期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 122, 期 51, 页码 29307-29318出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.8b09430
关键词
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资金
- Toyota Research Institute (TRI) through the SUNCAT Center for Interface Science and Catalysis
- National Science Foundation [ACI-1548562]
- Toyota Research Institute (TRI) through the National Science Foundation Graduate Research Fellowship Program (NSF GRFP)
Single-atom catalysts have recently emerged as promising low-cost alternatives to Pt for the oxygen reduction reaction (ORR). Given the unique properties that distinguish these systems from traditional transition-metal electrocatalysts, it is essential to benchmark and establish appropriate computational approaches to study these novel materials. Herein, we employ multiple levels of theory, including wave function methods, density functional theory (DFT), and classical simulations, to investigate Cu-modified covalent triazine framework catalysts (Cu/CTF). We consider three major aspects of treating this system computationally. First, we present a step-wise approach to predict the ORR mechanism and adsorbate coverages on Cu/CTF. We then benchmark various DFT methods to coupled-cluster theory with the domain-based local pair natural orbital approximation, which indicates that HSE06 and PBE0 hybrid functionals most accurately describe the adsorption energies of ORR adsorbates on Cu/CTF. We finally employ thermodynamic integration and other techniques to consider solvation effects, which play significant roles in predicting the energies of reaction intermediates and the overall ORR pathway. Our findings indicate that accurate descriptions of both the electronic structure and solvation are necessary to understand the ORR activity of Cu/CTF.
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