Photocatalytic activity of MoS2 with water monolayers: Global optimization
Atomically thin MoS2 has emerged to be promising for photocatalytic water splitting benefiting from its suitable geometrical and electronic structure for light harvesting. A better understanding of how water molecules affect the band edge levels of MoS2 is critical for promoting the interfacial reac...
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Veröffentlicht in: | The Journal of chemical physics 2022-11, Vol.157 (18), p.184703-184703 |
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description | Atomically thin MoS2 has emerged to be promising for photocatalytic water splitting benefiting from its suitable geometrical and electronic structure for light harvesting. A better understanding of how water molecules affect the band edge levels of MoS2 is critical for promoting the interfacial reactivity. Here, we determine the structures of water monolayers on MoS2 using global optimizations achieved by molecular dynamics in combination with local minimization. It is shown that cyclic water clusters are formed on a surface through a hydrogen-bonding network. The absolute band edge positions are explored taking into account the derivative discontinuity of the exchange–correlation functional. Shifts in band edges are observed with the increase in H2O coverage, while bandgaps tend to be slightly decreased. In particular, the band alignment relative to water redox potentials has been investigated in detail. We find that the dimer configuration is likely to suppress the hydrogen evolution reaction (HER), while the polygon clusters lift the conduction band by 0.2–0.7 eV, and thus, they would enhance HER. This effect is explained in terms of the linear dependence of the band edge offset on an interface electric dipole arising from water assemblies. |
doi_str_mv | 10.1063/5.0123684 |
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A better understanding of how water molecules affect the band edge levels of MoS2 is critical for promoting the interfacial reactivity. Here, we determine the structures of water monolayers on MoS2 using global optimizations achieved by molecular dynamics in combination with local minimization. It is shown that cyclic water clusters are formed on a surface through a hydrogen-bonding network. The absolute band edge positions are explored taking into account the derivative discontinuity of the exchange–correlation functional. Shifts in band edges are observed with the increase in H2O coverage, while bandgaps tend to be slightly decreased. In particular, the band alignment relative to water redox potentials has been investigated in detail. We find that the dimer configuration is likely to suppress the hydrogen evolution reaction (HER), while the polygon clusters lift the conduction band by 0.2–0.7 eV, and thus, they would enhance HER. This effect is explained in terms of the linear dependence of the band edge offset on an interface electric dipole arising from water assemblies.</description><identifier>ISSN: 0021-9606</identifier><identifier>EISSN: 1089-7690</identifier><identifier>DOI: 10.1063/5.0123684</identifier><identifier>CODEN: JCPSA6</identifier><language>eng</language><publisher>Melville: American Institute of Physics</publisher><subject>Catalytic activity ; Clusters ; Conduction bands ; Electric dipoles ; Electronic structure ; Global optimization ; Hydrogen bonding ; Hydrogen evolution reactions ; Molecular dynamics ; Molybdenum disulfide ; Monolayers ; Photocatalysis ; Physics ; Water chemistry ; Water splitting</subject><ispartof>The Journal of chemical physics, 2022-11, Vol.157 (18), p.184703-184703</ispartof><rights>Author(s)</rights><rights>2022 Author(s). 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A better understanding of how water molecules affect the band edge levels of MoS2 is critical for promoting the interfacial reactivity. Here, we determine the structures of water monolayers on MoS2 using global optimizations achieved by molecular dynamics in combination with local minimization. It is shown that cyclic water clusters are formed on a surface through a hydrogen-bonding network. The absolute band edge positions are explored taking into account the derivative discontinuity of the exchange–correlation functional. Shifts in band edges are observed with the increase in H2O coverage, while bandgaps tend to be slightly decreased. In particular, the band alignment relative to water redox potentials has been investigated in detail. We find that the dimer configuration is likely to suppress the hydrogen evolution reaction (HER), while the polygon clusters lift the conduction band by 0.2–0.7 eV, and thus, they would enhance HER. This effect is explained in terms of the linear dependence of the band edge offset on an interface electric dipole arising from water assemblies.</description><subject>Catalytic activity</subject><subject>Clusters</subject><subject>Conduction bands</subject><subject>Electric dipoles</subject><subject>Electronic structure</subject><subject>Global optimization</subject><subject>Hydrogen bonding</subject><subject>Hydrogen evolution reactions</subject><subject>Molecular dynamics</subject><subject>Molybdenum disulfide</subject><subject>Monolayers</subject><subject>Photocatalysis</subject><subject>Physics</subject><subject>Water chemistry</subject><subject>Water splitting</subject><issn>0021-9606</issn><issn>1089-7690</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><recordid>eNqd0M9LwzAUwPEgCs7pwf-g4EWFzpcfTVJvMnQqEwX1XLI0ZRltM5Nso_71dk4QPHp6lw-P974InWIYYeD0KhsBJpRLtocGGGSeCp7DPhoAEJzmHPghOgphAQBYEDZAjy9zF51WUdVdtDpROtq1jV3iquTJvZJkY-M82ahofNK41tWqMz5cJ5PazVSduGW0jf1U0br2GB1Uqg7m5GcO0fvd7dv4Pp0-Tx7GN9NUkxxiqkQ1E6XMsaYs4xlVQKucs0xmRlCipFAzAQxKCVUuFOGcGkVoWWWMMU5A0iE63-1devexMiEWjQ3a1LVqjVuFgggqMJY5Yz09-0MXbuXb_rqtorxvw0ivLnZKexeCN1Wx9LZRviswFNuqRVb8VO3t5c4GbeP32__Da-d_YbEsK_oF7CyDtg</recordid><startdate>20221114</startdate><enddate>20221114</enddate><creator>Zhang, Yachao</creator><general>American Institute of Physics</general><scope>AAYXX</scope><scope>CITATION</scope><scope>8FD</scope><scope>H8D</scope><scope>L7M</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0001-9233-876X</orcidid></search><sort><creationdate>20221114</creationdate><title>Photocatalytic activity of MoS2 with water monolayers: Global optimization</title><author>Zhang, Yachao</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c290t-a7fb7d891c345653a03f964585e732a87ab7040d80f97a2663ea23df544462083</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2022</creationdate><topic>Catalytic activity</topic><topic>Clusters</topic><topic>Conduction bands</topic><topic>Electric dipoles</topic><topic>Electronic structure</topic><topic>Global optimization</topic><topic>Hydrogen bonding</topic><topic>Hydrogen evolution reactions</topic><topic>Molecular dynamics</topic><topic>Molybdenum disulfide</topic><topic>Monolayers</topic><topic>Photocatalysis</topic><topic>Physics</topic><topic>Water chemistry</topic><topic>Water splitting</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhang, Yachao</creatorcontrib><collection>CrossRef</collection><collection>Technology Research Database</collection><collection>Aerospace Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>MEDLINE - Academic</collection><jtitle>The Journal of chemical physics</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhang, Yachao</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Photocatalytic activity of MoS2 with water monolayers: Global optimization</atitle><jtitle>The Journal of chemical physics</jtitle><date>2022-11-14</date><risdate>2022</risdate><volume>157</volume><issue>18</issue><spage>184703</spage><epage>184703</epage><pages>184703-184703</pages><issn>0021-9606</issn><eissn>1089-7690</eissn><coden>JCPSA6</coden><abstract>Atomically thin MoS2 has emerged to be promising for photocatalytic water splitting benefiting from its suitable geometrical and electronic structure for light harvesting. A better understanding of how water molecules affect the band edge levels of MoS2 is critical for promoting the interfacial reactivity. Here, we determine the structures of water monolayers on MoS2 using global optimizations achieved by molecular dynamics in combination with local minimization. It is shown that cyclic water clusters are formed on a surface through a hydrogen-bonding network. The absolute band edge positions are explored taking into account the derivative discontinuity of the exchange–correlation functional. Shifts in band edges are observed with the increase in H2O coverage, while bandgaps tend to be slightly decreased. In particular, the band alignment relative to water redox potentials has been investigated in detail. We find that the dimer configuration is likely to suppress the hydrogen evolution reaction (HER), while the polygon clusters lift the conduction band by 0.2–0.7 eV, and thus, they would enhance HER. This effect is explained in terms of the linear dependence of the band edge offset on an interface electric dipole arising from water assemblies.</abstract><cop>Melville</cop><pub>American Institute of Physics</pub><doi>10.1063/5.0123684</doi><tpages>8</tpages><orcidid>https://orcid.org/0000-0001-9233-876X</orcidid></addata></record> |
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subjects | Catalytic activity Clusters Conduction bands Electric dipoles Electronic structure Global optimization Hydrogen bonding Hydrogen evolution reactions Molecular dynamics Molybdenum disulfide Monolayers Photocatalysis Physics Water chemistry Water splitting |
title | Photocatalytic activity of MoS2 with water monolayers: Global optimization |
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