Formation of hydrided Pt-Ce-H sites in efficient, selective oxidation catalysts

• 成果类型: Article
• 署名作者: Yang, Ji; Falling, Lorenz J.; Yan, Siyang; Zhang, Biluan; Verma, Pragya; Daemen, Luke; Cheng, Yongqiang; Zhao, Xiao; Zhang, Shuchen; Chen, Jeng-Lung; Yao, Bingqing; Tan, Shengdong; Chae, Sudong; He, Qian; Nemsak, Slavomir; Wu, Zili; Prendergast, David; Guo, Yanbing; Liu, Jiaxu; Salmeron, Miquel; Su, Ji
• 署名单位: United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; Dalian University of Technology; State Key Laboratory Surfactant Fine Chemistry; Central China Normal University; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; United States Department of Energy (DOE); Oak Ridge National Laboratory; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; National Synchrotron Radiation Research Center; National University of Singapore; United States Department of Energy (DOE); Oak Ridge National Laboratory
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-11953
• DOI: 10.1126/science.adv0735
• 发表日期: 2025-05-01
• 页码: 514-519
• 关键词: temperature co oxidation; contact quantification model; metal-support interactions; total-energy calculations; platinum single atoms; cu-zno synergy; methanol synthesis; electronic-structure; oxide supports; gold

摘要

Single-atom site catalysts can improve the rates and selectivity of many catalytic reactions. We have modified Pt1/CeO2 single sites by combining them with molecular groups and with oxygen vacancies of the support. The new sites include hydrided (Pt2+-Ce3+H delta-) and hydroxylated (Pt2+-Ce3+OH) sites that exhibit higher reactivity and selectivity to previous single sites for several reactions, including a ninefold increase in the reaction rate for carbon monoxide oxidation and a 2.3-fold improvement of propylene selectivity for oxidative dehydrogenation of propane. The atomic structure and reaction steps of these sites were determined with in situ and ex situ spectroscopy techniques and theoretical methods.