Engineering Magnetic Heterostructures with Synergistic Regulation of Charge‐Transfer and Spin‐Ordering for Enhanced Water Oxidation
Abstract The design of heterojunctions offers a crucial solution for energy conversion and storage challenges, but current research predominantly focuses on charge transfer benefits, often neglecting spin attribute regulation despite the increasing recognition of spin‐sensitivity in many chemical re...
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| Format: | Article |
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Wiley
2025-01-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202409842 |
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| author | Chongyan Hao Yang Wu Xiaobo Zheng Yumeng Du Yameng Fan Weikong Pang Anton Tadich Shujun Zhang Thomas Frauenheim Tianyi Ma Xiaoning Li Zhenxiang Cheng |
| author_facet | Chongyan Hao Yang Wu Xiaobo Zheng Yumeng Du Yameng Fan Weikong Pang Anton Tadich Shujun Zhang Thomas Frauenheim Tianyi Ma Xiaoning Li Zhenxiang Cheng |
| author_sort | Chongyan Hao |
| collection | DOAJ |
| description | Abstract The design of heterojunctions offers a crucial solution for energy conversion and storage challenges, but current research predominantly focuses on charge transfer benefits, often neglecting spin attribute regulation despite the increasing recognition of spin‐sensitivity in many chemical reactions. In this study, a novel magnetic heterostructure, CoFe2O4@CoFeMo3O8, is designed to simultaneously modulate charge and spin characteristics, and systematically elucidated their synergistic impact on the oxygen evolution reaction (OER). Experimental results and density functional theory calculations confirmed that the magnetic heterostructure exhibits both charge transfer and spin polarization. It is found that the charge‐transfer behavior enhances conductivity and adsorption ability through band structure regulation. Meanwhile, magnetically polarized electrons promote triplet O2 generation and accelerate electron transport via spin‐selective pathways. Moreover, the heterostructure's effective response to external alternating magnetic fields further amplifies the spin‐dependent effect and introduces a magnetothermal effect, locally heating the active sites through spin flip, thereby boosting catalytic activity. Consequently, the OER activity of the magnetic heterostructure is improved by 83.8 times at 1.5 V compared to its individual components. This magnetic heterojunction strategy presents a promising avenue for advanced catalysis through synergistic regulating of charge‐transfer and spin‐ordering. |
| format | Article |
| id | doaj-art-2df86572f70a4e2d8e81207b9469de77 |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-2df86572f70a4e2d8e81207b9469de772025-01-20T13:04:18ZengWileyAdvanced Science2198-38442025-01-01123n/an/a10.1002/advs.202409842Engineering Magnetic Heterostructures with Synergistic Regulation of Charge‐Transfer and Spin‐Ordering for Enhanced Water OxidationChongyan Hao0Yang Wu1Xiaobo Zheng2Yumeng Du3Yameng Fan4Weikong Pang5Anton Tadich6Shujun Zhang7Thomas Frauenheim8Tianyi Ma9Xiaoning Li10Zhenxiang Cheng11Institute for Superconducting and Electronic Materials University of Wollongong Wollongong 2500 AustraliaBremen Center for Computational Materials Science University of Bremen 28359 Bremen GermanyInstitute for Superconducting and Electronic Materials University of Wollongong Wollongong 2500 AustraliaInstitute for Superconducting and Electronic Materials University of Wollongong Wollongong 2500 AustraliaInstitute for Superconducting and Electronic Materials University of Wollongong Wollongong 2500 AustraliaInstitute for Superconducting and Electronic Materials University of Wollongong Wollongong 2500 AustraliaAustralian Synchrotron Australian Nuclear Science and Technology Organization Clayton VIC 3168 AustraliaInstitute for Superconducting and Electronic Materials University of Wollongong Wollongong 2500 AustraliaSchool of Science Constructor University 28759 Bremen GermanySchool of Science RMIT University Melbourne VIC 3000 AustraliaInstitute for Superconducting and Electronic Materials University of Wollongong Wollongong 2500 AustraliaInstitute for Superconducting and Electronic Materials University of Wollongong Wollongong 2500 AustraliaAbstract The design of heterojunctions offers a crucial solution for energy conversion and storage challenges, but current research predominantly focuses on charge transfer benefits, often neglecting spin attribute regulation despite the increasing recognition of spin‐sensitivity in many chemical reactions. In this study, a novel magnetic heterostructure, CoFe2O4@CoFeMo3O8, is designed to simultaneously modulate charge and spin characteristics, and systematically elucidated their synergistic impact on the oxygen evolution reaction (OER). Experimental results and density functional theory calculations confirmed that the magnetic heterostructure exhibits both charge transfer and spin polarization. It is found that the charge‐transfer behavior enhances conductivity and adsorption ability through band structure regulation. Meanwhile, magnetically polarized electrons promote triplet O2 generation and accelerate electron transport via spin‐selective pathways. Moreover, the heterostructure's effective response to external alternating magnetic fields further amplifies the spin‐dependent effect and introduces a magnetothermal effect, locally heating the active sites through spin flip, thereby boosting catalytic activity. Consequently, the OER activity of the magnetic heterostructure is improved by 83.8 times at 1.5 V compared to its individual components. This magnetic heterojunction strategy presents a promising avenue for advanced catalysis through synergistic regulating of charge‐transfer and spin‐ordering.https://doi.org/10.1002/advs.202409842charge‐transfermagnetic heterostructuresspin‐orderingwater oxidation |
| spellingShingle | Chongyan Hao Yang Wu Xiaobo Zheng Yumeng Du Yameng Fan Weikong Pang Anton Tadich Shujun Zhang Thomas Frauenheim Tianyi Ma Xiaoning Li Zhenxiang Cheng Engineering Magnetic Heterostructures with Synergistic Regulation of Charge‐Transfer and Spin‐Ordering for Enhanced Water Oxidation Advanced Science charge‐transfer magnetic heterostructures spin‐ordering water oxidation |
| title | Engineering Magnetic Heterostructures with Synergistic Regulation of Charge‐Transfer and Spin‐Ordering for Enhanced Water Oxidation |
| title_full | Engineering Magnetic Heterostructures with Synergistic Regulation of Charge‐Transfer and Spin‐Ordering for Enhanced Water Oxidation |
| title_fullStr | Engineering Magnetic Heterostructures with Synergistic Regulation of Charge‐Transfer and Spin‐Ordering for Enhanced Water Oxidation |
| title_full_unstemmed | Engineering Magnetic Heterostructures with Synergistic Regulation of Charge‐Transfer and Spin‐Ordering for Enhanced Water Oxidation |
| title_short | Engineering Magnetic Heterostructures with Synergistic Regulation of Charge‐Transfer and Spin‐Ordering for Enhanced Water Oxidation |
| title_sort | engineering magnetic heterostructures with synergistic regulation of charge transfer and spin ordering for enhanced water oxidation |
| topic | charge‐transfer magnetic heterostructures spin‐ordering water oxidation |
| url | https://doi.org/10.1002/advs.202409842 |
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