Surface oxygenation of multicomponent nanoparticles toward active and stable oxidation catalysts

Shan, Shiyao; Li, Jing; Maswadeh, Yazan; O’Brien, Casey; Kareem, Haval; Tran, Dat T.; Lee, Ivan C.; Wu, Zhi-Peng; Wang, Shan; Yan, Shan; Cronk, Hannah; Mott, Derrick; Yang, Lefu; Luo, Jin; Petkov, Valeri; Zhong, Chuan-Jian

doi:10.1038/s41467-020-18017-3

Surface oxygenation of multicomponent nanoparticles toward active and stable oxidation catalysts

Journal Article · Fri Aug 21 00:00:00 EDT 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-18017-3· OSTI ID:1648581

; Li, Jing; Maswadeh, Yazan; O’Brien, Casey; Kareem, Haval; ; Lee, Ivan C.; Wu, Zhi-Peng; ; Yan, Shan; Cronk, Hannah; Mott, Derrick; Yang, Lefu; ; ;

Abstract

The need for active and stable oxidation catalysts is driven by the demands in production of valuable chemicals, remediation of hydrocarbon pollutants and energy sustainability. Traditional approaches focus on oxygen-activating oxides as support which provides the oxygen activation at the catalyst-support peripheral interface. Here we report a new approach to oxidation catalysts for total oxidation of hydrocarbons (e.g., propane) by surface oxygenation of platinum (Pt)-alloyed multicomponent nanoparticles (e.g., platinum-nickel cobalt (Pt–NiCo)). The in-situ/operando time-resolved studies, including high-energy synchrotron X-ray diffraction and diffuse reflectance infrared Fourier transform spectroscopy, demonstrate the formation of oxygenated Pt–NiOCoO surface layer and disordered ternary alloy core. The results reveal largely-irregular oscillatory kinetics associated with the dynamic lattice expansion/shrinking, ordering/disordering, and formation of surface-oxygenated sites and intermediates. The catalytic synergy is responsible for reduction of the oxidation temperature by ~100 °C and the high stability under 800 °C hydrothermal aging in comparison with Pt, and may represent a paradigm shift in the design of self-supported catalysts.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Science Foundation (NSF); US Army Research Laboratory (USARL); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0006877

OSTI ID:: 1648581

Alternate ID(s):: OSTI ID: 1651149

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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