Construction of Frustrated Lewis Pairs for Efficient Artificial Enzyme

Abstract Optimizing the binding sites of substrates for small molecules activation plays a crucial role in enzyme‐like catalysts design. Herein, the frustrated Lewis pairs (FLPs) are successfully constructed through boron (B) doping into CoO_x (CoBO_x) with abundant oxygen vacancies (O_v). The O_v optimizes the valence of active sites, creates a coordinatively unsaturated state, and elongates the distance of Lewis pairs. The electron‐deficient Lewis acid (LA) sites (Co) facilitate the adsorption and dissociation of O₂, and the electron‐rich Lewis base (LB) sites (O) draw the positively charged TMB closer to Co sites and shorten the reaction distance, which synergistically improve the oxidase (OXD)‐like activity. Besides, the increase of electron density induced by FLPs promotes the electrons transfer, intermediates stabilization, and decreases the energy barrier of the rate‐determining step in adsorption and dissociation of O₂. Significantly, in a proof‐of‐concept application of colorimetric biosensing platform, the as‐developed FLPs in CoBO_x demonstrate highly sensitive and selective detection capacity of dopamine (DA) targets. This work verifies the application possibility of activating small molecules through FLPs in enzyme‐like catalysis.