Atomic‐Level Design of Active Site on Two‐Dimensional MoS 2 toward Efficient Hydrogen Evolution: Experiment, Theory, and Artificial Intelligence Modelling

Abstract Atom‐economic catalysts open a new era of computationally driven atomistic design of catalysts. Rationally manipulating the structures of the catalyst with atomic‐level precision would definitely play a significant role in the future chemical industry. Of particular concern, there are growing research concentrating on MoS 2 as a typical representative of transition metal dichalcogenides for its great potential of diverse atomic‐level reactive sites for applications in catalysis for hydrogen evolution reaction. At present, the rational design of MoS 2 ‐based catalysts greatly depends on the comprehensive understanding of its structure–activity relationships of active sites that still lacks the systematic summary. In this regard, we dissected the internal relationships between diverse active‐site configurations of MoS 2 and the corresponding catalytic activity theoretically and experimentally to give impetus to the design of next‐generation high‐performance MoS 2 ‐based catalysts. The necessity of normalizing the existing activity evaluation methodology and developing more‐precise metrics is discussed. Moreover, the advancement of artificial intelligence as an effective tool for the research on physicochemical properties of catalysts as well as its important role in theoretical pre‐design has also been reviewed. Finally, we summarized the opportunities and challenges of the design of nanoscale catalysts with desired physicochemical properties by assembling atoms in a controllable way.