Tailoring Oxygen Vacancies with Atomically Dispersed Cu Sites for Stable and Efficient Photothermal CO <sub>2</sub> Conversion
Xueying Wan, Yilin Zhao, Yifan Li, Jun Ma, Yadi Gu, Caiyi Liu, Yanhua Luo, Guang Yang, Yi Cui, Dong Liu, Yujie Xiong
Abstract
Abstract Photothermal catalysis under mild conditions represents a promising and sustainable approach for CO 2 conversion into high‐value chemicals, thereby enabling efficient carbon recycling. However, precise manipulation of active sites and their coordination environments at the atomic level to enhance catalyst performance still remains a challenge. Here, we present a single‐atom doping strategy for oxygen vacancy engineering to facilitate efficient CO 2 conversion. Specifically, an In 2 O 3 ‐based catalyst with abundant oxygen vacancies induced by homogeneously dispersed Cu single atoms is constructed, exhibiting a competent CO 2 reduction performance in photothermal reverse water‐gas shift reaction. The optimal Cu‐In 2 O 3 catalyst achieves a CO yield rate of 46.17 mol g Cu −1 h −1 with near‐unity selectivity (>99%) and demonstrates stability over 450 h under 3 W cm −2 full‐spectrum light illumination. Comprehensive spectroscopic characterization and computational simulations elucidate that the Cu single atoms synergistically interact with oxygen vacancies to promote H 2 dissociation and CO 2 activation under photoexcitation. This work provides insights into the design of photothermal catalysts, emphasizing the transformative potential of atomic‐site engineering for efficient CO 2 conversion and sustainable energy technologies.