The α‐WC(0001) Surface as a Hydrogen Sponge: A First Principle Study of H2 Dissociation and Formation of Low and High Coverages
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 cove...
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| creator | Jimenez‐Orozco, Carlos Flórez, Elizabeth Rodriguez, Jose A. |
| description | 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, 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 |
| doi_str_mv | 10.1002/cctc.202300165 |
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H2 molecules dissociate on α‐WC(0001) surfaces with C‐ and W‐termination to achieve several hydrogen coverages, from low to high. The number of H‐adatoms on the surfaces depends upon pressure and temperature conditions. Both WC−C and WC−W can store high amounts of hydrogen, useful for hydrogenation reactions.</description><identifier>ISSN: 1867-3880</identifier><identifier>EISSN: 1867-3899</identifier><identifier>DOI: 10.1002/cctc.202300165</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>03 NATURAL GAS ; Catalysis ; copper ; coverage ; Density functional theory ; DFT ; First principles ; hydrogen ; Hydrogenation ; methane ; surface science ; Tungsten carbide ; zirconium oxide</subject><ispartof>ChemCatChem, 2023-07, Vol.15 (13), p.n/a</ispartof><rights>2023 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0003-1358-2081 ; 0000000313582081 ; 0000000256804214</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fcctc.202300165$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fcctc.202300165$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>230,315,781,785,886,1418,27926,27927,45576,45577</link.rule.ids><backlink>$$Uhttps://www.osti.gov/servlets/purl/1975242$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Jimenez‐Orozco, Carlos</creatorcontrib><creatorcontrib>Flórez, Elizabeth</creatorcontrib><creatorcontrib>Rodriguez, Jose A.</creatorcontrib><creatorcontrib>Brookhaven National Laboratory (BNL), Upton, NY (United States)</creatorcontrib><title>The α‐WC(0001) Surface as a Hydrogen Sponge: A First Principle Study of H2 Dissociation and Formation of Low and High Coverages</title><title>ChemCatChem</title><description>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, 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.
H2 molecules dissociate on α‐WC(0001) surfaces with C‐ and W‐termination to achieve several hydrogen coverages, from low to high. The number of H‐adatoms on the surfaces depends upon pressure and temperature conditions. Both WC−C and WC−W can store high amounts of hydrogen, useful for hydrogenation reactions.</description><subject>03 NATURAL GAS</subject><subject>Catalysis</subject><subject>copper</subject><subject>coverage</subject><subject>Density functional theory</subject><subject>DFT</subject><subject>First principles</subject><subject>hydrogen</subject><subject>Hydrogenation</subject><subject>methane</subject><subject>surface science</subject><subject>Tungsten carbide</subject><subject>zirconium oxide</subject><issn>1867-3880</issn><issn>1867-3899</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNo9kUtOAkEQhidGExHduu7oRhdgP5h-uDOjiAmJJmBcdnqaGmgC09g9SNgZT-BVvIiH8CQOYlhV_ZWvKpV8SXJKcJtgTK-srWybYsowJjzdSxpEctFiUqn9XS_xYXIU4xRjrphIG8nHcALo--vn_fMlu8D15iUaLENhLCATkUG99Sj4MZRosPDlGK7RDeq6ECv0FFxp3WIGaFAtR2vkC9Sj6NbF6K0zlfMlMuUIdX2Yb1MN9P3qb9hz4wnK_BsEM4Z4nBwUZhbh5L82k-fu3TDrtfqP9w_ZTb_lKcdpKwXGlaKFVayTcio4GJvTNLcjxQoBhVI5GCXyHAiRyhgiGMesIGCEkLwA1kzOtnd9rJyO1lVgJ9aXJdhKEyVS2qE1dL6FFsG_LiFWeuqXoaz_0lQyJmkqpawptaVWbgZrvQhubsJaE6w3JvTGhN6Z0Fk2zHaJ_QKelH6w</recordid><startdate>20230707</startdate><enddate>20230707</enddate><creator>Jimenez‐Orozco, Carlos</creator><creator>Flórez, Elizabeth</creator><creator>Rodriguez, Jose A.</creator><general>Wiley Subscription Services, Inc</general><general>ChemPubSoc Europe</general><scope>OIOZB</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0003-1358-2081</orcidid><orcidid>https://orcid.org/0000000313582081</orcidid><orcidid>https://orcid.org/0000000256804214</orcidid></search><sort><creationdate>20230707</creationdate><title>The α‐WC(0001) Surface as a Hydrogen Sponge: A First Principle Study of H2 Dissociation and Formation of Low and High Coverages</title><author>Jimenez‐Orozco, Carlos ; Flórez, Elizabeth ; Rodriguez, Jose A.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-o2605-5e36992fc93456276eacb25bcd93f7ef99bea97bbe1189aa173603f1ea7786fe3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>03 NATURAL GAS</topic><topic>Catalysis</topic><topic>copper</topic><topic>coverage</topic><topic>Density functional theory</topic><topic>DFT</topic><topic>First principles</topic><topic>hydrogen</topic><topic>Hydrogenation</topic><topic>methane</topic><topic>surface science</topic><topic>Tungsten carbide</topic><topic>zirconium oxide</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Jimenez‐Orozco, Carlos</creatorcontrib><creatorcontrib>Flórez, Elizabeth</creatorcontrib><creatorcontrib>Rodriguez, Jose A.</creatorcontrib><creatorcontrib>Brookhaven National Laboratory (BNL), Upton, NY (United States)</creatorcontrib><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>ChemCatChem</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Jimenez‐Orozco, Carlos</au><au>Flórez, Elizabeth</au><au>Rodriguez, Jose A.</au><aucorp>Brookhaven National Laboratory (BNL), Upton, NY (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>The α‐WC(0001) Surface as a Hydrogen Sponge: A First Principle Study of H2 Dissociation and Formation of Low and High Coverages</atitle><jtitle>ChemCatChem</jtitle><date>2023-07-07</date><risdate>2023</risdate><volume>15</volume><issue>13</issue><epage>n/a</epage><issn>1867-3880</issn><eissn>1867-3899</eissn><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, 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.
H2 molecules dissociate on α‐WC(0001) surfaces with C‐ and W‐termination to achieve several hydrogen coverages, from low to high. The number of H‐adatoms on the surfaces depends upon pressure and temperature conditions. Both WC−C and WC−W can store high amounts of hydrogen, useful for hydrogenation reactions.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/cctc.202300165</doi><tpages>10</tpages><orcidid>https://orcid.org/0000-0003-1358-2081</orcidid><orcidid>https://orcid.org/0000000313582081</orcidid><orcidid>https://orcid.org/0000000256804214</orcidid><oa>free_for_read</oa></addata></record> |
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| source | Wiley-Blackwell Journals |
| subjects | 03 NATURAL GAS Catalysis copper coverage Density functional theory DFT First principles hydrogen Hydrogenation methane surface science Tungsten carbide zirconium oxide |
| title | The α‐WC(0001) Surface as a Hydrogen Sponge: A First Principle Study of H2 Dissociation and Formation of Low and High Coverages |
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