Rational design of copper-based single-atom alloy catalysts for electrochemical CO2 reduction

Jiang, Jian-Chao1,2,3,4; Chen, Jun-Chi3,4; Zhao, Meng-die1,2; Yu, Qi1,2; Wang, Yang-Gang3,4; Li, Jun3,4,5,6

2022-06-01

10.1007/s12274-022-4476-2

Nano Research   影响因子和分区

1998-0124

1998-0000

Electrochemical CO2-reduction reaction (CO2RR) is a promising way to alleviate energy crisis and excessive carbon emission. The Cu-based electrocatalysts have been considered for CO2RR to generate hydrocarbons and alcohols. However, the application of Cu electrocatalysts has been restricted by a high onset potential for CO2RR and low selectivity. In this study, we have designed a series of Cu-based single-atom alloy catalysts (SAAs), denoted as TM1/Cu (111), by doping isolated 3d-transition metal (TM) atom onto the Cu (111) surface. We theoretically evaluated their stability and investigated the activity and selectivity toward CO2RR. Compared to the pure Cu catalyst, the majority TM1/Cu (111) catalysts are more favorable for hydrogenating CO2 and can efficiently avoid the hydrogen-evolution reaction due to the strong binding of carbonaceous intermediates. Based on the density functional theory calculations, instead of the HCOOH or CO products, the initial hydrogenation of CO2 on SAAs would form the *CO intermediate, which could be further hydrogenated to produce methane. In addition, we have identified the bond angle of adsorbed CO2* can describe the CO2 activation ability of TM1/Cu (111) and the binding energy of *OH can describe the CO2RR activity of TM1/Cu (111). We speculated that the V/Cu (111) can show the best activity and selectivity for CO2RR among all the 3d-TM-doped TM1/Cu (111). This work could provide a rational guide to the design of new type of single-atom catalysts for efficient CO2RR.

CO2 electrochemical reduction Cu single-atom alloy catalysts density functional theory

SCI ; EI

英语

ESI高被引

通讯

National Natural Science Foundation of China[92061109,22022504] ; Natural Science Basic Research Program of Shaanxi["2021JCW-20","S2020-JC-WT-0001"] ; Guangdong "Pearl River" Talent Plan[2019QN01L353] ; Higher Education Innovation Strong School Project of Guangdong Province of China[2020KTSCX122] ; Open Project Program of Fujian Key Laboratory of Functional Marine Sensing Materials[MJUKFFMSM202002] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied

WOS:000805729000005

TSINGHUA UNIV PRESS

20222312202749

Atoms ; Binding energy ; Catalyst selectivity ; Copper alloys ; Density functional theory ; Electrocatalysts ; Electrolytic reduction ; Energy policy ; Hydrogenation ; Reaction intermediates ; Transition metals

Energy Policy:525.6 ; Metallurgy and Metallography:531 ; Ore Treatment:533.1 ; Copper Alloys:544.2 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

Web of Science

1.Shaanxi Univ Technol, Sch Mat Sci & Engn, Hanzhong 723001, Peoples R China
2.Shaanxi Univ Technol, Shaanxi Lab Catalysis, Hanzhong 723001, Peoples R China
3.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
4.Southern Univ Sci & Technol, Guangdong Prov Key Lab Catalysis, Shenzhen 518055, Peoples R China
5.Tsinghua Univ, Minist Educ, Dept Chem, Beijing 100084, Peoples R China
6.Tsinghua Univ, Minist Educ, Key Lab Organ Optoelect & Mol Engn, Beijing 100084, Peoples R China

Jiang, Jian-Chao,Chen, Jun-Chi,Zhao, Meng-die,et al. Rational design of copper-based single-atom alloy catalysts for electrochemical CO2 reduction[J]. Nano Research,2022,15(8):7116-7123.

Jiang, Jian-Chao,Chen, Jun-Chi,Zhao, Meng-die,Yu, Qi,Wang, Yang-Gang,&Li, Jun.(2022).Rational design of copper-based single-atom alloy catalysts for electrochemical CO2 reduction.Nano Research,15(8),7116-7123.

Jiang, Jian-Chao,et al."Rational design of copper-based single-atom alloy catalysts for electrochemical CO2 reduction".Nano Research 15.8(2022):7116-7123.