Abstract
Single-atom catalysts (SACs) and single-cluster catalysts (SCCs) are the new frontier of heterogeneous catalysis, which exhibit high activity, selectivity, stability, and atomic efficiency as well as precise tunability. However, the lack of efficient methods for producing high-loading and high-purity SACs and SCCs hinders their industrial applications. In this work, we propose a general and efficient strategy for the production of high-loading and high-purity SACs and SCCs anchored on suitable substrates. Our strategy relies on the existence of an electrochemical potential window (EcPW) we predict within which any aggregate forms of the target metal on the substrate are leached away by electrochemical oxidation, while the strongly bound single atoms or single clusters remain at the substrate. We demonstrate the applicability of this strategy with modeling the production of Pt, Pd, and Ni SACs anchored on N-doped graphene and Fe2O3 as well as Pt3 and Ni3 SCCs anchored on graphdiyne.
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