摘要
Electrochemical water splitting(EWS),a sustainable pathway for green hydrogen production,faces critical industrial chal-lenges:insuffi cient activity and stability at high current densities,reliance on scarce noble metals,and unresolved kinetic bottlenecks in proton-coupled electron transfer(PCET)dynamics.Natural metalloenzymes drive water splitting at excep-tionally low overpotentials via precisely coordinated proton-coupled electron transfer(PCET)pathways within their active sites,achieving effi ciencies approaching the theoretical thermodynamic potential of the reaction(1.23 V vs.RHE),thereby off ering transformative design principles for synthetic catalysts.This review begins by analyzing the structural motifs and catalytic mechanisms of natural metalloenzymes involved in the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),with a particular focus on their PCET-driven reaction dynamics.Subsequently,we summarize the inspir-ing strategies derived from the design of the natural enzyme active sites and their ligand environments,highlighting their relevance to HER and OER catalyst development.In conclusion,we advocate for a multiscale,nature-inspired catalyst design paradigm that integrates deep learning,high-throughput computation,and cutting-edge in situ characterization to systematically understand and optimize intrinsic activity(overpotential),stability,and reaction pathway(selectivity),thereby achieving synergistic design from atomic-scale active sites to macroscopic system architectures.These nature-inspired strategies could bridge the gap between enzymatic precision and industrial scalability,unlocking EWS technologies with enzyme-like effi ciency and durability.
基金
supported by the National Natural Science Foundation of China(No.51832003)
the National Key Research and Development Program of China(No.2021YFA0715700).
