System Theoretical Study on the Effect of Variable Nonmetallic Doping on Improving Catalytic Activity of 2D-Ti3C2O2 for Hydrogen Evolution Reaction

Abstract

2D MXenes have been found to be one of the most promising catalysts for hydrogen evolution reaction (HER) due to their excellent electronic conductivity, hydrophilic nature, porosity and stability. Nonmetallic (NM) element doping is an effective approach to enhance the HER catalytic performance. By using the density functional theory (DFT) method, we researched the effect of nonmetallic doping (different element types, variable doping concentrations) and optimal hydrogen absorption concentration on the surface of NM-Ti3C2O2 for HER catalytic activity and stability. The calculation results show that doping nonmetallic elements can improve their HER catalytic properties; the P element dopants catalyst especially exhibits remarkable HER performance (∆GH = 0.008 eV when the P element doping concentration is 100% and the hydrogen absorption is 75%). The origin mechanism of the regulation of doping on stability and catalytic activity was analyzed by electronic structures. The results of this work proved that by controlling the doping elements and their concentrations we can tune the catalytic activity, which will accelerate the further research of HER catalysts.

Single atom supported on MXenes for the alkaline hydrogen evolution reaction: species, coordination environment, and action mechanism

“…Two-dimensional (2D) MXenes, a large family of 2D layered materials with the general formula M n +1 X n T x (M: the transition metal element, X: the carbon/nitrogen element, and T: the surface termination groups, with n = 1, 2, or 3) have shown excellent mechanical and electronic properties because of their stable layered structure, tunable surface functional groups and large specific surface area. 9,10 MXenes display excellent catalytic activity for the HER due to the presence of T x surface functional groups, which can improve the interaction of hydrogen with MXenes, produce additional active sites, and increase the reaction area. 11,12 Ti-based MXenes, especially Ti 3 C 2 , are the most commonly used MXenes, but their application in the field of HER is limited by excessive overpotential.…”

“…Two-dimensional (2D) MXenes, a large family of 2D layered materials with the general formula M n+1 X n T x (M: the transition metal element, X: the carbon/nitrogen element, and T: the surface termination groups, with n = 1, 2, or 3) have shown excellent mechanical and electronic properties because of their stable layered structure, tunable surface functional groups and large specific surface area. 9,10 MXenes display excellent catalytic activity for the HER due to the presence of T x surface a Shanxi Key Laboratory of Compound Air Pollutions Identification and Control, College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, P. R. China. E-mail: lirui13233699182@163.com, yuexiuping@tyut.edu.cn; Fax: +86 351 6018554; Tel: +86 13233699182, +86 13068076599 b College of Chemical Engineering and Technology, Taiyuan University of functional groups, which can improve the interaction of hydrogen with MXenes, produce additional active sites, and increase the reaction area.…”

Exploring efficient hydrogen evolution electrocatalysts of nonmetal atom doped Mo2CO2 MXenes by first-principles screening

“…O, OH, or F, and n = 1-3. MXene has shown excellent catalytic, electronic and magnetic properties, and has a range of practical applications, such as electrocatalysis, [15][16][17] lithium-ion batteries, [18][19][20] electromagnetic shielding 21 and electronic devices. 22,23 In particular, for electrocatalytic hydrogen evolution, the high specific surface area, excellent electronic conductivity and adjustable surface termination of MXene materials make them a promising candidate for low-cost HER catalysts.…”

“…Besides, recent first-principles calculations show that non-metal (e.g., B, C, F and N) doping into the lattice of Ti 3 C 2 O 2 optimizes conductivity and improves the electrocatalytic HER activity of 2D MXenes. 16 Overall, non-metal (NM) surface doping into 2D MXenes can significantly modulate their electrocatalytic performance. The incorporation of non-metal dopants can not only create additional reaction sites and improve the conductivity, but also regulate the surface chemistry of catalysts, thereby influencing the catalytic activity, which provides an effective route to design highly efficient HER electrocatalysts.…”

“…, B, C, F and N) doping into the lattice of Ti 3 C 2 O 2 optimizes conductivity and improves the electrocatalytic HER activity of 2D MXenes. 16…”