[{"title":"Lattice-level defect engineering of dense Mn2O3 hosts unlocks fast H+/Zn2+ storage and long-life aqueous zinc-ion batteries","acknowledgement":"Ao Y. acknowledges financial support from the China Scholarship Council (No. 202208320041), the National Natural Science Foundation of China (No. 22475231), and the Shenzhen Science and Technology Planning Project (No. KJZD20230923115227054). The XAS experiments were performed in collaboration with ALBA staff at the NOTOS beamline of ALBA Synchrotron (experiment ID: 2024028418), Barcelona, Spain. JL is a Serra Húnter Fellow and is grateful to the Academia Excellence program (Generalitat de Catalunya) and to the project PID2024-156765OB-C21 funded by MICIU/AEI/10.13039/501100011033 and the European Regional Development Fund (FEDER), and to the María de Maeztu Units of Excellence Programme CEX2023-001300 M, funded by MCIN/AEI/10.13039/501100011033.","oa_version":"None","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","article_processing_charge":"No","date_created":"2026-09-20T22:01:48Z","date_published":"2026-08-31T00:00:00Z","department":[{"_id":"MaIb"}],"language":[{"iso":"eng"}],"publication_identifier":{"issn":["2050-7488"],"eissn":["2050-7496"]},"month":"08","_id":"22965","quality_controlled":"1","status":"public","year":"2026","researchdata_availability":"no","publication_status":"epub_ahead","day":"31","fulldoi":"https://doi.org/10.1039/d6ta05844b","abstract":[{"text":"Manganese-based aqueous zinc-ion batteries (AZIBs) have emerged as promising candidates for large-scale energy storage owing to their low cost, intrinsic safety, and the abundance of constituent elements. However, their practical deployment is still restricted by severe capacity fading caused by Jahn–Teller-induced structural instability and sluggish Zn2+ transport in the cathode. Although surface coating, heteroatom doping, and structural regulation have been widely explored to improve Mn-based cathodes, these approaches may suffer from increased interfacial resistance, compositional complexity, or limited control over the intrinsic electronic structure. In this context, oxygen-vacancy engineering offers a more direct route to modulate local coordination environments and accelerate Zn2+/H+ storage kinetics. Herein, lattice-level defect engineering of a dense Mn2O3 host is achieved through a metal–organic framework-derived synthesis followed by mild secondary annealing. The introduced oxygen vacancies regulate the local electronic structure and coordination environment, thereby facilitating Zn2+ diffusion, accelerating charge-transfer kinetics, and improving electrochemical reversibility. Combined experimental and theoretical investigations further show that oxygen-vacancy engineering enhances electronic conductivity, reduces the Zn2+ migration barrier, and enables a reversible dual-ion storage mechanism involving both H+ and Zn2+. Benefiting from these effects, the Zn‖Vo-Mn2O3 battery delivers a high specific capacity of 359 mAh g−1 at 0.3 A g−1, maintains 210 mAh g−1 at 6 A g−1, and retains 74.3% of its capacity after 10 000 cycles at 12 A g−1 after only 150 s of initial preconditioning. This work highlights oxygen-vacancy engineering as an effective route to enhancing the kinetic and structural stability of Mn-based cathodes for advanced AZIBs.","lang":"eng"}],"article_type":"original","OA_type":"closed access","author":[{"last_name":"Yu","first_name":"Ao","full_name":"Yu, Ao"},{"last_name":"Chang","first_name":"Xingqi","full_name":"Chang, Xingqi"},{"last_name":"Lu","first_name":"Xuan","full_name":"Lu, Xuan"},{"id":"366c4efa-f61c-11f0-808b-d12a4547ac69","first_name":"Ren","full_name":"He, Ren","last_name":"He"},{"last_name":"Yang","full_name":"Yang, Linlin","first_name":"Linlin"},{"last_name":"Chai","first_name":"Jiali","full_name":"Chai, Jiali"},{"first_name":"Xiaoyu","full_name":"Bi, Xiaoyu","last_name":"Bi"},{"last_name":"Chacón-Borrero","first_name":"Jesús","full_name":"Chacón-Borrero, Jesús"},{"last_name":"Mejia-Centeno","full_name":"Mejia-Centeno, Karol V.","first_name":"Karol V."},{"last_name":"Llorca","first_name":"Jordi","full_name":"Llorca, Jordi"},{"full_name":"Villalobos-Portillo, Eduardo","first_name":"Eduardo","last_name":"Villalobos-Portillo"},{"full_name":"Liu, Qirong","first_name":"Qirong","last_name":"Liu"},{"first_name":"Jian","full_name":"Shang, Jian","last_name":"Shang"},{"last_name":"Cabot","first_name":"Andreu","full_name":"Cabot, Andreu"}],"scopus_import":"1","publisher":"Royal Society of Chemistry","supplementarymaterial":"yes","date_updated":"2026-10-06T10:34:27Z","doi":"10.1039/d6ta05844b","dataavailabilitystatement":"The data that support the findings of this study are available within the manuscript and the corresponding supplementary information (SI). Data are available upon request from the authors. Supplementary information is available. See DOI: https://doi.org/10.1039/d6ta05844b.","citation":{"mla":"Yu, Ao, et al. “Lattice-Level Defect Engineering of Dense Mn2O3 Hosts Unlocks Fast H+/Zn2+ Storage and Long-Life Aqueous Zinc-Ion Batteries.” <i>Journal of Materials Chemistry A</i>, Royal Society of Chemistry, 2026, doi:<a href=\"https://doi.org/10.1039/d6ta05844b\">10.1039/d6ta05844b</a>.","ama":"Yu A, Chang X, Lu X, et al. Lattice-level defect engineering of dense Mn2O3 hosts unlocks fast H+/Zn2+ storage and long-life aqueous zinc-ion batteries. <i>Journal of Materials Chemistry A</i>. 2026. doi:<a href=\"https://doi.org/10.1039/d6ta05844b\">10.1039/d6ta05844b</a>","short":"A. Yu, X. Chang, X. Lu, R. He, L. Yang, J. Chai, X. Bi, J. Chacón-Borrero, K.V. Mejia-Centeno, J. Llorca, E. Villalobos-Portillo, Q. Liu, J. Shang, A. Cabot, Journal of Materials Chemistry A (2026).","ista":"Yu A, Chang X, Lu X, He R, Yang L, Chai J, Bi X, Chacón-Borrero J, Mejia-Centeno KV, Llorca J, Villalobos-Portillo E, Liu Q, Shang J, Cabot A. 2026. Lattice-level defect engineering of dense Mn2O3 hosts unlocks fast H+/Zn2+ storage and long-life aqueous zinc-ion batteries. Journal of Materials Chemistry A.","chicago":"Yu, Ao, Xingqi Chang, Xuan Lu, Ren He, Linlin Yang, Jiali Chai, Xiaoyu Bi, et al. “Lattice-Level Defect Engineering of Dense Mn2O3 Hosts Unlocks Fast H+/Zn2+ Storage and Long-Life Aqueous Zinc-Ion Batteries.” <i>Journal of Materials Chemistry A</i>. Royal Society of Chemistry, 2026. <a href=\"https://doi.org/10.1039/d6ta05844b\">https://doi.org/10.1039/d6ta05844b</a>.","apa":"Yu, A., Chang, X., Lu, X., He, R., Yang, L., Chai, J., … Cabot, A. (2026). Lattice-level defect engineering of dense Mn2O3 hosts unlocks fast H+/Zn2+ storage and long-life aqueous zinc-ion batteries. <i>Journal of Materials Chemistry A</i>. Royal Society of Chemistry. <a href=\"https://doi.org/10.1039/d6ta05844b\">https://doi.org/10.1039/d6ta05844b</a>","ieee":"A. Yu <i>et al.</i>, “Lattice-level defect engineering of dense Mn2O3 hosts unlocks fast H+/Zn2+ storage and long-life aqueous zinc-ion batteries,” <i>Journal of Materials Chemistry A</i>. Royal Society of Chemistry, 2026."},"type":"journal_article","publication":"Journal of Materials Chemistry A","das_tickbox":"1"},{"corr_author":"1","fulldoi":"https://doi.org/10.1002/anie.2874510","abstract":[{"lang":"eng","text":"Lattice strain engineering can regulate the electronic structure of electrocatalysts, but stabilizing distorted metastable phases remains challenging. Here, we report an N,N-dimethylformamide-assisted strategy for synthesizing metastable hexagonal close-packed (HCP) Ni nanoparticles with local lattice-spacing deviations reaching approximately 5.2%. Structural and spectroscopic analyses support a dilute interstitial-carbon-stabilized HCP Ni framework dominated by expanded metallic Ni─Ni coordination rather than ordered Ni3C. Carbon-associated perturbations inhibit structural relaxation and retain the distorted HCP framework. Operando x-ray absorption and infrared spectroscopies indicate the formation of a NiOOH-like working surface coupled to an HCP-derived subsurface framework, accompanied by potential-dependent changes in the interfacial hydrogen-bonding environment and urea-derived species. Calculations using idealized metallic models show that HCP lattice strain induces a Ni d-band upshift, anisotropic Ni─Ni bonding, and localized charge redistribution, modifying adsorption-energy trends for the urea oxidation reaction. The optimized HCP-Ni delivers an apparent steady-state Tafel slope of 26.95 mV dec−1, over twice the electrochemically active surface area-normalized activity of the face-centered cubic-containing controls, and approximately 98% apparent urea conversion after 22 h. It sustains current for over 120 h in three-electrode testing and enables over 400 h of urea-assisted zinc–air battery cycling. This work demonstrates dilute interstitial-carbon stabilization as a route to strained metastable electrocatalysts."}],"researchdata_availability":"upon request","day":"15","publication_status":"epub_ahead","keyword":["electrocatalysis","HCP nickel","interstitial carbon","kinetic trapping","lattice strain engineering","urea oxidation reaction"],"author":[{"full_name":"Xue, Qian","first_name":"Qian","last_name":"Xue"},{"full_name":"Yu, Jing","first_name":"Jing","last_name":"Yu"},{"full_name":"Dai, Juguo","first_name":"Juguo","last_name":"Dai"},{"full_name":"Yang, Linlin","first_name":"Linlin","last_name":"Yang"},{"first_name":"Xiaoyu","full_name":"Bi, Xiaoyu","last_name":"Bi"},{"last_name":"Ren","full_name":"Ren, Yuchuan","first_name":"Yuchuan"},{"last_name":"Zhang","first_name":"Jia","full_name":"Zhang, Jia"},{"full_name":"Qi, Xuede","first_name":"Xuede","last_name":"Qi"},{"last_name":"Wang","full_name":"Wang, Yudi","first_name":"Yudi"},{"first_name":"Ying","full_name":"Xu, Ying","last_name":"Xu"},{"first_name":"Jordi","full_name":"Arbiol, Jordi","last_name":"Arbiol"},{"last_name":"He","full_name":"He, Ren","first_name":"Ren","id":"366c4efa-f61c-11f0-808b-d12a4547ac69"},{"first_name":"Xueqiang","full_name":"Qi, Xueqiang","last_name":"Qi"},{"last_name":"Cabot","first_name":"Andreu","full_name":"Cabot, Andreu"}],"article_type":"original","date_updated":"2026-10-07T08:33:58Z","doi":"10.1002/anie.2874510","publisher":"Wiley","scopus_import":"1","pmid":1,"supplementarymaterial":"yes","type":"journal_article","publication":"Angewandte Chemie International Edition","das_tickbox":"1","dataavailabilitystatement":"The data that support the findings of this study are available from thecorresponding author upon reasonable request.","citation":{"apa":"Xue, Q., Yu, J., Dai, J., Yang, L., Bi, X., Ren, Y., … Cabot, A. (2026). Dilute interstitial carbon stabilization of highly strained metastable HCP Nickel for enhanced electrocatalysis. <i>Angewandte Chemie International Edition</i>. Wiley. <a href=\"https://doi.org/10.1002/anie.2874510\">https://doi.org/10.1002/anie.2874510</a>","ieee":"Q. Xue <i>et al.</i>, “Dilute interstitial carbon stabilization of highly strained metastable HCP Nickel for enhanced electrocatalysis,” <i>Angewandte Chemie International Edition</i>. Wiley, 2026.","ama":"Xue Q, Yu J, Dai J, et al. Dilute interstitial carbon stabilization of highly strained metastable HCP Nickel for enhanced electrocatalysis. <i>Angewandte Chemie International Edition</i>. 2026. doi:<a href=\"https://doi.org/10.1002/anie.2874510\">10.1002/anie.2874510</a>","mla":"Xue, Qian, et al. “Dilute Interstitial Carbon Stabilization of Highly Strained Metastable HCP Nickel for Enhanced Electrocatalysis.” <i>Angewandte Chemie International Edition</i>, e2874510, Wiley, 2026, doi:<a href=\"https://doi.org/10.1002/anie.2874510\">10.1002/anie.2874510</a>.","ista":"Xue Q, Yu J, Dai J, Yang L, Bi X, Ren Y, Zhang J, Qi X, Wang Y, Xu Y, Arbiol J, He R, Qi X, Cabot A. 2026. Dilute interstitial carbon stabilization of highly strained metastable HCP Nickel for enhanced electrocatalysis. Angewandte Chemie International Edition., e2874510.","short":"Q. Xue, J. Yu, J. Dai, L. Yang, X. Bi, Y. Ren, J. Zhang, X. Qi, Y. Wang, Y. Xu, J. Arbiol, R. He, X. Qi, A. Cabot, Angewandte Chemie International Edition (2026).","chicago":"Xue, Qian, Jing Yu, Juguo Dai, Linlin Yang, Xiaoyu Bi, Yuchuan Ren, Jia Zhang, et al. “Dilute Interstitial Carbon Stabilization of Highly Strained Metastable HCP Nickel for Enhanced Electrocatalysis.” <i>Angewandte Chemie International Edition</i>. Wiley, 2026. <a href=\"https://doi.org/10.1002/anie.2874510\">https://doi.org/10.1002/anie.2874510</a>."},"article_number":"e2874510","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","article_processing_charge":"No","title":"Dilute interstitial carbon stabilization of highly strained metastable HCP Nickel for enhanced electrocatalysis","acknowledgement":"Q. X., J. Y., X. B., Y. R., J. Z. and X. Q. thank the China Scholarship Council (CSC) for the scholarship support. These experiments were performed at BL22 CLAESS (proposal 20250340148) and BL01 MIRAS(proposal 20250340424, 20250370488) beamlines at ALBA Synchrotron with the collaboration of ALBA staff. The authors acknowledge the use of instrumentation as well as the technical advice provided by JEMCA. This research was financially supported by the Science and Technology Research Program of Chongqing Municipal Education Com-mission (No. KJZD-K202401110) and the Natural Science Foundation of Chongqing (No. CSTB2023NSCQ-MSX0378). 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. ICN2 acknowledges funding from Generalitat de Catalunya2021SGR00457. 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”.ICN2 acknowledges funding from Grant IU16-014206 (METCAM-FIB)funded by the European Union through the European Regional Devel-opment Fund (ERDF), with the support of the Ministry of Research and Universities, Generalitat de Catalunya. ICN2 is founding member ofe-DREAM.","oa_version":"None","external_id":{"pmid":["42745541"]},"department":[{"_id":"MaIb"}],"date_created":"2026-09-27T22:01:53Z","date_published":"2026-09-15T00:00:00Z","_id":"23004","publication_identifier":{"eissn":["1521-3773"],"issn":["1433-7851"]},"language":[{"iso":"eng"}],"month":"09","year":"2026","status":"public","quality_controlled":"1"}]