Ultrastable nickel single-atom catalysts with high activity and selectivity for electrocatalytic CO2 methanation

Tian，Ling Chan1; Hu，Jin Nian1; Meng，Yang1; Liang，Jin Xia1; Zhu，Chun1,2; Li，Jun2,3

2023

10.1007/s12274-023-5640-z

Nano Research   影响因子和分区

1998-0124

1998-0000

Electrochemical conversion of CO into valuable hydrocarbon fuel is one of the key steps in solving carbon emission and energy issue. Herein, we report a non-noble metal catalyst, nickel single-atom catalyst (SAC) of Ni/UiO-66-NH, with high stability and selectivity for electrochemical reduction of CO to CH. Based on ab initio molecular dynamics (AIMD) simulations, the CO molecule is at first reduced into CO when stably adsorbed on a Ni single atom with the bidentate coordination mode. To evaluate its activity and selectivity for electrocatalytic reduction of CO to different products (HCOOH, CO, CHOH, and CH) on Ni/UiO-66-NH, we have used density functional theory (DFT) to study different reaction pathways. The results show that CH is generated preferentially on Ni/UiO-66-NH and the calculated limiting potential is as low as −0.24 V. Moreover, the competitive hydrogen evolution reaction is unfavorable at the activation site of Ni/UiO-66-NH owing to the higher limiting potential of −0.56 V. Furthermore, the change of Ni single atom valence state plays an important role in promoting CO reduction to CH. This work provides a theoretical foundation for further experimental studies and practical applications of metal-organic framework (UiO-66)-based SAC electrocatalysts with high activity and selectivity for the CO reduction reaction. [Figure not available: see fulltext.]

CO2 reduction density functional theory electrocatalysis metal–organic framework single atom catalyst

SCI ; EI

英语

通讯

National Key Research and Development Project["2022YFA1503900","2022YFA1503000"] ; National Natural Science Foundation of China["22033005","21963005"] ; Natural Science Special Foundation of Guizhou University[202140] ; 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:000979902800001

TSINGHUA UNIV PRESS

20231814026730

Atoms ; Carbon dioxide ; Catalyst activity ; Catalyst selectivity ; Electrocatalysis ; Electrocatalysts ; Electrolytic reduction ; Molecular dynamics ; Nickel ; Organometallics ; Precious metals ; Reaction kinetics

Ore Treatment:533.1 ; Precious Metals:547.1 ; Nickel:548.1 ; Physical Chemistry:801.4 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

2-s2.0-85153788182

Scopus

1.School of Chemistry and Chemical Engineering,Guizhou University,Guiyang,550025,China
2.Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry,Southern University of Science and Technology,Shenzhen,518055,China
3.Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education,Tsinghua University,Beijing,100084,China

Tian，Ling Chan,Hu，Jin Nian,Meng，Yang,et al. Ultrastable nickel single-atom catalysts with high activity and selectivity for electrocatalytic CO2 methanation[J]. Nano Research,2023,16(7):8987-8995.

Tian，Ling Chan,Hu，Jin Nian,Meng，Yang,Liang，Jin Xia,Zhu，Chun,&Li，Jun.(2023).Ultrastable nickel single-atom catalysts with high activity and selectivity for electrocatalytic CO2 methanation.Nano Research,16(7),8987-8995.

Tian，Ling Chan,et al."Ultrastable nickel single-atom catalysts with high activity and selectivity for electrocatalytic CO2 methanation".Nano Research 16.7(2023):8987-8995.