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Probing the mechanism of COR2R hydrogenation over Co and Fe single nanoparticles: Route to nanoparticle structural intimacy by Atom Probe Tomography


EMSL Project ID
51068

Abstract

Addressing the negative impact of COR2R on the global environment requires a multifaceted mitigation strategy which includes COR2R conversion to higher value compounds, satisfying both economic and environmental concerns [1]. COR2R conversion by catalytic hydrogenation, using hydrogen sourced from renewable sources of energy, appears as an ideal solution. Nanoparticle (NP) Co and Fe are promising materials for COR2R catalytic transformation into higher value long-chain hydrocarbons [2]. However, developing a catalyst material system with a practical efficiency of the reaction requires a deep understanding of the reaction steps on the catalyst nanoparticles down to the molecular level. More specifically, it is necessary to study the synergistic effect of the catalyst surface and subsurface structure with reactive gases to ultimately design effective and efficient catalytic systems. The Atom Probe equipped with a catalyst reactor system available at EMSL is a unique tool combination that allows one to image, at the molecular scale, the effect of reactive gases on the composition and structure of catalytic metal surfaces shaped as a sharp needle, the apex shape of which represents a model nanoparticle morphology. The hypothesis central to this proposal is that COR2R, CO and OR2R hydrogenation over Co or Fe will result in both surface AND subsurface structural changes to the catalyst, involving the formation of subsurface oxides. Our goals at EMSL is to use APT, STEM, XPS, and FTIR to study COR2R, CO and OR2R hydrogenation and resulting effects over Co and Fe. This work will also result in develop an innovative new technique to study surface chemistry by using APT and the catalyst reactor.

Project Details

Start Date
2019-10-01
End Date
2021-09-30
Status
Closed

Team

Principal Investigator

Daniel Perea
Institution
Environmental Molecular Sciences Laboratory

Team Members

Mark Wirth
Institution
Environmental Molecular Sciences Laboratory

Neeru Chaudhary
Institution
Washington State University

Sten Lambeets
Institution
Pacific Northwest National Laboratory

Alyssa Hensley
Institution
Washington State University

Jean-Sabin McEwen
Institution
Washington State University

Related Publications

Sten V. Lambeets, Thierry Visart de Bocarme, Daniel E. Perea and Norbert Kruse, Directional Gateway to Metal Oxidation: 3D Chemical Mapping Unfolds Oxygem Diffusional Pathways in Rhodium Nanoparticles, The Journal of Physical Chemistry Letters 2020, 11, 3144-3151 DOI:10.1021/acs.jpclett.0c00321
S.V. Lambeets, E. Kautz, M.G. Wirth, G.J.Orren, A. Deveraj and D.E.Perea, Nanoscale Perspectives of metal Degradation via in Situ Atom Probe Tomography, Topics in Catalysis (2020) 63:1606-1622 DOI:10.1007/s11244-020-01367-z