Selectivity of CO_(2)reduction reaction to CO on the graphitic edge active sites of Fe-single-atom and dual-atom catalysts:A combined DFT and microkinetic modeling  

作　　者：Ahmad Nuruddin Adhitya Gandaryus Saputro Arifin Luthfi Maulana Febdian Rusydi Fiki Taufik Akbar Hadi Teguh Yudistira Hermawan Kresno Dipojono 

机构地区：[1]Advanced Functional Materials Research Group,Faculty of Industrial Technology,Institut Teknologi Bandung,Jl.Ganesha No.10,Bandung 40132,Indonesia [2]Research Center for Nanosciences and Nanotechnology,Institut Teknologi Bandung,Jl.Ganesha No.10,Bandung 40132,Indonesia [3]Research Center for Quantum Engineering Design,Department of Physics,Faculty of Science and Technology,Universitas Airlangga,Surabaya 60115,Indonesia [4]Theoretical High Energy Physics Research Division,Faculty of Mathematics and Natural Sciences,Institut Teknologi Bandung,Jl.Ganesha No.10,Bandung 40132,Indonesia [5]Mechanical Engineering Study Program,Institut Teknologi Sumatera(ITERA),South Lampung,Lampung,Indonesia [6]Department of Materials Science and Engineering,University of California,Berkeley,Berkeley,CA 94720,United States

出　　处：《Carbon Resources Conversion》2024年第1期21-31,共11页碳资源转化（英文）

基　　金：supported by the Ministry of Education,Culture,Research,and Technology of the Republic of Indonesia through the‘WCR 2022’program under contract number 007/E5/PG.02.00.PT/2022.

摘　　要：We study the carbon dioxide reduction reaction(CO_(2)RR)activity and selectivity of Fe single-atom catalyst(Fe-SAC)and Fe dual-atom catalyst(Fe-DAC)active sites at the interior of graphene and the edges of graphitic nanopore by using a combination of DFT calculations and microkinetic simulations.The trend of limiting potentials for CO_(2)RR to produce CO can be described by using either the adsorption energy of COOH,CO,or their combination.CO_(2)RR process with reasonable reaction rates can be achieved only on the active site configurations with weak tendencies toward CO poisoning.The efficiency of CO_(2)RR on a catalyst depends on its ability to suppress the parasitic hydrogen evolution reaction(HER),which is directly related to the behavior of H adsorption on the catalyst’s active site.We find that the edges of the graphitic nanopore can act as potential adsorption sites for an H atom,and in some cases,the edge site can bind the H atom much stronger than the main Fe site.The linear scaling between CO and H adsorptions is broken if this condition is met.This condition also allows some edge active site configurations to have their CO_(2)RR limiting potential lower than the HER process favoring CO production over H2 production.

关 键 词：CO_(2)RR FexNy active site Fe-SAC Fe-DAC Graphitic edges DFT Microkinetic 

分 类 号：O64[理学—物理化学]