Wei Zhidong, Zhang Yuchen, Huang Huoshuai, Liu Junying, Zhang Yiran, Li Xinling, Shangguan Wenfeng, Huang Zhen
College of Smart Energy, Shanghai Jiao Tong University, Shanghai 200240, People's Republic of China.
Research Center for Combustion and Environmental Technology, Shanghai Jiao Tong University, Shanghai 200240, People's Republic of China.
Inorg Chem. 2025 Jun 23;64(24):12277-12285. doi: 10.1021/acs.inorgchem.5c01686. Epub 2025 Jun 11.
In this context, a AlO doped SrTiO (Al:SrTiO) was synthesized via the molten salt method. The spatial separation active sites of the hydrogen evolution and the CO reduction in photocatalysis were revealed by using absorbed H as a probe, which indicated that CoOOH could be the photocatalytic CO reduction active site while RhCrO could serve as the main site for hydrogen species activation and generation. The photocatalytic CO reduction could be determined by the spatial-temporal transfer of active hydrogen species coupled with carriers, from the interface of RhCrO-Al:SrTiO to CoOOH-Al:SrTiO probably. More importantly, the competitive relationship between liquid water molecules, active hydrogen species, and CO was proved, indicating that the water film may hinder the spatial-scale migration of active hydrogen species and CO absorption. This work explored photocatalytic CO reduction from overall water splitting systems and emphasized the importance of the spatial shielding effect of interfacial water molecules.
在此背景下，通过熔盐法合成了AlO掺杂的SrTiO（Al:SrTiO）。以吸附的H为探针揭示了光催化析氢和CO还原的空间分离活性位点，这表明CoOOH可能是光催化CO还原活性位点，而RhCrO可作为氢物种活化和产生的主要位点。光催化CO还原可能由活性氢物种与载流子的时空转移决定，可能是从RhCrO-Al:SrTiO界面到CoOOH-Al:SrTiO。更重要的是，证明了液态水分子、活性氢物种和CO之间的竞争关系，表明水膜可能阻碍活性氢物种的空间尺度迁移和CO吸收。这项工作探索了全水分解系统中的光催化CO还原，并强调了界面水分子空间屏蔽效应的重要性。
