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The α-WC(0001) Surface as a Hydrogen Sponge: A First Principle Study of H2 Dissociation and Formation of Low and High Coverages
Abstract
Tungsten carbide (WC) displays a Pt-like behavior in catalysis, applied in hydrogenation processes. Numerous theoretical studies have modeled the behavior and use of adsorbed hydrogen without obtaining a general picture, missing basic links between H2 dissociation and generation of high surface coverage (ΘH>0.5 ML). Here, in this study, the capability of C- and W-terminations of the α-WC(0001) surface is analyzed to dissociate several H2 molecules to produce coverages, ΘH, ranging from low to very high values (0.13<ΘH<2.00 ML). Density functional theory and an ab initio atomistic thermodynamic were used to achieve the conditions for H2 dissociation. The WC–C surface has higher capacity to dissociate H2 molecules than WC–W. However, both surfaces can reach full surface coverage, ΘH=1 ML, at mild ambient conditions, T=300 K and P=1 atm, and even up to 500 K at low and high pressures. The H-adatoms on WC–W are more labile than on WC–C. The binding of adsorbates is hindered at high ΘH, implying a need to modulate ΘH according to the application. The results give the basis to understand the capabilities of WC-based catalysts in hydrogenation-related reactions, with the advantage of WC being a hydrogen reservoir at mild practical catalytic conditions.
- Authors:
-
[1];
[2]
- Universidad de Medellín (Colombia)
- Brookhaven National Laboratory (BNL), Upton, NY (United States). Chemistry Division
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1975242
- Report Number(s):
- BNL-224448-2023-JAAM
Journal ID: ISSN 1867-3880
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 13; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 03 NATURAL GAS; methane; hydrogen; zirconium oxide; copper; coverage; DFT; surface science; tungsten carbide
Citation Formats
Jimenez‐Orozco, Carlos, Flórez, Elizabeth, and Rodriguez, Jose A. The α-WC(0001) Surface as a Hydrogen Sponge: A First Principle Study of H2 Dissociation and Formation of Low and High Coverages. United States: N. p., 2023.
Web. doi:10.1002/cctc.202300165.
Jimenez‐Orozco, Carlos, Flórez, Elizabeth, & Rodriguez, Jose A. The α-WC(0001) Surface as a Hydrogen Sponge: A First Principle Study of H2 Dissociation and Formation of Low and High Coverages. United States. https://doi.org/10.1002/cctc.202300165
Jimenez‐Orozco, Carlos, Flórez, Elizabeth, and Rodriguez, Jose A. Mon .
"The α-WC(0001) Surface as a Hydrogen Sponge: A First Principle Study of H2 Dissociation and Formation of Low and High Coverages". United States. https://doi.org/10.1002/cctc.202300165.
@article{osti_1975242,
title = {The α-WC(0001) Surface as a Hydrogen Sponge: A First Principle Study of H2 Dissociation and Formation of Low and High Coverages},
author = {Jimenez‐Orozco, Carlos and Flórez, Elizabeth and Rodriguez, Jose A.},
abstractNote = {Tungsten carbide (WC) displays a Pt-like behavior in catalysis, applied in hydrogenation processes. Numerous theoretical studies have modeled the behavior and use of adsorbed hydrogen without obtaining a general picture, missing basic links between H2 dissociation and generation of high surface coverage (ΘH>0.5 ML). Here, in this study, the capability of C- and W-terminations of the α-WC(0001) surface is analyzed to dissociate several H2 molecules to produce coverages, ΘH, ranging from low to very high values (0.13<ΘH<2.00 ML). Density functional theory and an ab initio atomistic thermodynamic were used to achieve the conditions for H2 dissociation. The WC–C surface has higher capacity to dissociate H2 molecules than WC–W. However, both surfaces can reach full surface coverage, ΘH=1 ML, at mild ambient conditions, T=300 K and P=1 atm, and even up to 500 K at low and high pressures. The H-adatoms on WC–W are more labile than on WC–C. The binding of adsorbates is hindered at high ΘH, implying a need to modulate ΘH according to the application. The results give the basis to understand the capabilities of WC-based catalysts in hydrogenation-related reactions, with the advantage of WC being a hydrogen reservoir at mild practical catalytic conditions.},
doi = {10.1002/cctc.202300165},
journal = {ChemCatChem},
number = 13,
volume = 15,
place = {United States},
year = {Mon May 08 00:00:00 EDT 2023},
month = {Mon May 08 00:00:00 EDT 2023}
}
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