[{"doi":"10.1039/d4ee03750b","acknowledged_ssus":[{"_id":"EM-Fac"},{"_id":"NanoFab"}],"date_updated":"2025-07-10T11:51:27Z","title":"Modulating the solvation structure to enhance amorphous solid electrolyte interface formation for ultra-stable aqueous zinc anode","year":"2025","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","quality_controlled":"1","status":"public","_id":"18853","isi":1,"intvolume":"        18","publisher":"Royal Society of Chemistry","author":[{"full_name":"Zeng, Guifang","last_name":"Zeng","first_name":"Guifang"},{"last_name":"Sun","full_name":"Sun, Qing","first_name":"Qing"},{"id":"03a7e858-01b1-11ec-8b71-99ae6c4a05bc","first_name":"Sharona","full_name":"Horta, Sharona","last_name":"Horta"},{"full_name":"Martínez-Alanis, Paulina R.","last_name":"Martínez-Alanis","first_name":"Paulina R."},{"first_name":"Peng","full_name":"Wu, Peng","last_name":"Wu"},{"last_name":"Li","full_name":"Li, Jing","first_name":"Jing"},{"first_name":"Shang","full_name":"Wang, Shang","last_name":"Wang"},{"id":"43C61214-F248-11E8-B48F-1D18A9856A87","first_name":"Maria","orcid":"0000-0001-5013-2843","last_name":"Ibáñez","full_name":"Ibáñez, Maria"},{"full_name":"Tian, Yanhong","last_name":"Tian","first_name":"Yanhong"},{"full_name":"Ci, Lijie","last_name":"Ci","first_name":"Lijie"},{"last_name":"Cabot","full_name":"Cabot, Andreu","first_name":"Andreu"}],"fulldoi":"https://doi.org/10.1039/d4ee03750b","date_published":"2025-02-21T00:00:00Z","type":"journal_article","date_created":"2025-01-19T23:01:52Z","external_id":{"isi":["001389898000001"]},"OA_type":"closed access","department":[{"_id":"MaIb"}],"month":"02","article_processing_charge":"No","publication_status":"published","volume":18,"abstract":[{"lang":"eng","text":"Electrolyte additives are extensively validated effective in mitigating dendrite growth and parasitic reactions in aqueous zinc-ion batteries (AZIBs). Nonetheless, the mechanisms by which additives influence the formation and characteristics of the inorganic solid–electrolyte interphase (SEI) are not yet fully elucidated. Herein, we investigate how Zn(CF3COO)2 additives influence solvation structure and elucidate the mechanism by which these additives promote the dual reduction of anions. Through cryo-transmission electron microscopy analysis, we identified the SEI as a highly amorphous ZnS/ZnF2 phase. This amorphous hybrid SEI demonstrates exceptional stability, mechanical robustness, and high Zn2+ conductivity, effectively mitigating parasitic reactions and enhancing Zn plating/stripping reversibility. Even under elevated current densities, the Zn anode exhibits ultra-stable longevity and ultra-high reversibility. This study provides a comprehensive understanding of the intrinsic mechanisms governing solvation structure modulation that lead to the formation of amorphous hybrid SEI, underscoring their efficacy in enhancing the performance and durability of AZIBs."}],"day":"21","article_type":"original","scopus_import":"1","publication":"Energy and Environmental Science","page":"1683-1695","language":[{"iso":"eng"}],"issue":"4","acknowledgement":"The authors acknowledge financial support from the Joint Fund of Henan Province Science and Technology R&D Program (235200810097) and the Generalitat de Catalunya (2021SGR01581). This research was supported by the Scientific Service Units (SSU) of ISTA Austria through resources provided by the Electron Microscopy Facility (EMF) and the Nanofabrication Facility (NFF). G. Z. and J. L. thank the China Scholarship Council (CSC) for the scholarship support.","oa_version":"None","citation":{"apa":"Zeng, G., Sun, Q., Horta, S., Martínez-Alanis, P. R., Wu, P., Li, J., … Cabot, A. (2025). Modulating the solvation structure to enhance amorphous solid electrolyte interface formation for ultra-stable aqueous zinc anode. <i>Energy and Environmental Science</i>. Royal Society of Chemistry. <a href=\"https://doi.org/10.1039/d4ee03750b\">https://doi.org/10.1039/d4ee03750b</a>","short":"G. Zeng, Q. Sun, S. Horta, P.R. Martínez-Alanis, P. Wu, J. Li, S. Wang, M. Ibáñez, Y. Tian, L. Ci, A. Cabot, Energy and Environmental Science 18 (2025) 1683–1695.","ieee":"G. Zeng <i>et al.</i>, “Modulating the solvation structure to enhance amorphous solid electrolyte interface formation for ultra-stable aqueous zinc anode,” <i>Energy and Environmental Science</i>, vol. 18, no. 4. Royal Society of Chemistry, pp. 1683–1695, 2025.","chicago":"Zeng, Guifang, Qing Sun, Sharona Horta, Paulina R. Martínez-Alanis, Peng Wu, Jing Li, Shang Wang, et al. “Modulating the Solvation Structure to Enhance Amorphous Solid Electrolyte Interface Formation for Ultra-Stable Aqueous Zinc Anode.” <i>Energy and Environmental Science</i>. Royal Society of Chemistry, 2025. <a href=\"https://doi.org/10.1039/d4ee03750b\">https://doi.org/10.1039/d4ee03750b</a>.","ama":"Zeng G, Sun Q, Horta S, et al. Modulating the solvation structure to enhance amorphous solid electrolyte interface formation for ultra-stable aqueous zinc anode. <i>Energy and Environmental Science</i>. 2025;18(4):1683-1695. doi:<a href=\"https://doi.org/10.1039/d4ee03750b\">10.1039/d4ee03750b</a>","ista":"Zeng G, Sun Q, Horta S, Martínez-Alanis PR, Wu P, Li J, Wang S, Ibáñez M, Tian Y, Ci L, Cabot A. 2025. Modulating the solvation structure to enhance amorphous solid electrolyte interface formation for ultra-stable aqueous zinc anode. Energy and Environmental Science. 18(4), 1683–1695.","mla":"Zeng, Guifang, et al. “Modulating the Solvation Structure to Enhance Amorphous Solid Electrolyte Interface Formation for Ultra-Stable Aqueous Zinc Anode.” <i>Energy and Environmental Science</i>, vol. 18, no. 4, Royal Society of Chemistry, 2025, pp. 1683–95, doi:<a href=\"https://doi.org/10.1039/d4ee03750b\">10.1039/d4ee03750b</a>."},"publication_identifier":{"issn":["1754-5692"],"eissn":["1754-5706"]}},{"citation":{"ama":"He R, Wang S, Yang L, et al. Active site switching on high entropy phosphides as bifunctional oxygen electrocatalysts for rechargeable/robust Zn-air battery. <i>Energy and Environmental Science</i>. 2024;17(19):7193-7208. doi:<a href=\"https://doi.org/10.1039/d4ee01912a\">10.1039/d4ee01912a</a>","mla":"He, Ren, et al. “Active Site Switching on High Entropy Phosphides as Bifunctional Oxygen Electrocatalysts for Rechargeable/Robust Zn-Air Battery.” <i>Energy and Environmental Science</i>, vol. 17, no. 19, Royal Society of Chemistry, 2024, pp. 7193–208, doi:<a href=\"https://doi.org/10.1039/d4ee01912a\">10.1039/d4ee01912a</a>.","ista":"He R, Wang S, Yang L, Horta S, Ding Y, Di C, Zhang X, Xu Y, Ibáñez M, Zhou Y, Mebs S, Dau H, Hausmann JN, Huo W, Menezes PW, Cabot A. 2024. Active site switching on high entropy phosphides as bifunctional oxygen electrocatalysts for rechargeable/robust Zn-air battery. Energy and Environmental Science. 17(19), 7193–7208.","short":"R. He, S. Wang, L. Yang, S. Horta, Y. Ding, C. Di, X. Zhang, Y. Xu, M. Ibáñez, Y. Zhou, S. Mebs, H. Dau, J.N. Hausmann, W. Huo, P.W. Menezes, A. Cabot, Energy and Environmental Science 17 (2024) 7193–7208.","apa":"He, R., Wang, S., Yang, L., Horta, S., Ding, Y., Di, C., … Cabot, A. (2024). Active site switching on high entropy phosphides as bifunctional oxygen electrocatalysts for rechargeable/robust Zn-air battery. <i>Energy and Environmental Science</i>. Royal Society of Chemistry. <a href=\"https://doi.org/10.1039/d4ee01912a\">https://doi.org/10.1039/d4ee01912a</a>","chicago":"He, Ren, Shiqi Wang, Linlin Yang, Sharona Horta, Yang Ding, Chong Di, Xuesong Zhang, et al. “Active Site Switching on High Entropy Phosphides as Bifunctional Oxygen Electrocatalysts for Rechargeable/Robust Zn-Air Battery.” <i>Energy and Environmental Science</i>. Royal Society of Chemistry, 2024. <a href=\"https://doi.org/10.1039/d4ee01912a\">https://doi.org/10.1039/d4ee01912a</a>.","ieee":"R. He <i>et al.</i>, “Active site switching on high entropy phosphides as bifunctional oxygen electrocatalysts for rechargeable/robust Zn-air battery,” <i>Energy and Environmental Science</i>, vol. 17, no. 19. Royal Society of Chemistry, pp. 7193–7208, 2024."},"publication_identifier":{"issn":["1754-5692"],"eissn":["1754-5706"]},"language":[{"iso":"eng"}],"acknowledgement":"This work was financially supported by the SyDEC at project from the Spanish MCIN/AEI/FEDER (PID2022-136883OB-C22) and Generalitat de Catalunya 2021SGR01581. J. N. H. and P. W. M. acknowledge support from the German Federal Ministry of Education and Research in the framework of the project “Catlab” (03EW0015A/B). L. Yang thanks the China Scholarship Council (CSC) for the scholarship support (202008130132). This work was supported by the European Union Horizon 2020 research and innovation program (No. 857470) and the European Regional Development Fund via the Foundation for Polish Science International Research Agenda PLUS program (No. MAB PLUS/2018/8). The publication was created within the framework of the project of the Minister of Science and Higher Education, Poland “Support for the activities of Centres of Excellence established in Poland under Horizon 2020” under contract no. MEiN/2023/DIR/3795. H. D. and S. M. thank the German Federal Ministry of Education and Research (BMBF) for supporting the Live-XAS project (05K22KE1) and the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) for support under Germany's Excellence Strategy – EXC 2008/1 – 390540038 – UniSysCat. The authors thank the Helmholtz-Zentrum Berlin (HZB) for beamtime allocation at the KMC-3 synchrotron beamline of the BESSY synchrotron in Berlin-Adlershof and Dr Ivo Zizak as well as Dr Michael Haumann for technical support.","issue":"19","oa_version":"None","publication":"Energy and Environmental Science","page":"7193-7208","abstract":[{"lang":"eng","text":"High-entropy materials (HEMs) offer a quasi-continuous spectrum of active sites and have generated great expectations in fields such as electrocatalysis and energy storage. Despite their potential, the complex composition and associated surface phenomena of HEMs pose challenges to their rational design and development. In this context, we have synthesized FeCoNiPdWP high entropy phosphide (HEP) nanoparticles using a low-temperature colloidal method, and explored their application as bifunctional electrocatalysts for the oxygen evolution and reduction reactions (OER/ORR). Our analysis provides a detailed understanding of the individual roles and transformations of each element during OER/ORR operation. Notably, the HEPs exhibit an exceptionally low OER overpotential of 227 mV at 10 mA cm−2, attributed to the reconstructed HEP surface into a FeCoNiPdW high entropy oxyhydroxide with high oxidation states of Fe, Co, and Ni serving as the active sites. Additionally, Pd and W play crucial roles in modulating the electronic structure to optimize the adsorption energy of oxygen intermediates. For the ORR, Pd emerges as the most active component. In the reconstructed catalyst, the strong d–d orbital coupling of especially Pd, Co, and W fine-tunes ORR electron transfer pathways, delivering an ORR half-wave potential of 0.81 V with a pure four-electron reduction mechanism. The practicality of these HEPs catalysts is showcased through the assembly of aqueous zinc–air batteries. These batteries demonstrate a superior specific capacity of 886 mA h gZn−1 and maintain excellent stability over more than 700 hours of continuous operation. Overall, this study not only elucidates the role of each element in HEMs but also establishes a foundational framework for the design and development of next-generation bifunctional oxygen catalysts, broadening the potential applications of these complex materials in advanced energy systems."}],"supplementarymaterial":"yes","volume":17,"scopus_import":"1","article_type":"original","day":"22","researchdata_availability":"upon request","date_created":"2024-09-08T22:01:13Z","external_id":{"isi":["001298924700001"]},"dataavailabilitystatement":"The data that support the findings of this study are available from the corresponding author upon reasonable request.","article_processing_charge":"No","month":"08","OA_type":"closed access","department":[{"_id":"MaIb"}],"publication_status":"published","das_tickbox":"1","fulldoi":"https://doi.org/10.1039/d4ee01912a","type":"journal_article","date_published":"2024-08-22T00:00:00Z","publisher":"Royal Society of Chemistry","intvolume":"        17","author":[{"first_name":"Ren","full_name":"He, Ren","last_name":"He"},{"first_name":"Shiqi","last_name":"Wang","full_name":"Wang, Shiqi"},{"first_name":"Linlin","full_name":"Yang, Linlin","last_name":"Yang"},{"full_name":"Horta, Sharona","last_name":"Horta","id":"03a7e858-01b1-11ec-8b71-99ae6c4a05bc","first_name":"Sharona"},{"first_name":"Yang","last_name":"Ding","full_name":"Ding, Yang"},{"full_name":"Di, Chong","last_name":"Di","first_name":"Chong"},{"first_name":"Xuesong","last_name":"Zhang","full_name":"Zhang, Xuesong"},{"full_name":"Xu, Ying","last_name":"Xu","first_name":"Ying"},{"orcid":"0000-0001-5013-2843","id":"43C61214-F248-11E8-B48F-1D18A9856A87","first_name":"Maria","full_name":"Ibáñez, Maria","last_name":"Ibáñez"},{"first_name":"Yingtang","last_name":"Zhou","full_name":"Zhou, Yingtang"},{"first_name":"Stefan","last_name":"Mebs","full_name":"Mebs, Stefan"},{"last_name":"Dau","full_name":"Dau, Holger","first_name":"Holger"},{"full_name":"Hausmann, Jan Niklas","last_name":"Hausmann","first_name":"Jan Niklas"},{"last_name":"Huo","full_name":"Huo, Wenyi","first_name":"Wenyi"},{"last_name":"Menezes","full_name":"Menezes, Prashanth W.","first_name":"Prashanth W."},{"last_name":"Cabot","full_name":"Cabot, Andreu","first_name":"Andreu"}],"date_updated":"2026-10-16T10:04:37Z","year":"2024","title":"Active site switching on high entropy phosphides as bifunctional oxygen electrocatalysts for rechargeable/robust Zn-air battery","doi":"10.1039/d4ee01912a","status":"public","quality_controlled":"1","user_id":"317138e5-6ab7-11ef-aa6d-ffef3953e345","_id":"17897","isi":1},{"month":"11","article_processing_charge":"No","department":[{"_id":"MaIb"}],"publication_status":"published","date_created":"2023-01-12T12:08:41Z","external_id":{"isi":["000863642400001"]},"date_published":"2022-11-01T00:00:00Z","type":"journal_article","related_material":{"link":[{"relation":"erratum","url":"https://doi.org/10.1039/d3ee90067c"}]},"fulldoi":"https://doi.org/10.1039/d2ee02408j","intvolume":"        15","publisher":"Royal Society of Chemistry","author":[{"full_name":"Qin, Yongxin","last_name":"Qin","first_name":"Yongxin"},{"full_name":"Qin, Bingchao","last_name":"Qin","first_name":"Bingchao"},{"full_name":"Wang, Dongyang","last_name":"Wang","first_name":"Dongyang"},{"last_name":"Chang","full_name":"Chang, Cheng","first_name":"Cheng","id":"9E331C2E-9F27-11E9-AE48-5033E6697425","orcid":"0000-0002-9515-4277"},{"last_name":"Zhao","full_name":"Zhao, Li-Dong","first_name":"Li-Dong"}],"_id":"12155","isi":1,"title":"Solid-state cooling: Thermoelectrics","date_updated":"2024-01-22T08:13:43Z","year":"2022","doi":"10.1039/d2ee02408j","quality_controlled":"1","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","status":"public","citation":{"ama":"Qin Y, Qin B, Wang D, Chang C, Zhao L-D. Solid-state cooling: Thermoelectrics. <i>Energy &#38; Environmental Science</i>. 2022;15(11):4527-4541. doi:<a href=\"https://doi.org/10.1039/d2ee02408j\">10.1039/d2ee02408j</a>","ista":"Qin Y, Qin B, Wang D, Chang C, Zhao L-D. 2022. Solid-state cooling: Thermoelectrics. Energy &#38; Environmental Science. 15(11), 4527–4541.","mla":"Qin, Yongxin, et al. “Solid-State Cooling: Thermoelectrics.” <i>Energy &#38; Environmental Science</i>, vol. 15, no. 11, Royal Society of Chemistry, 2022, pp. 4527–41, doi:<a href=\"https://doi.org/10.1039/d2ee02408j\">10.1039/d2ee02408j</a>.","apa":"Qin, Y., Qin, B., Wang, D., Chang, C., &#38; Zhao, L.-D. (2022). Solid-state cooling: Thermoelectrics. <i>Energy &#38; Environmental Science</i>. Royal Society of Chemistry. <a href=\"https://doi.org/10.1039/d2ee02408j\">https://doi.org/10.1039/d2ee02408j</a>","short":"Y. Qin, B. Qin, D. Wang, C. Chang, L.-D. Zhao, Energy &#38; Environmental Science 15 (2022) 4527–4541.","ieee":"Y. Qin, B. Qin, D. Wang, C. Chang, and L.-D. Zhao, “Solid-state cooling: Thermoelectrics,” <i>Energy &#38; Environmental Science</i>, vol. 15, no. 11. Royal Society of Chemistry, pp. 4527–4541, 2022.","chicago":"Qin, Yongxin, Bingchao Qin, Dongyang Wang, Cheng Chang, and Li-Dong Zhao. “Solid-State Cooling: Thermoelectrics.” <i>Energy &#38; Environmental Science</i>. Royal Society of Chemistry, 2022. <a href=\"https://doi.org/10.1039/d2ee02408j\">https://doi.org/10.1039/d2ee02408j</a>."},"keyword":["Pollution","Nuclear Energy and Engineering","Renewable Energy","Sustainability and the Environment","Environmental Chemistry"],"publication_identifier":{"eissn":["1754-5706"],"issn":["1754-5692"]},"oa_version":"None","language":[{"iso":"eng"}],"acknowledgement":"We acknowledge support from the National Key Research and Development Program of China (2018YFA0702100), the National Natural Science Foundation of China (51571007, 51772012, 52002011 and 52002042), the Basic Science Center Project of National Natural Science Foundation of China (51788104), Beijing Natural Science Foundation (JQ18004), 111 Project (B17002), and the National Science Fund for Distinguished Young Scholars (51925101).","issue":"11","publication":"Energy & Environmental Science","page":"4527-4541","abstract":[{"lang":"eng","text":"The growing demand of thermal management in various fields such as miniaturized 5G chips has motivated researchers to develop new and high-performance solid-state refrigeration technologies, typically including multicaloric and thermoelectric (TE) cooling. Among them, TE cooling has attracted huge attention owing to its advantages of rapid response, large cooling temperature difference, high stability, and tunable device size. Bi2Te3-based alloys have long been the only commercialized TE cooling materials, while novel systems SnSe and Mg3(Bi,Sb)2 have recently been discovered as potential candidates. However, challenges and problems still require to be summarized and further resolved for realizing better cooling performance. In this review, we systematically investigate TE cooling from its internal mechanism, crucial parameters, to device design and applications. Furthermore, we summarize the current optimization strategies for existing TE cooling materials, and finally provide some personal prospects especially the material-planification concept on future research on establishing better TE cooling."}],"volume":15,"scopus_import":"1","day":"01","article_type":"original"}]