Theoretical screening of single-atom electrocatalysts of MXene-supported 3d-metals for efficient nitrogen reduction

Hu, Jin-Nian1; Tian, Ling -Chan1; Wang, Haiyan1; Meng, Yang1; Liang, Jin-Xia1; Zhu, Chun1,2,3; Li, Jun2,3,4

2023-09-01

10.1016/S1872-2067(23)64501-2

CHINESE JOURNAL OF CATALYSIS   影响因子和分区

0253-9837

1872-2067

Single-atom catalysts (SACs) with metal atoms embedded in MXenes are potentially low-cost, highly efficient, and environment-friendly electrocatalysts for ammonia production due to their high sta-bility, unique electronic structure, and the highest atom utilization. Here, density functional theory calculations are carried out to systematically investigate the geometries, stability, electronic proper-ties of SACs with the 3d-transition metal M (Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn) atoms embedded in the Ti defect sites of Ti2CO2 (denoted as M1@Ti2CO2). A highly stable V1@Ti2CO2 catalyst has been found to show excellent catalytic performance for N2 reduction reaction to produce NH3 after screening the 3d transition metals. The results show that V1@Ti2CO2 can not only strongly adsorb N2, but also exhibits an excellent Nitrogen reduction reaction (NRR) catalytic activity with a limiting potential of only -0.20 V and a high ability to suppress the competing hydrogen evolution reaction. The excellent NRR catalytic activity of V1@Ti2CO2 is attributed to the strong covalent metal-support interaction that leads to superb N2 adsorption ability of V atom. Furthermore, the embedded V sin-gle atoms facilitate electron transfer, thus improving the catalytic performance for NRR. These re-sults demonstrate that V1@Ti2CO2 is a potentially promising 2D material for building robust elec-trocatalyst for NRR.(c) 2023, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.

Single -atom catalyst Density functional theory N 2 reduction Defective Ti 2 CO 2 Electrocatalysis

SCI ; EI

英语

通讯

National Key RD Project["2022YFA1503900","2022YFA1503000"] ; National Natural Science Foundation of China["21963005","22033005"] ; Natural Science Special Foundation of Guizhou University[202140] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002]

Chemistry ; Engineering

Chemistry, Applied ; Chemistry, Physical ; Engineering, Chemical

WOS:001120002500001

ELSEVIER

20234214879509

Ammonia ; Atoms ; Catalyst activity ; Defects ; Electrocatalysis ; Electrocatalysts ; Electronic properties ; Electronic structure ; Nitrogen ; Transition metals

Metallurgy and Metallography:531 ; Electrochemistry:801.4.1 ; 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 ; Materials Science:951

CHEMISTRY

Web of Science

1.Guizhou Univ, Sch Chem & Chem Engn, Guiyang 550025, Guizhou, Peoples R China
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Guangdong Prov Key Lab Catalyt Chem, Shenzhen 518055, Guangdong, Peoples R China
4.Tsinghua Univ, Res Ctr Adv Rare Earth Mat, Minist Educ, Dept Chem & Engn, Beijing 100084, Peoples R China

Hu, Jin-Nian,Tian, Ling -Chan,Wang, Haiyan,et al. Theoretical screening of single-atom electrocatalysts of MXene-supported 3d-metals for efficient nitrogen reduction[J]. CHINESE JOURNAL OF CATALYSIS,2023,52:252-262.

Hu, Jin-Nian.,Tian, Ling -Chan.,Wang, Haiyan.,Meng, Yang.,Liang, Jin-Xia.,...&Li, Jun.(2023).Theoretical screening of single-atom electrocatalysts of MXene-supported 3d-metals for efficient nitrogen reduction.CHINESE JOURNAL OF CATALYSIS,52,252-262.

Hu, Jin-Nian,et al."Theoretical screening of single-atom electrocatalysts of MXene-supported 3d-metals for efficient nitrogen reduction".CHINESE JOURNAL OF CATALYSIS 52(2023):252-262.