Universität zu Köln

Nam, Hyunjun ORCID: 0000-0002-3816-2174, Sim, Eun Seob ORCID: 0000-0003-2674-1205, Je, Minyeong, Choi, Heechae ORCID: 0000-0002-9390-6607 and Chung, Yong-Chae ORCID: 0000-0002-7545-4934 (2021). Theoretical Approach toward Optimum Anion-Doping on MXene Catalysts for Hydrogen Evolution Reaction: an Ab Initio Thermodynamics Study. ACS Appl. Mater. Interfaces, 13 (31). S. 37035 - 37044. WASHINGTON: AMER CHEMICAL SOC. ISSN 1944-8252

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Abstract

Developing highly active catalysts for hydrogen evolution reaction based on earth-abundant materials is challenging. Nitrogen doping has recently been reported to improve catalytic properties by modifying the electrochemical properties of titanium carbide MXene. However, systematic doping engineering, such as optimization of doping concentration, doping site, and thermodynamic phase stabilization have not been systematically controlled, which retards the reliable production of high-activity MXene catalysts. In this study, the optimum doping concentration of nitrogen and doping process conditions on O-functionalized Ti2C MXene for hydrogen evolution reaction were investigated using density functional theory with thermodynamics. To confirm the optimum nitrogen concentration, the catalytic properties are examined considering the Gibbs free energy of hydrogen adsorption and conductivity for 2.2-11.0 at % nitrogen concentration. It was confirmed that 8.8 at % nitrogen-doped Ti2CO2 had optimum catalytic properties under standard conditions. Moreover, when the doping concentration was higher, the decrease in the adsorption energies of hydrogen and the transition in the energy dispersion of the conduction band led to deterioration of the catalytic properties. Through theoretical results, the feasible process conditions for optimum nitrogen concentration while maintaining the structure of MXene are presented using a thermodynamics model taking into account chemical reactions with various nitrogen sources. This study provides further understanding of the nitrogen-doping mechanism of Ti2CO2 for hydrogen evolution reactions.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Nam, Hyunjun UNSPECIFIED orcid.org/0000-0002-3816-2174 UNSPECIFIED Sim, Eun Seob UNSPECIFIED orcid.org/0000-0003-2674-1205 UNSPECIFIED Je, Minyeong UNSPECIFIED UNSPECIFIED UNSPECIFIED Choi, Heechae UNSPECIFIED orcid.org/0000-0002-9390-6607 UNSPECIFIED Chung, Yong-Chae UNSPECIFIED orcid.org/0000-0002-7545-4934 UNSPECIFIED
URN:	urn:nbn:de:hbz:38-570176
DOI:	10.1021/acsami.1c07476
Journal or Publication Title:	ACS Appl. Mater. Interfaces
Volume:	13
Number:	31
Page Range:	S. 37035 - 37044
Date:	2021
Publisher:	AMER CHEMICAL SOC
Place of Publication:	WASHINGTON
ISSN:	1944-8252
Language:	English
Faculty:	Unspecified
Divisions:	Unspecified
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language TITANIUM CARBIDE MXENE; ELECTROCATALYTIC ACTIVITY; CARRIER MOBILITY; MONOLAYER TI2CO2; TI3C2TX MXENE; EFFICIENT; HAMILTON; ELECTROCHEMISTRY; ADSORPTION; OXIDATION Multiple languages Nanoscience & Nanotechnology; Materials Science, Multidisciplinary Multiple languages
URI:	http://kups.ub.uni-koeln.de/id/eprint/57017