Computational screening of single atoms anchored on defective Mo2CO2 MXene nanosheet as efficient electrocatalysts for the synthesis of ammonia

Wang, Shuo, Li, Lei, San Hui, Kwan, Bin, Feng, Zhou, Wei, Fan, Xi, Zalnezhad, E., Li, Jing and Hui, Kwun Nam (2021) Computational screening of single atoms anchored on defective Mo2CO2 MXene nanosheet as efficient electrocatalysts for the synthesis of ammonia. Advanced Engineering Materials. ISSN 1438-1656

[img] PDF (Accepted_Manuscript) - Accepted Version
Restricted to Repository staff only until 1 July 2022.

Download (1MB) | Request a copy

Abstract

The electrochemical nitrogen reduction reaction (NRR) over single-atom catalysts (SACs) anchored on Mo vacancies of Mo 2CO 2 MXene nanosheets under ambient conditions suffers from poor selectivity, low yield, and low Faradaic efficiency because of their sluggish kinetics and the competing hydrogen evolution reaction. Herein, density functional theory calculations are performed to improve the understanding of the selectivity and yielding of ammonia through NRR over various isolated SACs, that is, from Sc to Au, anchored on the Mo vacancy of the Mo 2CO 2 MXene nanosheet (denoted as MO 2CO 2-M SA). The potential-determining step of the NRR shows that eight candidates (i.e., Y, Zr, Nb, Hf, Ta, W, Re, and Os) confined on the defective Mo 2CO 2 layer could promote the electroreduction from N 2 to NH 3. Among these, Mo 2CO 2-Y SA presented the lowest reported reaction Presents the lowest reported reaction energy barrier (0.08 eV) through the distal pathway and high selectivity to NRR compared with the previously synthesized Mo 2CO 2-Ru SA with a relatively high energy barrier (0.65 eV) and poor selectivity. In addition, the formation energy of Mo 2CO 2-Y SA is more negative than that of the Mo 2CO 2-Ru SA catalyst, suggesting that the experimental preparation of the Mo 2CO 2-Y SA catalyst is highly feasible. This work lays a solid foundation for improving the rational design of MXene-based systems as efficient electrocatalysts for the synthesis of ammonia.

Item Type: Article
Uncontrolled Keywords: mxene,density functional theory calculations,electrocatalysis,nitrogen reduction reaction,single-atom catalysts,materials science(all),condensed matter physics ,/dk/atira/pure/subjectarea/asjc/2500
Faculty \ School:
Related URLs:
Depositing User: LivePure Connector
Date Deposited: 18 Aug 2021 11:40
Last Modified: 24 Aug 2021 00:18
URI: https://ueaeprints.uea.ac.uk/id/eprint/81137
DOI: 10.1002/adem.202100405

Actions (login required)

View Item View Item