Isomolar high-entropy engineering and Ac-coordination regulated nanocubic hydroxystannate for synergistic adsorption-photocatalytic acetaldehyde abatement under anoxic conditions

Abstract

High-entropy materials have attracted increasing attention in many applications due to their unusual properties, yet little is known about the effects of cationic ratios and anionic ligands on their catalytic activity. Herein, a novel isomolar high-entropy and Ac-coordinated hydroxystannate nanocube (iHEOH-Ac) is fabricated using NaOH as precipitant and acetate anion as ligand in one step. The unique strategy simultaneously employing isomolar high-entropy engineering and Ac coordination in iHEOH-Ac synergistically facilitates the formation of oxygen vacancies and acid sites and significantly enhances optical absorption, charge separation and acetaldehyde activation, leading to the highest amount of ROS (•OH and •O2– and h+). The synergistic adsorption-photocatalytic performance of iHEOH-Ac in acetaldehyde abatement outperforms its net photocatalytic mode and other counterparts, with maximum removal ratio up to ∼ 100% under anoxic conditions and reversible deactivation of ∼ 10% over 360 min. This work not only sheds light on the enhancement mechanism on the acetaldehyde oxidation performance through isomolar high-entropy and Ac-coordinated strategy, but also successfully regulates the acetaldehyde oxidation pathways by the reaction mode and anionic coordination environment, providing a new route for the design of high-performance acetaldehyde oxidation photocatalysts under anoxic environments.