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

doi:10.1021/acs.jpclett.2c00667

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

electron Microscopy and Microanalysis

Research output: Contribution to journal › Article › peer-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 language	English
Pages (from-to)	3896-3903
Number of pages	8
Journal	Journal of Physical Chemistry Letters
Volume	13
Issue number	17
DOIs	https://doi.org/10.1021/acs.jpclett.2c00667
State	Published - 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.

Funders	Funder number
National Science Foundation	1906014
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-FG02-04ER15513, DE-AC02-76SF00515
Lawrence Berkeley National Laboratory	DE-AC02-05CH11231
Chemical Sciences, Geosciences, and Biosciences Division	DE-SC0020320

Access to Document

10.1021/acs.jpclett.2c00667

Cite this

Chen, Y., Rana, R., Huang, Z., Vila, F. D., Sours, T., Perez-Aguilar, J. E., Zhao, X., Hong, J., Hoffman, A. S., Li, X., Shang, C., Blum, T., Zeng, J., Chi, M., Salmeron, M., Kronawitter, C. X., Bare, S. R., Kulkarni, A. R., & Gates, B. C. (2022). Atomically Dispersed Platinum in Surface and Subsurface Sites on MgO Have Contrasting Catalytic Properties for CO Oxidation. Journal of Physical Chemistry Letters, 13(17), 3896-3903. https://doi.org/10.1021/acs.jpclett.2c00667

@article{cad295514d19413ea9d96f944a7dcb35,

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

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.",

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

year = "2022",

month = may,

day = "5",

doi = "10.1021/acs.jpclett.2c00667",

language = "English",

volume = "13",

pages = "3896--3903",

journal = "Journal of Physical Chemistry Letters",

issn = "1948-7185",

publisher = "American Chemical Society",

number = "17",

}

Chen, Y, Rana, R, Huang, Z, Vila, FD, Sours, T, Perez-Aguilar, JE, Zhao, X, Hong, J, Hoffman, AS, Li, X, Shang, C, Blum, T, Zeng, J, Chi, M, Salmeron, M, Kronawitter, CX, Bare, SR, Kulkarni, AR & Gates, BC 2022, 'Atomically Dispersed Platinum in Surface and Subsurface Sites on MgO Have Contrasting Catalytic Properties for CO Oxidation', Journal of Physical Chemistry Letters, vol. 13, no. 17, pp. 3896-3903. https://doi.org/10.1021/acs.jpclett.2c00667

TY - JOUR

T1 - Atomically Dispersed Platinum in Surface and Subsurface Sites on MgO Have Contrasting Catalytic Properties for CO Oxidation

AU - Chen, Yizhen

AU - Rana, Rachita

AU - Huang, Zhennan

AU - Vila, Fernando D.

AU - Sours, Tyler

AU - Perez-Aguilar, Jorge E.

AU - Zhao, Xiao

AU - Hong, Jiyun

AU - Hoffman, Adam S.

AU - Li, Xu

AU - Shang, Chunyan

AU - Blum, Thomas

AU - Zeng, Jie

AU - Chi, Miaofang

AU - Salmeron, Miquel

AU - Kronawitter, Coleman X.

AU - Bare, Simon R.

AU - Kulkarni, Ambarish R.

AU - Gates, Bruce C.

PY - 2022/5/5

Y1 - 2022/5/5

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85129324448&partnerID=8YFLogxK

U2 - 10.1021/acs.jpclett.2c00667

DO - 10.1021/acs.jpclett.2c00667

M3 - Article

C2 - 35471032

AN - SCOPUS:85129324448

SN - 1948-7185

VL - 13

SP - 3896

EP - 3903

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

IS - 17

ER -

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

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this