Adsorption and activation of CO2 on Pt/CeOx/TiO2(110): Role of the Pt-CeOx interface

Grinter, David C.; Graciani, Jesús; Palomino, Robert M.; Xu, Fang; Waluyo, Iradwikanari; Sanz, Javier Fdez; Senanayake, Sanjaya D.; Rodriguez, José A.

doi:10.1016/j.susc.2021.121852

Title: Adsorption and activation of CO₂ on Pt/CeOx/TiO₂(110): Role of the Pt-CeO_x interface

Journal Article · Tue Apr 20 00:00:00 EDT 2021 · Surface Science

DOI:https://doi.org/10.1016/j.susc.2021.121852· OSTI ID:1778799

Grinter, David C. ^[1];

^[2];

^[3]; Xu, Fang ^[4]; Waluyo, Iradwikanari ^[5]; Sanz, Javier Fdez ^[2]; Senanayake, Sanjaya D. ^[3];

^[4]

Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Div.; Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.
Univ. of Sevilla (Spain). Dept. de Quimica Fisica
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Div.
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Div.; Univ. of Texas at San Antonio, TX (United States). Dept. of Chemistry
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

The adsorption and dissociation of CO₂ on TiO₂(110), CeO_x/TiO₂(110) and Pt/CeO_x/TiO₂(110) surfaces has been examined using Ambient Pressure X-ray Photoelectron Spectroscopy (AP-XPS). The substrates under study exhibited different degrees of complexity which were tested for the binding of the adsorbate and the cleavage of C-O bonds. The surfaces were prepared by depositing CeO_x (0.1 ML) onto TiO₂(110) to form a mixed oxide support, onto which Pt nanoparticles (0.2 ML) were deposited. This configuration yields a complex set of interfaces between metal and oxides and we have systematically titrated the active role of each component (Pt 4f, Ce 3d and Ti 2p regions) and the arising surface intermediates (C 1s and O 1s regions). CO₂ barely bonds to stoichiometric TiO₂(110). It heals oxygen vacancies of this oxide surface (CO_2,gas → CO_gas + O_a) and does not form stable carbonates. A stable carbonate was seen upon adsorption of CO₂ on CeO_x/TiO₂(110) and on this type of substrate the adsorbate also removed O vacancies leading to the oxidation of Ti³⁺and Ce³⁺ sites. Pt nanoparticles dispersed on CeO_x/TiO₂(110) were highly effective for the binding and dissociation of CO₂, with the formation of CO₃, CO, C and CH_x species on the Pt/CeO_x/TiO₂(110) system. The results of theoretical calculations based on density-functional theory (DFT) show that Pt/CeOx/TiO2(110) binds CO2 much stronger than surfaces of bulk platinum {(111), (100), (110)} or other late transition metals. On a Pt-CeO_x interface, the molecule adsorbs with a bent configuration (~ 130° O-C-O bond angle) and with a substantial elongation (~ 0.1 Å) of the C-O bonds, facilitating its transformation into high value chemicals.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC0012704

OSTI ID:: 1778799

Alternate ID(s):: OSTI ID: 1779323

Report Number(s):: BNL-221312-2021-JAAM

Journal Information:: Surface Science, Vol. 710; ISSN 0039-6028

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
Carbon dioxide
platinum
ceria
titania
ambient-pressure x-ray photoelectron spectroscopy
density functional calculations

Title: Adsorption and activation of CO2 on Pt/CeOx/TiO2(110): Role of the Pt-CeOx interface

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References (41)

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Title: Adsorption and activation of CO₂ on Pt/CeOx/TiO₂(110): Role of the Pt-CeO_x interface