Binding of Formic Acid on Anatase TiO2(101)

Wang, Yang; Wen, Bo; Dahal, Arjun; Kimmel, Greg A.; Rousseau, Roger; Selloni, Annabella; Petrik, Nikolay G.; Dohnálek, Zdenek

doi:10.1021/acs.jpcc.0c06031

Binding of Formic Acid on Anatase TiO₂(101)

Journal Article · Fri Aug 14 00:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c06031· OSTI ID:1774039

Wang, Yang ^[1]; Wen, Bo ^[2]; ^[3]; ^[4]; ^[4]; ^[2]; ^[4]; ^[5]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Princeton University
Princeton Univ., NJ (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of South Alabama, Mobile, AL (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)

The adsorption of formic acid (FA) and the formation of formate species on metal oxide surfaces are of great interest in catalysis. Formic acid is used to probe the adsorption properties of surface sites, and formates are common intermediates in many catalytic reactions. In this paper, we focus on the interaction of FA with a prototypical anatase TiO₂(101) surface by using a combination of scanning tunneling microscopy (STM), infrared reflection absorption spectroscopy (IRAS), electron-stimulated desorption (ESD), and density functional theory (DFT) to assess the coverage-dependent evolution of different FA-derived surface species at low temperatures (80-240 K). We find that isolated FA adsorbs at 80 K in both monodentate (MD) and bidentate (BD) configurations on top of undercoordinated Ti sites (Ti_5c). The MD form is likely deprotonated and readily converts upon annealing to deprotonated bridging BD on two neighboring Ti_5c sites. DFT calculations show that molecularly bound MD FA is metastable and readily converts to a deprotonated state in the proximity of subsurface oxygen vacancy. The stability of the MD species increases as the availability of the paired Ti_5c sites for BD formation diminishes at high coverages. Upon surface saturation, a mixed configuration of alternating MD and BD species with a coverage of 2/3 FA/Ti_5c represents the most favorable configuration. This is in contrast with the adsorption of FA on rutile TiO₂(110) and many other oxides, where bidentate formate species dominate.

View Accepted Manuscript (DOE)

Research Organization:: Princeton Univ., NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0007347

OSTI ID:: 1774039

Alternate ID(s):: OSTI ID: 1701727

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 37 Vol. 124; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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