Wan Xueying, Zhao Yilin, Li Yifan, Ma Jun, Gu Yadi, Liu Caiyi, Luo Yan, Yang Guang, Cui Yi, Liu Dong, Xiong Yujie
School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026, China.
State Key Laboratory of Bioinspired Interfacial Materials Science, Sustainable Energy and Environmental Materials Innovation Center, School of Nano Science and Technology, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu, 215123, China.
Angew Chem Int Ed Engl. 2025 Jul 21;64(30):e202505244. doi: 10.1002/anie.202505244. Epub 2025 Apr 27.
Photothermal catalysis under mild conditions represents a promising and sustainable approach for CO 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 conversion. Specifically, an InO-based catalyst with abundant oxygen vacancies induced by homogeneously dispersed Cu single atoms is constructed, exhibiting a competent CO reduction performance in photothermal reverse water-gas shift reaction. The optimal Cu-InO catalyst achieves a CO yield rate of 46.17 mol g h with near-unity selectivity (>99%) and demonstrates stability over 450 h under 3 W cm full-spectrum light illumination. Comprehensive spectroscopic characterization and computational simulations elucidate that the Cu single atoms synergistically interact with oxygen vacancies to promote H dissociation and CO activation under photoexcitation. This work provides insights into the design of photothermal catalysts, emphasizing the transformative potential of atomic-site engineering for efficient CO conversion and sustainable energy technologies.
温和条件下的光热催化是一种将CO转化为高价值化学品的有前景且可持续的方法，从而实现高效的碳循环利用。然而，在原子水平上精确调控活性位点及其配位环境以提高催化剂性能仍然是一项挑战。在此，我们提出一种用于氧空位工程的单原子掺杂策略，以促进高效的CO转化。具体而言，构建了一种由均匀分散的Cu单原子诱导产生大量氧空位的InO基催化剂，该催化剂在光热逆水煤气变换反应中表现出良好的CO还原性能。最优的Cu-InO催化剂实现了46.17 mol g⁻¹ h⁻¹的CO产率，选择性接近100%（>99%），并在3 W cm⁻²全光谱光照下450 h内表现出稳定性。综合光谱表征和计算模拟表明，Cu单原子与氧空位协同相互作用，在光激发下促进H解离和CO活化。这项工作为光热催化剂的设计提供了见解，强调了原子位点工程在高效CO转化和可持续能源技术方面的变革潜力。
