Computational Insights on the Electrocatalytic Behavior of [Cp*Rh] Molecular Catalysts Immobilized on Graphene for Heterogeneous Hydrogen Evolution Reaction

<p dir="ltr">The heterogeneous metal-based molecular electrocatalyst can typically exhibit attractive features compared to its homogeneous analogue including recoverability and durability. As such, it is necessary to evaluate the electrocatalytic behavior of heterogenized molecular c...

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التفاصيل البيبلوغرافية
المؤلف الرئيسي: Abdulilah Dawoud Bani-Yaseen (14152812) (author)
مؤلفون آخرون: Elkhansa Elbashier (14152815) (author)
منشور في: 2020
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author Abdulilah Dawoud Bani-Yaseen (14152812)
author2 Elkhansa Elbashier (14152815)
author2_role author
author_facet Abdulilah Dawoud Bani-Yaseen (14152812)
Elkhansa Elbashier (14152815)
author_role author
dc.creator.none.fl_str_mv Abdulilah Dawoud Bani-Yaseen (14152812)
Elkhansa Elbashier (14152815)
dc.date.none.fl_str_mv 2020-04-01T18:00:00Z
dc.identifier.none.fl_str_mv 10.1038/s41598-020-62758-6
dc.relation.none.fl_str_mv https://figshare.com/articles/journal_contribution/Computational_Insights_on_the_Electrocatalytic_Behavior_of_Cp_Rh_Molecular_Catalysts_Immobilized_on_Graphene_for_Heterogeneous_Hydrogen_Evolution_Reaction/21598161
dc.rights.none.fl_str_mv CC BY 4.0
info:eu-repo/semantics/openAccess
dc.subject.none.fl_str_mv Engineering
Nanotechnology
Information and computing sciences
Applied computing
Molecular Electrocatalysts
Rhodium Complexes
Nanographene-based Catalysts
Electrocatalytic Behavior
dc.title.none.fl_str_mv Computational Insights on the Electrocatalytic Behavior of [Cp*Rh] Molecular Catalysts Immobilized on Graphene for Heterogeneous Hydrogen Evolution Reaction
dc.type.none.fl_str_mv Text
Journal contribution
info:eu-repo/semantics/publishedVersion
text
contribution to journal
description <p dir="ltr">The heterogeneous metal-based molecular electrocatalyst can typically exhibit attractive features compared to its homogeneous analogue including recoverability and durability. As such, it is necessary to evaluate the electrocatalytic behavior of heterogenized molecular catalysts of interest toward gaining insights concerning the retainability of such behaviors while benefiting from heterogenization. In this work, we examined computationally the electrochemical properties of nanographene-based heterogenized molecular complexes of Rhodium. We assessed, as well, the electrocatalytic behavior of the heterogenized molecular catalyst for hydrogen evolution reaction (HER). Two electrochemical pathways were examined, namely one- and two-electron electrochemical reduction pathways. Interestingly, it is computationally demonstrated that [Rh<sup>III</sup>(Cp*)(phen)Cl]<sup>+</sup>-Gr can exhibit redox and electrocatalytic properties for HER that are comparable to its homogeneous analogue via a two-electron reduction pathway. On the other hand, the one-electron reduction pathway is notably found to be less favorable kinetically and thermodynamically. Furthermore, molecular insights are provided with respect to the HER employing molecular orbitals analyses and mechanistic aspects. Importantly, our findings may provide insights toward designing more efficient graphene-based molecular heterogeneous electrocatalysts for more efficient energy production.</p><h2>Other Information</h2><p dir="ltr">Published in: Scientific Reports<br>License: <a href="https://creativecommons.org/licenses/by/4.0" target="_blank">https://creativecommons.org/licenses/by/4.0</a><br>See article on publisher's website: <a href="http://dx.doi.org/10.1038/s41598-020-62758-6" target="_blank">http://dx.doi.org/10.1038/s41598-020-62758-6</a></p>
eu_rights_str_mv openAccess
id Manara2_2b0cef4a778325c236cc8e4264a94c2f
identifier_str_mv 10.1038/s41598-020-62758-6
network_acronym_str Manara2
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oai_identifier_str oai:figshare.com:article/21598161
publishDate 2020
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spelling Computational Insights on the Electrocatalytic Behavior of [Cp*Rh] Molecular Catalysts Immobilized on Graphene for Heterogeneous Hydrogen Evolution ReactionAbdulilah Dawoud Bani-Yaseen (14152812)Elkhansa Elbashier (14152815)EngineeringNanotechnologyInformation and computing sciencesApplied computingMolecular ElectrocatalystsRhodium ComplexesNanographene-based CatalystsElectrocatalytic Behavior<p dir="ltr">The heterogeneous metal-based molecular electrocatalyst can typically exhibit attractive features compared to its homogeneous analogue including recoverability and durability. As such, it is necessary to evaluate the electrocatalytic behavior of heterogenized molecular catalysts of interest toward gaining insights concerning the retainability of such behaviors while benefiting from heterogenization. In this work, we examined computationally the electrochemical properties of nanographene-based heterogenized molecular complexes of Rhodium. We assessed, as well, the electrocatalytic behavior of the heterogenized molecular catalyst for hydrogen evolution reaction (HER). Two electrochemical pathways were examined, namely one- and two-electron electrochemical reduction pathways. Interestingly, it is computationally demonstrated that [Rh<sup>III</sup>(Cp*)(phen)Cl]<sup>+</sup>-Gr can exhibit redox and electrocatalytic properties for HER that are comparable to its homogeneous analogue via a two-electron reduction pathway. On the other hand, the one-electron reduction pathway is notably found to be less favorable kinetically and thermodynamically. Furthermore, molecular insights are provided with respect to the HER employing molecular orbitals analyses and mechanistic aspects. Importantly, our findings may provide insights toward designing more efficient graphene-based molecular heterogeneous electrocatalysts for more efficient energy production.</p><h2>Other Information</h2><p dir="ltr">Published in: Scientific Reports<br>License: <a href="https://creativecommons.org/licenses/by/4.0" target="_blank">https://creativecommons.org/licenses/by/4.0</a><br>See article on publisher's website: <a href="http://dx.doi.org/10.1038/s41598-020-62758-6" target="_blank">http://dx.doi.org/10.1038/s41598-020-62758-6</a></p>2020-04-01T18:00:00ZTextJournal contributioninfo:eu-repo/semantics/publishedVersiontextcontribution to journal10.1038/s41598-020-62758-6https://figshare.com/articles/journal_contribution/Computational_Insights_on_the_Electrocatalytic_Behavior_of_Cp_Rh_Molecular_Catalysts_Immobilized_on_Graphene_for_Heterogeneous_Hydrogen_Evolution_Reaction/21598161CC BY 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/215981612020-04-01T18:00:00Z
spellingShingle Computational Insights on the Electrocatalytic Behavior of [Cp*Rh] Molecular Catalysts Immobilized on Graphene for Heterogeneous Hydrogen Evolution Reaction
Abdulilah Dawoud Bani-Yaseen (14152812)
Engineering
Nanotechnology
Information and computing sciences
Applied computing
Molecular Electrocatalysts
Rhodium Complexes
Nanographene-based Catalysts
Electrocatalytic Behavior
status_str publishedVersion
title Computational Insights on the Electrocatalytic Behavior of [Cp*Rh] Molecular Catalysts Immobilized on Graphene for Heterogeneous Hydrogen Evolution Reaction
title_full Computational Insights on the Electrocatalytic Behavior of [Cp*Rh] Molecular Catalysts Immobilized on Graphene for Heterogeneous Hydrogen Evolution Reaction
title_fullStr Computational Insights on the Electrocatalytic Behavior of [Cp*Rh] Molecular Catalysts Immobilized on Graphene for Heterogeneous Hydrogen Evolution Reaction
title_full_unstemmed Computational Insights on the Electrocatalytic Behavior of [Cp*Rh] Molecular Catalysts Immobilized on Graphene for Heterogeneous Hydrogen Evolution Reaction
title_short Computational Insights on the Electrocatalytic Behavior of [Cp*Rh] Molecular Catalysts Immobilized on Graphene for Heterogeneous Hydrogen Evolution Reaction
title_sort Computational Insights on the Electrocatalytic Behavior of [Cp*Rh] Molecular Catalysts Immobilized on Graphene for Heterogeneous Hydrogen Evolution Reaction
topic Engineering
Nanotechnology
Information and computing sciences
Applied computing
Molecular Electrocatalysts
Rhodium Complexes
Nanographene-based Catalysts
Electrocatalytic Behavior