Microwave-pulse assisted synthesis of tunable ternary-doped 2D molybdenum carbide for efficient hydrogen evolution

Abstract

Amidst the urgent demand for carbon-neutral strategies, electrocatalytic hydrogen evolution reaction (HER) has garnered significant attention as an efficient and environmentally friendly energy conversion pathway. Non-precious metal layered transition metal carbides, particularly various modified two-dimensional molybdenum carbides (2D Mo₂C), have emerged as promising HER catalysts due to their superior intrinsic catalytic activity. While common non-metal doping strategies have been widely employed to enhance the electronic configuration and bulk/interface activity, the mechanism of HER performance dependence on the doping-induced electronic configuration in 2D Mo₂C remains unclear, especially for more complex binary or ternary doping configurations. To address the issue of uncontrollable doping atom percentages in conventional methods, herein, we propose a strategy for rapidly synthesizing highly tunable non-metal multielement-doped 2D Mo₂C using microwave pulse-assisted synthesis. By designing doping configurations with similar atomic ratios, we delve into the impact mechanisms of various doping configurations on the HER performance of 2D Mo₂C, with phosphorus doping potentially exerting the most significant positive influence. Furthermore, leveraging the unique thermodynamic and kinetic advantages of microwaves, this approach efficiently prevents potential side reactions associated with multi-element doping, enabling the rapid and precise synthesis of binary and ternary-doped 2D Mo₂C. The synthesized ternary-doped 2D Mo₂C with the same doping atomic ratios (2D P,N,S-Mo₂C) exhibits outstanding HER performance. This method not only offers a novel approach for precisely designing non-metallic atomic doping configurations in 2D TMCs but also provides insights into the theoretical structure-activity mechanism for other carbides with unique structures.

Keywords

Microwave / 2D material / tunable / ternary-doped / hydrogen evolution

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