onset potentials, U-onset, towards CO, HCOOH, and CH4 as a function of the GCN values of the adsorption sites. For each product, we observed volcano plots of U-onset as a function of GCN that indicate activity peaks. We also compared the evolution of U-onset for different products to show that, regardless of the small U-onset values for CH4 on low-coordination sites, such adsorption sites should be more selective towards CO. For Cu nanoparticles, the analysis showed that decreasing the nanoparticle size could lead to more active catalysts that should be highly selective towards CO, which qualitatively agrees with experimental results. (AU)

• FAPESP's process: 17/11631-2 - CINE: computational materials design based on atomistic simulations, meso-scale, multi-physics, and artificial intelligence for energy applications
• Grantee: Juarez Lopes Ferreira da Silva
• Support Opportunities: Research Grants - Research Centers in Engineering Program
• FAPESP's process: 18/21401-7 - Multi-User Equipment approved in grant 2017/11631-2: cluster computational de alto desempenho - ENIAC
• Grantee: Juarez Lopes Ferreira da Silva
• Support Opportunities: Multi-user Equipment Program
• FAPESP's process: 19/05561-7 - A Multiscale Framework Applied to the Investigation of CO2 Reduction on Metallic Nanoparticles: The Role of Size and Adsorbate Coverage Effects
• Grantee: Lucas Garcia Verga
• Support Opportunities: Scholarships in Brazil - Post-Doctoral
• FAPESP's process: 21/07129-5 - CO2 reduction on Cu-Au intermetallic surfaces: atomic ordering and adsorbate coverage effects
• Grantee: Lucas Garcia Verga
• Support Opportunities: Scholarships abroad - Research Internship - Post-doctor