物理化学学报2025，Vol.41Issue(6)：115-122,8.DOI:10.1016/j.actphy.2025.100067
设计热力学稳定的贵金属单原子光催化剂用于乙醇的高效非氧化转化形成高纯氢和增值产物乙醛
Designing thermodynamically stable noble metal single-atom photocatalysts for highly efficient non-oxidative conversion of ethanol into high-purity hydrogen and value-added acetaldehyde
摘要
Abstract
The intrinsic surface atomic configuration of photocatalyst without unstable or difficult-to-generate atomic vacancies often limits the formation of effective interaction between metal single atom(MSA)cocatalyst and photocatalyst,thus inhibiting the stability and performance improvement of single-atom photocatalysts.In this study,we present a convenient and cost-effective photochemical oxygen reduction reaction(ORR)mechanism to prepare thermodynamically stable noble metal single-atom cocatalysts on TiO2 photocatalyst under mild condition(only consuming water and oxygen at 101325 Pa and 25 China).The first-principles simulation firstly theoretically reveals that the intrinsic surface configuration of TiO2 can only produce unstable Pt―O2 structure.However,ORR occurring on TiO2 can not only provide one foreign oxygen to coordinate with Pt single atom(PtSA),but also induce one surface lattice oxygen to move toward PtSA,promoting the formation of one thermodynamically stable Pt―O4 species,demonstrated by the experimental synthesis of PtSA on TiO2 in oxygen atmosphere instead of inert atmosphere.The obtained stable PtSA-TiO2 photocatalysts exhibit a photocatalytic rate of 320.4 mmol·g-1·h-1 for the coproduction of high-purity hydrogen and value-added acetaldehyde with a selectivity of 99.65%,three-fold higher than the activity of Pt nanoparticles-loaded TiO2.This strategy is further extended to other noble metals,such as Rh and Pd.关键词
金属单原子/表面重构/热稳定性/光催化/氢气Key words
Metal single atom/Surface reconstruction/Thermal stability/Photocatalysis/Hydrogen分类
化学化工引用本文复制引用
周昱晨,刘焕敏,李红星,宋欣妤,唐永华,周鹏..设计热力学稳定的贵金属单原子光催化剂用于乙醇的高效非氧化转化形成高纯氢和增值产物乙醛[J].物理化学学报,2025,41(6):115-122,8.基金项目
The project was supported by the start-up support from Peking University Shenzhen Graduate School and the National Natural Science Foundation Excellent Young Scientist Project,PKUSZ,China.The authors would like to thank the calculation support from Shuguang Supercomputer Center.北京大学深圳研究生院启动基金和国家自然科学基金优秀青年科学家项目资助,同时感谢曙光超级计算机中心对本文计算的支持 （）
