Abstract

Hydrogen evolution reaction (HER) plays a critical role in exploiting clean energy, but which remains a great challenge of low-cost catalysts and inadequate cognition about the spin-related catalytic activity. Distinguished from conventional microstructural strategy, this work suggests a super-exchange interaction between single-atom dimers (SADs) and metal clusters to increase the reactive activity in HER and simultaneously the ability of electron migration. Herein, a stronger electronic interaction is built between metallic clusters and satellite SADs because of unblocked electron transfer pathway and very short interacting distances. The introduced metallic clusters can optimise the adsorption ability of the reactants and weaken their bonding interaction as well, leading to a fast dissociation. As a result, both the Gibbs free energy and carrier transfer are optimised effectively. This work demonstrates a great potential of super-exchange interaction between multiphase metal structures for enhancing the HER performance in SADs.

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