Interfacial Engineering on Hierarchical Zro2 Nanoframes Realizes Efficient Nanozyme Photocatalytic Co2 Reduction

Abstract

Designing and fabricating nanozymes with photoactivity for CO2 reduction poses a significant challenge. Here, a hierarchical ZFs-tpyNi heterojunction nanozyme, comprising a terpyridine-based Ni complex supported on ZrO2 nanoframes, has been created through an interfacial engineering strategy for efficient CO2 reduction under visible light. Due to its unique structural and compositional advantages, ZFs-tpyNi demonstrates superior photocatalytic CO2-to-CO conversion compared to its counterpart, achieving a CO yield of 18.2 µmol and a selectivity of 92.4% with a high apparent quantum efficiency of 0.96% in 3 hours. These special catalysts also show excellent stability, maintaining a robust nanoframe structure and repeated catalytic performance. Systematic investigations reveal that the ZFs-tpyNi heterostructures possess more catalytically active sites, enhanced CO2 activation, alternative band energy regulation, and accelerated separation and mobility of photoexcited charge carriers. This work aims to illuminate the role of nanozyme catalysts in sustainable energy production.

Keywords: Interfacial engineering, CO2 photoreduction, nanozyme, hierarchical heterostructure