Atomically Dispersed Platinum in Surface and Subsurface Sites on MgO Have Contrasting Catalytic Properties for CO Oxidation

Yizhen Chen, Rachita Rana, Zhennan Huang, Fernando D. Vila, Tyler Sours, Jorge E. Perez-Aguilar, Xiao Zhao, Jiyun Hong, Adam S. Hoffman, Xu Li, Chunyan Shang, Thomas Blum, Jie Zeng, Miaofang Chi, Miquel Salmeron, Coleman X. Kronawitter, Simon R. Bare, Ambarish R. Kulkarni, Bruce C. Gates

Research output: Contribution to journalArticlepeer-review

12 Scopus citations

Abstract

Atomically dispersed metals on metal oxide supports are a rapidly growing class of catalysts. Developing an understanding of where and how the metals are bonded to the supports is challenging because support surfaces are heterogeneous, and most reports lack a detailed consideration of these points. Herein, we report two atomically dispersed CO oxidation catalysts having markedly different metal-support interactions: platinum in the first layer of crystalline MgO powder and platinum in the second layer of this support. Structural models have been determined on the basis of data and computations, including those determined by extended X-ray absorption fine structure and X-ray absorption near edge structure spectroscopies, infrared spectroscopy of adsorbed CO, and scanning transmission electron microscopy. The data demonstrate the transformation of surface to subsurface platinum as the temperature of sample calcination increased. Catalyst performance data demonstrate the lower activity but greater stability of the subsurface platinum than of the surface platinum.

Original languageEnglish
Pages (from-to)3896-3903
Number of pages8
JournalJournal of Physical Chemistry Letters
Volume13
Issue number17
DOIs
StatePublished - May 5 2022

Funding

Y.C. and B.C.G. were supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) grant DE-FG02-04ER15513. Stanford Synchrotron Radiation Lightsource (SSRL) of SLAC National Accelerator Laboratory is supported by BES under Contract No. DE-AC02-76SF00515. Co-ACCESS is supported by the BES Chemical Sciences, Geosciences, and Biosciences Division. C.X.K. and A.R.K. were supported by the DOE, Office of Science, BES grant DE-SC0020320. R.R. acknowledges support from the DOE (DE-SC0020320, for DFT calculations) and from Co-ACCESS. Z.H. was supported by the DOE BES, Chemical Sciences, Geosciences, and Biosciences Division. Electron microscopy was performed at the Oak Ridge National Laboratory Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility (T.B., M.C.). T.S. acknowledges support from the DOE (DE-SC0020320). X.Z and M.S were supported by the National Science Foundation grant number 1906014. The DFT and HERFD-XANES calculations were performed using the resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231. XPS characterizations were performed at the Molecular Foundry supported by the DOE under Contract No. DE-AC02-05CH11231. The authors acknowledge Noah W. Felvey for help in the experiments.

FundersFunder number
National Science Foundation1906014
U.S. Department of Energy
Office of Science
Basic Energy SciencesDE-FG02-04ER15513, DE-AC02-76SF00515
Lawrence Berkeley National LaboratoryDE-AC02-05CH11231
Chemical Sciences, Geosciences, and Biosciences DivisionDE-SC0020320

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