Atomically dispersed Pt to boost adjacent frustrated Lewis pair for 2,6‐diamino‐3,5‐dinitropyridine hydrogenation

Achieving atomic‐level control over local environment of metal oxide to boost catalytic activity is challenging yet significant for heterogeneous hydrogenations. Herein, we propose anchoring atomically dispersed Pt species onto indium oxide using a precisely conditioned atomic layer deposition (ALD) technology to manipulate the local electronic properties of In2O3 toward enhanced hydrogenation of 2,6‐diamino‐3,5‐dinitropyridine (DADNP) to 2,3,5,6‐tetraaminopyridine (TAP). Experimental and theoretical studies unravel that the isolated Pt atoms localize the electron density surrounding them and thus activate the adjacent frustrated Lewis pair for hydrogen activation. In addition, the adsorption of DADNP is enhanced by such regulation, while that of TAP is suppressed on the Pt1‐In2O3 catalyst. The as‐synthesized Pt1‐In2O3 catalyst thus exhibits 91.7% of TAP selectivity at 100% conversion of DADNP, demonstrating remarkably improved catalytic performances as compared with the In2O3 catalyst for DADNP hydrogenation.