Boosting high-loading zinc-ion battery performance: Zn-Doped d-MnO2 cathodes to promote Zn2+ storage
Rechargeable aqueous zinc-ion batteries (AZIBs) have emerged as a leading contender for stationary energy storage systems due to their low cost, safety, and environmental sustainability. However, their widespread practical application is hindered by the limited stability and capacity of current AZIB...
| Autores: | , , , , , , , , , , , , , |
|---|---|
| Tipo de recurso: | artículo |
| Fecha de publicación: | 2025 |
| País: | España |
| Institución: | Universitat Politècnica de Catalunya (UPC) |
| Repositorio: | UPCommons. Portal del coneixement obert de la UPC |
| Idioma: | inglés |
| OAI Identifier: | oai:upcommons.upc.edu:2117/443989 |
| Acceso en línea: | https://hdl.handle.net/2117/443989 https://dx.doi.org/10.1016/j.ensm.2025.104486 |
| Access Level: | acceso abierto |
| Palabra clave: | Zn-MnO2 Zinc-ion battery Zn storage mechanism High-capacity retention Binder-free Self-supporting electrode Àrees temàtiques de la UPC::Enginyeria dels materials |
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Boosting high-loading zinc-ion battery performance: Zn-Doped d-MnO2 cathodes to promote Zn2+ storage |
| title |
Boosting high-loading zinc-ion battery performance: Zn-Doped d-MnO2 cathodes to promote Zn2+ storage |
| spellingShingle |
Boosting high-loading zinc-ion battery performance: Zn-Doped d-MnO2 cathodes to promote Zn2+ storage Chacón Borrero, Jesús Zn-MnO2 Zinc-ion battery Zn storage mechanism High-capacity retention Binder-free Self-supporting electrode Àrees temàtiques de la UPC::Enginyeria dels materials |
| title_short |
Boosting high-loading zinc-ion battery performance: Zn-Doped d-MnO2 cathodes to promote Zn2+ storage |
| title_full |
Boosting high-loading zinc-ion battery performance: Zn-Doped d-MnO2 cathodes to promote Zn2+ storage |
| title_fullStr |
Boosting high-loading zinc-ion battery performance: Zn-Doped d-MnO2 cathodes to promote Zn2+ storage |
| title_full_unstemmed |
Boosting high-loading zinc-ion battery performance: Zn-Doped d-MnO2 cathodes to promote Zn2+ storage |
| title_sort |
Boosting high-loading zinc-ion battery performance: Zn-Doped d-MnO2 cathodes to promote Zn2+ storage |
| dc.creator.none.fl_str_mv |
Chacón Borrero, Jesús Chang, Xingqi Min, Zhiwen Yu, Jing Montaña Mora, Guillem Mejia Centeno, Karol V. Sun, Yuanmiao Zhou, Xiaolong Tunmee, Sarayut Kidkhunthod, Pinit Li, Junshan Llorca Piqué, Jordi|||0000-0002-7447-9582 Arbiol Cobos, Jordi Cabot Codina, Andreu |
| author |
Chacón Borrero, Jesús |
| author_facet |
Chacón Borrero, Jesús Chang, Xingqi Min, Zhiwen Yu, Jing Montaña Mora, Guillem Mejia Centeno, Karol V. Sun, Yuanmiao Zhou, Xiaolong Tunmee, Sarayut Kidkhunthod, Pinit Li, Junshan Llorca Piqué, Jordi|||0000-0002-7447-9582 Arbiol Cobos, Jordi Cabot Codina, Andreu |
| author_role |
author |
| author2 |
Chang, Xingqi Min, Zhiwen Yu, Jing Montaña Mora, Guillem Mejia Centeno, Karol V. Sun, Yuanmiao Zhou, Xiaolong Tunmee, Sarayut Kidkhunthod, Pinit Li, Junshan Llorca Piqué, Jordi|||0000-0002-7447-9582 Arbiol Cobos, Jordi Cabot Codina, Andreu |
| author2_role |
author author author author author author author author author author author author author |
| dc.subject.none.fl_str_mv |
Zn-MnO2 Zinc-ion battery Zn storage mechanism High-capacity retention Binder-free Self-supporting electrode Àrees temàtiques de la UPC::Enginyeria dels materials |
| topic |
Zn-MnO2 Zinc-ion battery Zn storage mechanism High-capacity retention Binder-free Self-supporting electrode Àrees temàtiques de la UPC::Enginyeria dels materials |
| description |
Rechargeable aqueous zinc-ion batteries (AZIBs) have emerged as a leading contender for stationary energy storage systems due to their low cost, safety, and environmental sustainability. However, their widespread practical application is hindered by the limited stability and capacity of current AZIB cathodes, such as man- ganese oxide (MnO2), which affects their long-term cost-effectiveness. To overcome this limitation, we introduce zinc (Zn) doping in d-MnO2, which modulates the electronic states of Mn atoms, suppresses Jahn–Teller distortion, and enhances structural stability. Additionally, the use of a binder-free, self-supported porous elec- trode without current collectors facilitates three-dimensional ion diffusion, further improving electrochemical performance. As a result, the assembled AZIBs demonstrate outstanding rate capability, delivering 440 mAh•g-1 at 0.2 A•g-1 and retaining 118 mAh•g-1 at 24 A•g-1 for Zn-doped d-MnO2, outperforming the bare d-MnO2 with 356 mAh•g-1 at 0.2 A•g-1 and 80 mAh•g-1 at 24 A•g-1. Additionally, the Zn-doped d-MnO2 exhibits excellent cycling performance with ~100 % capacity retention after 6000 cycles at 150 mAh•g-1 at 10 A•g-1. Furthermore, Zn-doped MnO2 electrodes integrated with carbon nanotubes achieve a high capacity of ~210 mAh•g-1, even at an ultrahigh mass loading (~20 mg•cm-2) at 0.6 mA•g-1. While energy storage in MnO2 involves the reaction and insertion of H+, Mn2+, and Zn2+ cations, density functional theory calculations reveal that Zn intercalation is the dominant storage mechanism in these cells. Overall, this study highlights the potential of Zn-doped MnO2 cathodes as a promising strategy for advancing the stability, capacity, and rate performance of next-generation AZIBs. |
| publishDate |
2025 |
| dc.date.none.fl_str_mv |
2025 2025-09-01 2025 2025-10-17 |
| dc.type.none.fl_str_mv |
journal article http://purl.org/coar/resource_type/c_6501 VoR http://purl.org/coar/version/c_970fb48d4fbd8a85 |
| dc.type.openaire.fl_str_mv |
info:eu-repo/semantics/article |
| format |
article |
| dc.identifier.none.fl_str_mv |
https://hdl.handle.net/2117/443989 https://dx.doi.org/10.1016/j.ensm.2025.104486 |
| url |
https://hdl.handle.net/2117/443989 https://dx.doi.org/10.1016/j.ensm.2025.104486 |
| dc.language.none.fl_str_mv |
Inglés eng |
| language_invalid_str_mv |
Inglés |
| language |
eng |
| dc.rights.none.fl_str_mv |
open access http://purl.org/coar/access_right/c_abf2 Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/ |
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info:eu-repo/semantics/openAccess |
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open access http://purl.org/coar/access_right/c_abf2 Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/ |
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openAccess |
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application/pdf |
| dc.publisher.none.fl_str_mv |
Elsevier |
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Elsevier |
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reponame:UPCommons. Portal del coneixement obert de la UPC instname:Universitat Politècnica de Catalunya (UPC) |
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Universitat Politècnica de Catalunya (UPC) |
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UPCommons. Portal del coneixement obert de la UPC |
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UPCommons. Portal del coneixement obert de la UPC |
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Boosting high-loading zinc-ion battery performance: Zn-Doped d-MnO2 cathodes to promote Zn2+ storageChacón Borrero, JesúsChang, XingqiMin, ZhiwenYu, JingMontaña Mora, GuillemMejia Centeno, Karol V.Sun, YuanmiaoZhou, XiaolongTunmee, SarayutKidkhunthod, PinitLi, JunshanLlorca Piqué, Jordi|||0000-0002-7447-9582Arbiol Cobos, JordiCabot Codina, AndreuZn-MnO2Zinc-ion batteryZn storage mechanismHigh-capacity retentionBinder-freeSelf-supporting electrodeÀrees temàtiques de la UPC::Enginyeria dels materialsRechargeable aqueous zinc-ion batteries (AZIBs) have emerged as a leading contender for stationary energy storage systems due to their low cost, safety, and environmental sustainability. However, their widespread practical application is hindered by the limited stability and capacity of current AZIB cathodes, such as man- ganese oxide (MnO2), which affects their long-term cost-effectiveness. To overcome this limitation, we introduce zinc (Zn) doping in d-MnO2, which modulates the electronic states of Mn atoms, suppresses Jahn–Teller distortion, and enhances structural stability. Additionally, the use of a binder-free, self-supported porous elec- trode without current collectors facilitates three-dimensional ion diffusion, further improving electrochemical performance. As a result, the assembled AZIBs demonstrate outstanding rate capability, delivering 440 mAh•g-1 at 0.2 A•g-1 and retaining 118 mAh•g-1 at 24 A•g-1 for Zn-doped d-MnO2, outperforming the bare d-MnO2 with 356 mAh•g-1 at 0.2 A•g-1 and 80 mAh•g-1 at 24 A•g-1. Additionally, the Zn-doped d-MnO2 exhibits excellent cycling performance with ~100 % capacity retention after 6000 cycles at 150 mAh•g-1 at 10 A•g-1. Furthermore, Zn-doped MnO2 electrodes integrated with carbon nanotubes achieve a high capacity of ~210 mAh•g-1, even at an ultrahigh mass loading (~20 mg•cm-2) at 0.6 mA•g-1. While energy storage in MnO2 involves the reaction and insertion of H+, Mn2+, and Zn2+ cations, density functional theory calculations reveal that Zn intercalation is the dominant storage mechanism in these cells. Overall, this study highlights the potential of Zn-doped MnO2 cathodes as a promising strategy for advancing the stability, capacity, and rate performance of next-generation AZIBs.This work was supported by the project SyDECat (PID2022–136883OB-C22), financed by the Spanish MCIN/AEI, EHAWEDRY (964524), financed by European EXCELLENT SCIENCE – Further and Emerging Technologies, the National Natural Science Foundation of China (52272054, 52125105, 52061160484, 51972329), Natural Science Foundation of Guangdong Province (2019TX05L389, 2022A1515011365), Shenzhen Science and Technology Planning Project (GJHZ20220913142809019, JCYJ20200109115624923), and the Foundation of the National Research Council of Thailand (N42A650253). Thanks to the China Scholarship Council (CSC) for the scholarship support. Part of the present work has been performed in the framework of the Universitat Autònoma de Barcelona Materials Science PhD program. ICN2 acknowledges funding from Generalitat de Catalunya 2021SGR00457. This study is part of the Advanced Materials programme and was supported by MCIN with funding from European Union NextGenerationEU (PRTR-C17.I1) and by Generalitat de Catalunya (In-CAEM Project). The authors thank support from the project AMaDE (PID2023–149158OB-C43), funded by MCIN/ AEI/10.13039/501100011033/ and by “ERDF A way of making Europe”, by the “European Union”. Grant RED2022–134508-T (CAT&SCALE) funded by MCIN/AEI /10.13039/501100011033. ICN2 is supported by the Severo Ochoa program from Spanish MCIN / AEI (Grant No.: CEX2021–001214-S) and is funded by the CERCA Programme / Generalitat de Catalunya. The authors acknowledge the use of instrumentation as well as the technical advice provided by the Joint Electron Microscopy Center at ALBA (JEMCA). ICN2 acknowledges funding from Grant IU16–014206 (METCAM-FIB) funded by the European Union through the European Regional Development Fund (ERDF), with the support of the Ministry of Research and Universities, Generalitat de Catalunya. ICN2 is a founding member of e-DREAM． [59] J.L. is a Serra Húnter Fellow and is grateful to the ICREA Academia program and projects MCIN/FEDER PID2021–124572OB-C31, CEX2023–001300-M, and GC 2021 SGR 01061.Elsevier20252025-09-0120252025-10-17journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/2117/443989https://dx.doi.org/10.1016/j.ensm.2025.104486reponame:UPCommons. Portal del coneixement obert de la UPCinstname:Universitat Politècnica de Catalunya (UPC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:upcommons.upc.edu:2117/4439892026-05-27T15:37:01Z |
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15,811543 |