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.