On the structure sensitivity of and CO coverage effects on formic acid decomposition on Pd surfaces
Abstract
Using density functional theory calculations, the Pd-catalyzed vapor-phase formic acid decomposition was studied, with a focus on the structure sensitivity and CO coverage effects. A comprehensive reaction network was developed on both the (111) and (100) facets of Pd, at CO coverages of 0 and 5/9 monolayer (ML). Pd(100) was determined to be more reactive than Pd(111) at both CO coverages. The introduction of 5/9 ML CO decreased the activity of both facets significantly, due to destabilization of the surface intermediates and transition states on the CO-decorated surfaces. Three reaction pathways were explored on the clean surfaces: the formate (HCOO) pathway, the carboxyl (COOH) pathway leading to the formation of CO2, and the COOH pathway leading to the formation of CO (COOH→CO). Based on the DFT-derived energetics alone, it appears that all three pathways contribute to the reaction on clean Pd, whereas the presence of 5/9 ML of CO inhibits the HCOO pathway on both facets and favors the COOH→CO pathway on the (111) facet, but the COOH→CO2 one on the (100) facet. Moreover, at high CO coverages, alternative spectator CO-assisted adsorbate decomposition pathways were discovered, which could potentially play a role in formic acid decomposition on Pd catalysts undermore »
- Authors:
-
- University of Wisconsin, Madison, WI (United States)
- Publication Date:
- Research Org.:
- Univ. of Wisconsin, Madison, WI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1849599
- Alternate Identifier(s):
- OSTI ID: 1818597
- Grant/Contract Number:
- FG02-05ER15731; AC02-05CH11231; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Surface Science
- Additional Journal Information:
- Journal Volume: 709; Journal Issue: C; Journal ID: ISSN 0039-6028
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Li, Sha, Rangarajan, Srinivas, Scaranto, Jessica, and Mavrikakis, Manos. On the structure sensitivity of and CO coverage effects on formic acid decomposition on Pd surfaces. United States: N. p., 2021.
Web. doi:10.1016/j.susc.2021.121846.
Li, Sha, Rangarajan, Srinivas, Scaranto, Jessica, & Mavrikakis, Manos. On the structure sensitivity of and CO coverage effects on formic acid decomposition on Pd surfaces. United States. https://doi.org/10.1016/j.susc.2021.121846
Li, Sha, Rangarajan, Srinivas, Scaranto, Jessica, and Mavrikakis, Manos. Thu .
"On the structure sensitivity of and CO coverage effects on formic acid decomposition on Pd surfaces". United States. https://doi.org/10.1016/j.susc.2021.121846. https://www.osti.gov/servlets/purl/1849599.
@article{osti_1849599,
title = {On the structure sensitivity of and CO coverage effects on formic acid decomposition on Pd surfaces},
author = {Li, Sha and Rangarajan, Srinivas and Scaranto, Jessica and Mavrikakis, Manos},
abstractNote = {Using density functional theory calculations, the Pd-catalyzed vapor-phase formic acid decomposition was studied, with a focus on the structure sensitivity and CO coverage effects. A comprehensive reaction network was developed on both the (111) and (100) facets of Pd, at CO coverages of 0 and 5/9 monolayer (ML). Pd(100) was determined to be more reactive than Pd(111) at both CO coverages. The introduction of 5/9 ML CO decreased the activity of both facets significantly, due to destabilization of the surface intermediates and transition states on the CO-decorated surfaces. Three reaction pathways were explored on the clean surfaces: the formate (HCOO) pathway, the carboxyl (COOH) pathway leading to the formation of CO2, and the COOH pathway leading to the formation of CO (COOH→CO). Based on the DFT-derived energetics alone, it appears that all three pathways contribute to the reaction on clean Pd, whereas the presence of 5/9 ML of CO inhibits the HCOO pathway on both facets and favors the COOH→CO pathway on the (111) facet, but the COOH→CO2 one on the (100) facet. Moreover, at high CO coverages, alternative spectator CO-assisted adsorbate decomposition pathways were discovered, which could potentially play a role in formic acid decomposition on Pd catalysts under realistic reaction conditions.},
doi = {10.1016/j.susc.2021.121846},
journal = {Surface Science},
number = C,
volume = 709,
place = {United States},
year = {Thu Mar 18 00:00:00 EDT 2021},
month = {Thu Mar 18 00:00:00 EDT 2021}
}
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