Modulation of Hydrogen Evolution Reaction Performance of MXenes by Doped Transition Metals: Comprehensive Exploration...

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• MXenes possess unique properties suitable for catalytic applications.
• Transition metal (TM) doping can modulate MXene catalytic performance, particularly for the hydrogen evolution reaction (HER).
• The vast combinatorial space of potential dopants hinders rapid catalyst screening.

Purpose of the Study:

• To investigate the effect of transition metal doping on MXene properties for HER.
• To develop a predictive model for rapid screening of HER catalysts.
• To identify effective dopant atoms for enhancing MXene-based HER catalysis.

Main Methods:

• High-throughput calculations were performed on doped Ti3CNO2 and Zr2HfCNO2 structures.
• Analysis of local and electronic structure changes influenced by doping.
• Development and application of a multisite prediction model (R² = 0.97) for hydrogen adsorption Gibbs free energy (ΔG_H*).

Main Results:

• Specific TM dopants (Nb, Sc, Rh, W, Ti, V) significantly improved HER properties, achieving |ΔG_H*| < 0.2 eV for over 38 MXene structures.
• The multisite prediction model accurately predicted trends in hydrogen adsorption free energy.
• Doping with Nb, Sc, Rh, W, Ti, and V proved effective for enhancing catalytic ability.

Conclusions:

• Doped transition metals show significant potential for enhancing MXene performance in HER.
• Multisite prediction models are crucial for accelerating the discovery and development of efficient HER catalysts.
• This work provides a pathway for designing advanced MXene-based electrocatalysts.