A General Dual-Metal Nanocrystal Dissociation Strategy to Generate Robust High-Temperature-Stable Alumina-Supported Single-Atom Catalysts

Abstract

Designing new synthesis routes to fabricate highly thermally durable precious metal single-atom catalysts (SACs) is challenging in industrial applications. Herein, a general strategy is presented that starts from dual-metal nanocrystals (NCs), using bimetallic NCs as a facilitator to spontaneously convert a series of noble metals to single atoms on aluminum oxide. The metal single atoms are captured by cation defects in situ formed on the surface of the inverse spinel (AB2O4) structure, which process provides numerous anchoring sites, thus facilitating generation of the isolated metal atoms that contributes to the extraordinary thermodynamic stability. The Pd1/AlCo2O4–Al2O3 shows not only improved low-temperature activity but also unprecedented (hydro)­thermal stability for CO and propane oxidation under harsh aging conditions. Furthermore, our strategy exhibits a small scaling-up effect by the simple physical mixing of commercial metal oxide aggregates with Al2O3. The good regeneration between oxidative and reductive atmospheres of these ionic palladium species makes this catalyst system of potential interest for emissions control.

Regulating the Electronic Synergy of Asymmetric Atomic Fe Sites with Adjacent Defects for Boosting Activity and Durability toward Oxygen Reduction

“…[9,13,14] These SACs possess fascinating physicochemical properties such as distinctive atom configuration, maximum atom utilization efficiency, unsaturated coordination environment, and unique electronic properties. [15][16][17][18][19][20] The rational design of low-cost and high activity metal-based nitrogen-doped carbon (M─N─C, M═Fe, Co, Ni, Cu, Mn, etc.) materials as efficient electrocatalysts for metal-air batteries and fuel cells is one of the major fields.…”