Atomic-Scale View of Redox Induced Changes for Monolayer MoOx on α-TiO2(110) with Chemical-State Sensitivity

Das, Anusheela; Jones, Leighton O.; Chen, Yanna; Choudhury, Devika; Keane, Denis T.; Elam, Jeffrey W.; Schatz, George C.; Bedzyk, Michael J.

doi:10.1021/acs.jpclett.2c01267

Atomic-Scale View of Redox Induced Changes for Monolayer MoO_x on α-TiO₂(110) with Chemical-State Sensitivity

Journal Article · Wed Jun 08 00:00:00 EDT 2022 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.2c01267· OSTI ID:1910050

Das, Anusheela ^[1]; ^[1]; ^[1]; Choudhury, Devika ^[2]; Keane, Denis T. ^[1]; ^[2]; ^[1]; ^[1]

Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Supported molybdenum oxide (MoO_x) plays an important role in catalytic transformations from alcohol dehydrogenation to transesterification. During these reactions, Mo and oxygen surface species undergo structural and chemical changes. A detailed, chemical-state specific, atomic-scale structural analysis of the catalyst under redox conditions is important for improving catalytic properties. In this study, monolayer of MoO_x grown on α-TiO₂(110) by atomic-layer deposition is analyzed by X-ray standing wave (XSW) excited X-ray photoelectron spectroscopy (XPS). The chemical shifts for Mo 2p_3/2 and O 1s peaks are used to distinguish Mo⁶⁺ from Mo⁴⁺ and surface O from bulk O. Excitation of XPS by XSW allows pin-pointing the location of these surface species relative to the underlying substrate lattice. Finally, measured 3D composite atomic density maps for the oxidized and reduced interfaces compare well with our density functional theory models, and collectively create a unique view of the redoxdriven dynamics for this complex catalytic structure.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern University, Evanston, IL (United States)

Sponsoring Organization:: NSF; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; FG02-03ER15457

OSTI ID:: 1910050

Alternate ID(s):: OSTI ID: 2481087

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 23 Vol. 13; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Atomic-Scale View of Redox Induced Changes for Monolayer MoOx on α-TiO2(110) with Chemical-State Sensitivity

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Atomic-Scale View of Redox Induced Changes for Monolayer MoO_x on α-TiO₂(110) with Chemical-State Sensitivity