The Surface Chemistry of Methanol on TiO2(110): Effects of Pressure and Temperature on the Stability of C–O and C–H Bonds

Reddy, Kasala Prabhakar; Islam, Arephin; Barba-Nieto, Irene; Hunt, Adrian; Waluyo, Iradwikanari; Rodriguez, José Antonio

doi:10.1021/acs.jpcc.5c04763

Title: The Surface Chemistry of Methanol on TiO₂(110): Effects of Pressure and Temperature on the Stability of C–O and C–H Bonds

Journal Article · Wed Aug 20 00:00:00 UTC 2025 · The Journal of Physical Chemistry C

DOI: https://doi.org/10.1021/acs.jpcc.5c04763 · OSTI ID:2587792

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Brookhaven National Laboratory (BNL), Upton, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Synchrotron-based ambient pressure X-ray photoelectron spectroscopy (AP-XPS) was used to study the surface chemistry of methanol on TiO₂(110), examining the effects of methanol pressure, oxide temperature, and coadsorption with H₂. At 300 K, the adsorption of methanol on TiO₂(110) leads to the formation of CH₃O on the surface with a minor amount of CH₃OH present. The easy cleavage of the O–H bond in the alcohol agrees with the predictions of theoretical calculations, and most of the adsorbed CH₃O was not associated with the presence of Ti³⁺ sites in the oxide substrate. The adsorbed CH₃O was removed from the TiO₂(110) surface by heating to 600 K without the deposition of CH_x fragments or C on the oxide. The results of temperature-programmed desorption (TPD) showed the evolution of methanol and formaldehyde at 360 and 490 K as a result of a disproportionation reaction: 2CH₃O → CH₃OH + CH₂O. This surface chemistry, where there is no rupture of the C–O bond, and only selective cleavage of O–H and C–H bonds, is very different from that found on metals used in catalysts for methanol reforming, where massive conversion of the alcohol into CO, CH_x and C species is seen. Furthermore, the TPD data indicate that any CH₃O formed on the oxide surface can be hydrogenated and desorbed as CH₃OH at temperatures below 550 K. In this respect, titania is an ideal support for catalysts employed to achieve methanol synthesis through CO₂ hydrogenation.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2587792

Report Number(s):: BNL--228875-2025-JAAM

Journal Information:: The Journal of Physical Chemistry C, Journal Name: The Journal of Physical Chemistry C Journal Issue: 35 Vol. 129; ISSN 1932-7455; ISSN 1932-7447

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Alcohols
Aldehydes
Methanol
Organic reactions
Oxides
Stability
carbon dioxide
catalysis
titanium oxide

Title: The Surface Chemistry of Methanol on TiO2(110): Effects of Pressure and Temperature on the Stability of C–O and C–H Bonds

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Title: The Surface Chemistry of Methanol on TiO₂(110): Effects of Pressure and Temperature on the Stability of C–O and C–H Bonds