Surface Modifications of 2D-Ti3C2O2 by Nonmetal Doping for Obtaining High Hydrogen Evolution Reaction Activity: A Computational Approach

Fangtao Li,Xiaoxu Wang,Rongming Wang

doi:10.3390/catal11020161

Abstract

As a typical two-dimensional (2D) MXene, Ti3C2O2 has been considered as a potential material for high-performance hydrogen evolution reaction (HER) catalyst, due to its anticorrosion and hydrophilic surface. However, it is still a challenge to improve the Ti3C2O2 surficial HER catalytic activity. In this work, we investigated the HER activity of Ti3C2O2 after the surface was doped with S, Se, and Te by the first principles method. The results indicated that the HER activity of Ti3C2O2 is improved after being doped with S, Se, Te because the Gibbs free energy of hydrogen adsorption (ΔGH) is increased from −2.19 eV to 0.08 eV. Furthermore, we also found that the ΔGH of Ti3C2O2 increased from 0.182 eV to 0.08 eV with the doping concentration varied from 5.5% to 16.7%. The HER catalytic activity improvement of Ti3C2O2 is attributed to the local crystal structure distortion in catalytic active sites and Fermi level shift leads to the p-d orbital hybridization. Our results pave a new avenue for preparing a low-cost and high performance HER catalyst.

Highlights

IntroductionEnvironmental pollution and the energy crisis are two tough issues in human development
Catalysts 2021, 11, 161. https://Environmental pollution and the energy crisis are two tough issues in human development
It of Ti changing the electronic total density of states analysis (TDOS), and is shown that nonmetal doping caused the hybridization between p-orbitals of Te and dleading to the Fermi level increasing from −2.043 eV to −1.522 eV, and weakening the orbitals of Ti, which led to the rearrangement structures near density the Fermi obtained electrons ability of Ti27 C18of

Summary

Introduction

Environmental pollution and the energy crisis are two tough issues in human development. Previous theoretical studies have shown that element loading or doping at the transition metal surface can effectively improve the catalytic activity, but these results need to be further verified by actual experiments [4,5,6]. Catalysts 2021, 11, 161 improve the catalytic activity, but these results need to be further verified by actual exper of 9 iments [4,5,6]. The results indiIn this carefully studied the ∆GH of 2D-Ti. 3C2O2 is effectively improved after being beingdoped dopedwith withS,Te. Te on the surface by first principles density functional theory (DFT). The improvement of HER is ascribed theexperimental local crystal orbital which provides ancatalytic effectiveactivity theoretical modeltofor structure distortion of catalytic active site and Fermi level shift leading to the p-d orbital preparation. Hybridization, which provides an effective theoretical model for experimental preparation

Results and Discussion

Hydrogen atoms were adsorbedononthe theoxygen oxygenatoms’

Computational

Conclusions