High‐Density Frustrated Lewis Pair for High‐Performance Hydrogen Evolution

Abstract It is significant to develop catalysts with high‐density and adjacent frustrated Lewis pair (FLP) sites. Herein, a method is designed to construct FLPs on an intermetallic alloy (IMA) with regulable acidity and basicity by using the Mott–Schottky effect. By dint of the high‐density FLP site and suitable acidity and basicity on IMA, the fct‐PtCo@NC displays excellent hydrogen evolution reaction performance. The catalyst fct‐PtCo@NC, with high‐density FLP sites, exhibits a fast water adsorption and decomposition rate, which is derived from the synergistic effect of FLP‐acid sites and FLP‐base sites significantly reducing the energy barrier between the two processes. Due to the FLP‐base Pt site, fct‐PtCo@NC has the best binding energy of hydrogen intermediates, the H 3 O + generated during the reaction can accumulate on it and form an acid‐like environment, and thus speed up the kinetics of the reaction. In comparison, the catalyst without FLP shows lower binding energy and the formation of H 3 O + is not observed. This work opens a new horizon for the design of new‐style heterogeneous FLP catalysts and the catalysts with high‐density and adjacent FLP sites are expected to be used in a variety of multistep catalytic reactions.