Lei Jian, Wang Zhongliao, Huo Jinquan, Sang Shuaikang, Zhang Chao, Zhu Enquan, Kong Tingting, Karadas Ferdi, Low Jingxiang, Xiong Yujie
Anhui Engineering Research Center of Carbon Neutrality, The Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecular-Based Materials, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui, 241002, China.
Key Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Huaibei Normal University, Huaibei, Anhui, 235000, China.
Angew Chem Int Ed Engl. 2025 May 12;64(20):e202422667. doi: 10.1002/anie.202422667. Epub 2025 Mar 6.
Acetaldehyde (CHCHO) is of great industrial importance and serves as a key intermediate in various organic transformations. Photocatalytic production of acetaldehyde from CO represents a sustainable route compared to conventional oxidation processes. However, current photocatalytic systems often face challenges, including limited product selectivity and dependence on sacrificial reagents. Here, we present a CdZnS (CZS) photocatalyst co-modified with sulfur vacancies and atomically dispersed Cu (Cu/CZS-Vs) for the efficient conversion of CO to acetaldehyde. Charge density analysis reveals that sulfur vacancies induce charge accumulation around the adjacent metal atoms, creating active sites that strongly anchor CO and H, thereby promoting CO conversion while suppressing the competing hydrogen evolution reaction. The atomically dispersed Cu sites facilitate the conversion of key intermediates (i.e., *CHO and *CO) to the crucial C intermediate *OCCHO, which can subsequently be converted to acetaldehyde. As a result, this catalyst achieves an acetaldehyde yield of 121.5 μmol g h with a selectivity of ca. 80 % via photocatalytic CO conversion in the absence of sacrificial agents, along with a quantum efficiency of ca. 0.53 % at 400 nm, underscoring its potential for practical CO conversion applications. These results are expected to pave the way for future developments in green chemical processes.
