Tuning dual-Fe sites in Fe–N–C dual-atom catalysts by sulfur doping for enhanced CO₂ electroreduction: Insights from the first-principles computations
<p dir="ltr">This study explores the impact of sulfur doping on the surface and electronic structure of Fe–N–C dual-atom catalysts for electrochemical CO<sub>2</sub> reduction, using first-principles density functional theory (DFT) computations. By introducing one or two...
محفوظ في:
| المؤلف الرئيسي: | |
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| مؤلفون آخرون: | , |
| منشور في: |
2025
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| الموضوعات: | |
| الوسوم: |
إضافة وسم
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| _version_ | 1864513541010096128 |
|---|---|
| author | Manal B. AlHamdan (22150285) |
| author2 | Mazen Khaled (2979294) Abdulilah Dawoud Bani-Yaseen (14152812) |
| author2_role | author author |
| author_facet | Manal B. AlHamdan (22150285) Mazen Khaled (2979294) Abdulilah Dawoud Bani-Yaseen (14152812) |
| author_role | author |
| dc.creator.none.fl_str_mv | Manal B. AlHamdan (22150285) Mazen Khaled (2979294) Abdulilah Dawoud Bani-Yaseen (14152812) |
| dc.date.none.fl_str_mv | 2025-09-01T00:00:00Z |
| dc.identifier.none.fl_str_mv | 10.1016/j.surfin.2025.107310 |
| dc.relation.none.fl_str_mv | https://figshare.com/articles/journal_contribution/Tuning_dual-Fe_sites_in_Fe_N_C_dual-atom_catalysts_by_sulfur_doping_for_enhanced_CO_electroreduction_Insights_from_the_first-principles_computations/30018868 |
| dc.rights.none.fl_str_mv | CC BY 4.0 info:eu-repo/semantics/openAccess |
| dc.subject.none.fl_str_mv | Engineering Materials engineering Nanotechnology FeNC single-atom catalysts Dual surface sites Sulfur doping CO₂ Electroreduction First-principle DFT |
| dc.title.none.fl_str_mv | Tuning dual-Fe sites in Fe–N–C dual-atom catalysts by sulfur doping for enhanced CO₂ electroreduction: Insights from the first-principles computations |
| dc.type.none.fl_str_mv | Text Journal contribution info:eu-repo/semantics/publishedVersion text contribution to journal |
| description | <p dir="ltr">This study explores the impact of sulfur doping on the surface and electronic structure of Fe–N–C dual-atom catalysts for electrochemical CO<sub>2</sub> reduction, using first-principles density functional theory (DFT) computations. By introducing one or two sulfur atoms near the catalytically active Fe centers, we systematically assess changes in geometry, electronic structure, and adsorption behavior. Sulfur incorporation significantly modifies the local electronic environment, notably increasing the density of states near the Fermi level and enhancing charge redistribution at the active sites. These effects result in stronger and more selective adsorption of key reaction intermediates, including CO<sub>2</sub>, *COOH, and *CO<sub>2</sub> as revealed by adsorption energy and charge density analyses. Dual-sulfur doping, in particular, leads to marked improvements in intermediate stabilization, indicating a synergistic effect on catalytic performance. These findings highlight the potential of surface heteroatom doping as an effective strategy for tailoring the activity and selectivity of transition-metal-based catalysts, providing valuable guidance for the rational design of advanced electrocatalysts for CO<sub>2</sub> electroreduction.</p><h2>Other Information</h2><p dir="ltr">Published in: Surfaces and Interfaces<br>License: <a href="http://creativecommons.org/licenses/by/4.0/" target="_blank">http://creativecommons.org/licenses/by/4.0/</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.1016/j.surfin.2025.107310" target="_blank">https://dx.doi.org/10.1016/j.surfin.2025.107310</a></p> |
| eu_rights_str_mv | openAccess |
| id | Manara2_0a01bbb5153876c398d6520a961a62ea |
| identifier_str_mv | 10.1016/j.surfin.2025.107310 |
| network_acronym_str | Manara2 |
| network_name_str | Manara2 |
| oai_identifier_str | oai:figshare.com:article/30018868 |
| publishDate | 2025 |
| repository.mail.fl_str_mv | |
| repository.name.fl_str_mv | |
| repository_id_str | |
| rights_invalid_str_mv | CC BY 4.0 |
| spelling | Tuning dual-Fe sites in Fe–N–C dual-atom catalysts by sulfur doping for enhanced CO₂ electroreduction: Insights from the first-principles computationsManal B. AlHamdan (22150285)Mazen Khaled (2979294)Abdulilah Dawoud Bani-Yaseen (14152812)EngineeringMaterials engineeringNanotechnologyFeNC single-atom catalystsDual surface sitesSulfur dopingCO₂ ElectroreductionFirst-principle DFT<p dir="ltr">This study explores the impact of sulfur doping on the surface and electronic structure of Fe–N–C dual-atom catalysts for electrochemical CO<sub>2</sub> reduction, using first-principles density functional theory (DFT) computations. By introducing one or two sulfur atoms near the catalytically active Fe centers, we systematically assess changes in geometry, electronic structure, and adsorption behavior. Sulfur incorporation significantly modifies the local electronic environment, notably increasing the density of states near the Fermi level and enhancing charge redistribution at the active sites. These effects result in stronger and more selective adsorption of key reaction intermediates, including CO<sub>2</sub>, *COOH, and *CO<sub>2</sub> as revealed by adsorption energy and charge density analyses. Dual-sulfur doping, in particular, leads to marked improvements in intermediate stabilization, indicating a synergistic effect on catalytic performance. These findings highlight the potential of surface heteroatom doping as an effective strategy for tailoring the activity and selectivity of transition-metal-based catalysts, providing valuable guidance for the rational design of advanced electrocatalysts for CO<sub>2</sub> electroreduction.</p><h2>Other Information</h2><p dir="ltr">Published in: Surfaces and Interfaces<br>License: <a href="http://creativecommons.org/licenses/by/4.0/" target="_blank">http://creativecommons.org/licenses/by/4.0/</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.1016/j.surfin.2025.107310" target="_blank">https://dx.doi.org/10.1016/j.surfin.2025.107310</a></p>2025-09-01T00:00:00ZTextJournal contributioninfo:eu-repo/semantics/publishedVersiontextcontribution to journal10.1016/j.surfin.2025.107310https://figshare.com/articles/journal_contribution/Tuning_dual-Fe_sites_in_Fe_N_C_dual-atom_catalysts_by_sulfur_doping_for_enhanced_CO_electroreduction_Insights_from_the_first-principles_computations/30018868CC BY 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/300188682025-09-01T00:00:00Z |
| spellingShingle | Tuning dual-Fe sites in Fe–N–C dual-atom catalysts by sulfur doping for enhanced CO₂ electroreduction: Insights from the first-principles computations Manal B. AlHamdan (22150285) Engineering Materials engineering Nanotechnology FeNC single-atom catalysts Dual surface sites Sulfur doping CO₂ Electroreduction First-principle DFT |
| status_str | publishedVersion |
| title | Tuning dual-Fe sites in Fe–N–C dual-atom catalysts by sulfur doping for enhanced CO₂ electroreduction: Insights from the first-principles computations |
| title_full | Tuning dual-Fe sites in Fe–N–C dual-atom catalysts by sulfur doping for enhanced CO₂ electroreduction: Insights from the first-principles computations |
| title_fullStr | Tuning dual-Fe sites in Fe–N–C dual-atom catalysts by sulfur doping for enhanced CO₂ electroreduction: Insights from the first-principles computations |
| title_full_unstemmed | Tuning dual-Fe sites in Fe–N–C dual-atom catalysts by sulfur doping for enhanced CO₂ electroreduction: Insights from the first-principles computations |
| title_short | Tuning dual-Fe sites in Fe–N–C dual-atom catalysts by sulfur doping for enhanced CO₂ electroreduction: Insights from the first-principles computations |
| title_sort | Tuning dual-Fe sites in Fe–N–C dual-atom catalysts by sulfur doping for enhanced CO₂ electroreduction: Insights from the first-principles computations |
| topic | Engineering Materials engineering Nanotechnology FeNC single-atom catalysts Dual surface sites Sulfur doping CO₂ Electroreduction First-principle DFT |