Rational Design of MoS2 Electrocatalyst for pH-universal Hydrogen Evolution: Mechanisms, Kinetics and Optimization

Description

Developing effective, low-cost electrocatalysts for hydrogen evolution reaction (HER) is crucial to solving the bottleneck problem in hydrogen production for the implementation of hydrogen economy. Based on our recent research, molybdenum disulfide (MoS2) based catalysts can perform as promising non-precious-metal HER electrocatalysts in acidic environment. However, the MoS2 electrocatalysts generally exhibit poor performance under alkaline condition and show inferiority in pH-universal activity. The challenge in the present development is to design MoS2 catalysts with high hydrogen evolution catalytic performance under both acidic and alkaline conditions. In this project, we will conduct both computational modeling and experimental studies. As previous research has shown that the material microstructure can manipulate the electrocatalytic effect, the first step of our study aims to gain insightful knowledge on the HER kinetics of the intrinsic connection between the microstructure and electrocatalytic behaviors of MoS2. First-principle electronic structure calculation and kinetics simulation will be conducted to accomplish rational design of MoS2 based catalysts for efficient HER catalysis. In the experimental part, we will develop the synthesis method of MoS2 based catalysts with controllable growth direction, distribution of active sites and specific heterostructure through the regulation of growth process. MoS2 catalysts will be fabricated and characterized for the microstructure and electrocatalytic behaviors. The mechanisms of the effect of MoS2 microstructure on the HER process will be investigated by conducting HER dual-path kinetic simulation, in situ synchrotron radiation X-ray absorption spectroscopy and density functional theory calculation. Finally, we will conduct parametric optimization of MoS2 catalyst design for maximum pH-universal HER performance. This project will enable better understanding of the electrocatalytic hydrogen evolution mechanisms and subsequently provide a new strategy to develop effective microstructured electrocatalysts with controllable synthesis method for high HER kinetics.