Huang Huining, Shi Run, Li Zhenhua, Zhao Jiaqi, Su Chenliang, Zhang Tierui
Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, 518060, China.
Angew Chem Int Ed Engl. 2022 Apr 19;61(17):e202200802. doi: 10.1002/anie.202200802. Epub 2022 Feb 28.
Photocatalytic CO reduction reaction (CO RR) is an attractive process to convert CO into valuable chemicals. But this reaction is often restricted by the poor mass transfer of CO in the liquid phase. Here, we have developed a triphase photocatalytic CO RR system by supporting Ag-decorated TiO nanoparticles at a gas-water boundary with hydrophobic-hydrophilic abrupt interfacial wettability. Such a triphase system allows the rapid delivery of gas-phase CO to the surface of photocatalysts while maintaining an efficient water supply and uncovered active sites. Ag-TiO supported at the gas-water boundary showed a CO reduction rate of 305.7 μmol g h , without hole scavengers, approximately 8 times higher than the nanoparticles dispersed in the liquid phase. Even using diluted CO (10 %) as the reactant, the CO RR activity was superior to most reported Ag-TiO based photocatalysts using pure CO . The findings provide a general strategy to promote the interfacial CO mass transfer to improve photoactivity and selectivity.
光催化CO还原反应(CO RR)是将CO转化为有价值化学品的一个有吸引力的过程。但该反应常常受到CO在液相中传质较差的限制。在此,我们通过在具有疏水 - 亲水突变界面润湿性的气 - 水边界负载Ag修饰的TiO纳米颗粒,开发了一种三相光催化CO RR系统。这样的三相系统能够使气相CO快速输送至光催化剂表面,同时保持高效的水供应和未覆盖的活性位点。负载在气 - 水边界的Ag - TiO显示出305.7 μmol g h的CO还原速率,在没有空穴清除剂的情况下,大约比分散在液相中的纳米颗粒高8倍。即使使用稀释的CO(10 %)作为反应物,CO RR活性也优于大多数报道的使用纯CO的基于Ag - TiO的光催化剂。这些发现提供了一种促进界面CO传质以提高光活性和选择性的通用策略。