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

Yang, Ji [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:000000023997385X); Falling, Lorenz J. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000226225166); Yan, Siyang [Dalian University of Technology (China)] (ORCID:000000025171990X); Zhang, Biluan [Central China Normal University, Wuhan (China)] (ORCID:0009000069780461); Verma, Pragya [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000257220894); Daemen, Luke [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)]; Cheng, Yongqiang [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000232634812); Zhao, Xiao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:000000031079664X); Zhang, Shuchen [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000185600045); Chen, Jeng-Lung [National Synchrotron Radiation Research Center, Hsinchu (Taiwan)] (ORCID:0000000202235538); Yao, Bingqing [National University of Singapore (Singapore)] (ORCID:000000027769021X); Tan, Shengdong [National University of Singapore (Singapore)] (ORCID:000900005305393X); Chae, Sudong [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]; He, Qian [National University of Singapore (Singapore)] (ORCID:0000000348913581); Nemsak, Slavomir [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000261032925); Wu, Zili [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000244683240); Prendergast, David [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000305981453); Guo, Yanbing [Central China Normal University, Wuhan (China)] (ORCID:0000000253991739); Liu, Jiaxu [Dalian University of Technology (China)] (ORCID:0000000308153979); Salmeron, Miquel [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0000000228878128); Su, Ji [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:000000032258162X)

doi:10.1126/science.adv0735

DOE OSTI · 2563159

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

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Abstract

Single-atom site catalysts can improve the rates and selectivity of many catalytic reactions. For this work, we have modified Pt 1 /CeO 2 single sites by combining them with molecular groups and with oxygen vacancies of the support. The new sites include hydrided (Pt 2+ -Ce 3+ Hδ) and hydroxylated (Pt 2+ -Ce 3+ 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 (CO) 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.

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Yang, Ji [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:000000023997385X), Falling, Lorenz J. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000226225166), Yan, Siyang [Dalian University of Technology (China)] (ORCID:000000025171990X), Zhang, Biluan [Central China Normal University, Wuhan (China)] (ORCID:0009000069780461), Verma, Pragya [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000257220894), Daemen, Luke [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)], Cheng, Yongqiang [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000232634812), Zhao, Xiao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:000000031079664X), Zhang, Shuchen [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000185600045), Chen, Jeng-Lung [National Synchrotron Radiation Research Center, Hsinchu (Taiwan)] (ORCID:0000000202235538), Yao, Bingqing [National University of Singapore (Singapore)] (ORCID:000000027769021X), Tan, Shengdong [National University of Singapore (Singapore)] (ORCID:000900005305393X), Chae, Sudong [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], He, Qian [National University of Singapore (Singapore)] (ORCID:0000000348913581), Nemsak, Slavomir [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000261032925), Wu, Zili [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000244683240), Prendergast, David [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000305981453), Guo, Yanbing [Central China Normal University, Wuhan (China)] (ORCID:0000000253991739), Liu, Jiaxu [Dalian University of Technology (China)] (ORCID:0000000308153979), Salmeron, Miquel [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0000000228878128), Su, Ji [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:000000032258162X). 2025-04-03. Formation of hydrided Pt-Ce-H sites in efficient, selective oxidation catalysts. https://doi.org/10.1126/science.adv0735

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