Liu Xingbing, Zhu Changyan, Li Mengying, Xing Hongzhu, Zhu Siyang, Liu Xin, Zhu Guangshan
College of Chemistry, Northeast Normal University, 130021, Changchun, China.
Angew Chem Int Ed Engl. 2024 Nov 4;63(45):e202412408. doi: 10.1002/anie.202412408. Epub 2024 Sep 13.
Photocatalytic CO reduction to value-added fuels displays an attractive scenario to enhance energy supply and reduce global warming. We report herein the confinement synthesis of polymeric carbon nitride (PCN) incorporating with Cu single atoms (CuSAs) inside the crystalline UiO-66-NH, which combines the merits of heterojunction photocatalysis and single-atom catalysis (SAC) to achieve high-performance CO-to-CHOH conversion. A series of spectral studies displays the formation of CuSAs@PCN inside the crystalline UiO-66-NH. Remarkably, the ternary composite shows an excellent photocatalytic turnover frequency of 4.15 mmol ⋅ h ⋅ g for CO-to-CHOH conversion. Theoretical and experimental studies demonstrate the doping of CuSAs, as well as the formation of type-II heterojunction, are causal factors to achieve CHOH generation. The study provides new insights designing high-performance photocatalyst for CO conversion to fuels at atomic scale.
光催化将CO还原为增值燃料为增强能源供应和减少全球变暖展现了一个诱人的前景。我们在此报告了在晶体UiO-66-NH内部限域合成掺入铜单原子（CuSAs）的聚合氮化碳（PCN），它结合了异质结光催化和单原子催化（SAC）的优点，以实现高性能的CO到CHOH的转化。一系列光谱研究表明在晶体UiO-66-NH内部形成了CuSAs@PCN。值得注意的是，这种三元复合材料对于CO到CHOH的转化显示出4.15 mmol ⋅ h ⋅ g的优异光催化周转频率。理论和实验研究表明，CuSAs的掺杂以及II型异质结的形成是实现CHOH生成的成因。该研究为在原子尺度设计用于将CO转化为燃料的高性能光催化剂提供了新的见解。
