Aliovalent Doping of CeO2Improves the Stability of Atomically Dispersed Pt

Haodong Wang; Matthew Kottwitz; Ning Rui; Sanjaya D. Senanayake; Nebojsa Marinkovic; Yuanyuan Li; Ralph G. Nuzzo; Anatoly I. Frenkel

doi:10.1021/acsami.1c18330

Aliovalent Doping of CeO₂Improves the Stability of Atomically Dispersed Pt

Haodong Wang, Matthew Kottwitz, Ning Rui, Sanjaya D. Senanayake, Nebojsa Marinkovic, Yuanyuan Li, Ralph G. Nuzzo, Anatoly I. Frenkel

Research output: Contribution to journal › Article › peer-review

17 Scopus citations

Abstract

Atomically dispersed supported catalysts hold considerable promise as catalytic materials. The ability to employ and stabilize them against aggregation in complex process environments remains a key challenge to the elusive goal of 100% atom utilization in catalysis. Herein, using a Gd-doped ceria support for atomically dispersed surface Pt atoms, we establish how the combined effects of aliovalent doping and oxygen vacancy generation provide dynamic mechanisms that serve to enhance the stability of supported single-atom configurations. Using correlated, in situ X-ray absorption, photoelectron, and vibrational spectroscopy methods for the analysis of samples on the two types of support (with and without Gd doping), we establish that the Pt atoms are located proximal to Gd dopants, forming a speciation that serves to enhance the thermal stability of Pt atoms against aggregation.

Original language	English
Pages (from-to)	52736-52742
Number of pages	7
Journal	ACS Applied Materials and Interfaces
Volume	13
Issue number	44
DOIs	https://doi.org/10.1021/acsami.1c18330
State	Published - Nov 10 2021
Externally published	Yes

Funding

A.I.F. and R.G.N. acknowledge support of the U.S. DOE BES grant no. DE-SC0022199. DRIFTS measurements at Brookhaven National Laboratory were made possible due to the Program Development fund 21-017 to A.I.F. Work by S.D.S. and N.R. at Brookhaven National Laboratory was supported by the U.S. DOE BES under contract no. DE-SC0012704. S.D.S. was partially supported by a U.S. DOE Early Career Award. M.K. acknowledges the fellowship support from the Department of Chemistry at the University of Illinois. This research used beamline 7-BM (QAS) of the National Synchrotron Light Source II, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. Beamline operations were supported in part by the Synchrotron Catalysis Consortium (U.S. DOE, Office of Basic Energy Sciences, grant no. DE-SC0012335). We thank Drs. S. Ehrlich and L. Ma for help with the beamline measurements at the QAS beamline. We are grateful to Dr. I. Lubomirsky for discussion of properties of Gd-doped CeO and to Drs. A. Bruix and K. Neyman for discussion of theoretical models of Pt on the CeO support. 2 2

Keywords

aliovalent doping
catalysis
metal-support
single atom
vacancies

Access to Document

10.1021/acsami.1c18330

Cite this

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abstract = "Atomically dispersed supported catalysts hold considerable promise as catalytic materials. The ability to employ and stabilize them against aggregation in complex process environments remains a key challenge to the elusive goal of 100% atom utilization in catalysis. Herein, using a Gd-doped ceria support for atomically dispersed surface Pt atoms, we establish how the combined effects of aliovalent doping and oxygen vacancy generation provide dynamic mechanisms that serve to enhance the stability of supported single-atom configurations. Using correlated, in situ X-ray absorption, photoelectron, and vibrational spectroscopy methods for the analysis of samples on the two types of support (with and without Gd doping), we establish that the Pt atoms are located proximal to Gd dopants, forming a speciation that serves to enhance the thermal stability of Pt atoms against aggregation.",

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