[{"title":"Exclusive solution discharge in Li-O₂ batteries?","external_id":{"isi":["000860787000001"]},"year":"2022","doi":"10.1021/acsenergylett.2c01711","acknowledged_ssus":[{"_id":"EM-Fac"},{"_id":"M-Shop"}],"ddc":["540"],"isi":1,"tmp":{"image":"/images/cc_by.png","legal_code_url":"https://creativecommons.org/licenses/by/4.0/legalcode","name":"Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)","short":"CC BY (4.0)"},"author":[{"full_name":"Prehal, Christian","last_name":"Prehal","first_name":"Christian"},{"first_name":"Soumyadip","last_name":"Mondal","full_name":"Mondal, Soumyadip","id":"d25d21ef-dc8d-11ea-abe3-ec4576307f48"},{"first_name":"Ludek","full_name":"Lovicar, Ludek","last_name":"Lovicar","id":"36DB3A20-F248-11E8-B48F-1D18A9856A87"},{"orcid":"0000-0003-2902-5319","full_name":"Freunberger, Stefan Alexander","last_name":"Freunberger","first_name":"Stefan Alexander","id":"A8CA28E6-CE23-11E9-AD2D-EC27E6697425"}],"abstract":[{"lang":"eng","text":"Capacity, rate performance, and cycle life of aprotic Li–O2 batteries critically depend on reversible electrodeposition of Li2O2. Current understanding states surface-adsorbed versus solvated LiO2 controls Li2O2 growth as surface film or as large particles. Herein, we show that Li2O2 forms across a wide range of electrolytes, carbons, and current densities as particles via solution-mediated LiO2 disproportionation, bringing into question the prevalence of any surface growth under practical conditions. We describe a unified O2 reduction mechanism, which can explain all found capacity relations and Li2O2 morphologies with exclusive solution discharge. Determining particle morphology and achievable capacities are species mobilities, true areal rate, and the degree of LiO2 association in solution. Capacity is conclusively limited by mass transport through the tortuous Li2O2 rather than electron transport through a passivating Li2O2 film. Provided that species mobilities and surface growth are high, high capacities are also achieved with weakly solvating electrolytes, which were previously considered prototypical for low capacity via surface growth."}],"citation":{"chicago":"Prehal, Christian, Soumyadip Mondal, Ludek Lovicar, and Stefan Alexander Freunberger. “Exclusive Solution Discharge in Li-O₂ Batteries?” <i>ACS Energy Letters</i>. American Chemical Society, 2022. <a href=\"https://doi.org/10.1021/acsenergylett.2c01711\">https://doi.org/10.1021/acsenergylett.2c01711</a>.","ieee":"C. Prehal, S. Mondal, L. Lovicar, and S. A. Freunberger, “Exclusive solution discharge in Li-O₂ batteries?,” <i>ACS Energy Letters</i>, vol. 7, no. 9. American Chemical Society, pp. 3112–3119, 2022.","apa":"Prehal, C., Mondal, S., Lovicar, L., &#38; Freunberger, S. A. (2022). Exclusive solution discharge in Li-O₂ batteries? <i>ACS Energy Letters</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/acsenergylett.2c01711\">https://doi.org/10.1021/acsenergylett.2c01711</a>","short":"C. Prehal, S. Mondal, L. Lovicar, S.A. Freunberger, ACS Energy Letters 7 (2022) 3112–3119.","ista":"Prehal C, Mondal S, Lovicar L, Freunberger SA. 2022. Exclusive solution discharge in Li-O₂ batteries? ACS Energy Letters. 7(9), 3112–3119.","ama":"Prehal C, Mondal S, Lovicar L, Freunberger SA. Exclusive solution discharge in Li-O₂ batteries? <i>ACS Energy Letters</i>. 2022;7(9):3112-3119. doi:<a href=\"https://doi.org/10.1021/acsenergylett.2c01711\">10.1021/acsenergylett.2c01711</a>","mla":"Prehal, Christian, et al. “Exclusive Solution Discharge in Li-O₂ Batteries?” <i>ACS Energy Letters</i>, vol. 7, no. 9, American Chemical Society, 2022, pp. 3112–19, doi:<a href=\"https://doi.org/10.1021/acsenergylett.2c01711\">10.1021/acsenergylett.2c01711</a>."},"publication_status":"published","oa_version":"Published Version","quality_controlled":"1","acknowledgement":"S.A.F. and C.P. are indebted to the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (Grant Agreement No. 636069). This project has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant NanoEvolution, Grant Agreement No. 894042. S.A.F. and S.M. are indebted to Institute of Science and Technology Austria (ISTA) for support. This research was supported by the Scientific Service Units of ISTA through resources provided by the Electron Microscopy Facility and the Miba Machine Shop. C.P. thanks Vanessa Wood (ETH Zürich) for her continuing support.","user_id":"4359f0d1-fa6c-11eb-b949-802e58b17ae8","publication_identifier":{"eissn":["2380-8195"]},"_id":"12065","article_processing_charge":"Yes (via OA deal)","oa":1,"date_updated":"2023-08-03T13:47:56Z","volume":7,"language":[{"iso":"eng"}],"scopus_import":"1","publisher":"American Chemical Society","article_type":"original","date_published":"2022-08-29T00:00:00Z","month":"08","file":[{"success":1,"creator":"dernst","file_id":"12319","content_type":"application/pdf","relation":"main_file","date_created":"2023-01-20T08:43:51Z","checksum":"cf0bed3a2535c11d27244cd029dbc1d0","file_name":"2022_ACSEnergyLetters_Prehal.pdf","file_size":3827583,"date_updated":"2023-01-20T08:43:51Z","access_level":"open_access"}],"date_created":"2022-09-08T09:51:09Z","department":[{"_id":"StFr"},{"_id":"EM-Fac"}],"has_accepted_license":"1","status":"public","intvolume":"         7","type":"journal_article","day":"29","file_date_updated":"2023-01-20T08:43:51Z","page":"3112-3119","publication":"ACS Energy Letters","issue":"9"},{"_id":"9118","publication_identifier":{"eissn":["2380-8195"]},"acknowledgement":"M.C. has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie Grant Agreement No. 665385. ICN2\r\nacknowledges funding from Generalitat de Catalunya 2017 SGR 327. ICN2 is supported by the Severo Ochoa program from Spanish MINECO (Grant No. SEV-2017-0706) and is funded by the CERCA Programme/Generalitat de Catalunya. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 − ESTEEM3. M.V.K. acknowledges the support by the European Research Council under the Horizon 2020 Framework Program (ERC Consolidator Grant SCALEHALO\r\nGrant Agreement No. 819740) and by FET-OPEN project no. 862656 (DROP-IT).","user_id":"4359f0d1-fa6c-11eb-b949-802e58b17ae8","project":[{"call_identifier":"H2020","name":"International IST Doctoral Program","_id":"2564DBCA-B435-11E9-9278-68D0E5697425","grant_number":"665385"}],"quality_controlled":"1","oa_version":"Published Version","date_updated":"2023-08-07T13:46:00Z","oa":1,"volume":6,"article_processing_charge":"Yes (via OA deal)","abstract":[{"lang":"eng","text":"Cesium lead halides have intrinsically unstable crystal lattices and easily transform within perovskite and nonperovskite structures. In this work, we explore the conversion of the perovskite CsPbBr3 into Cs4PbBr6 in the presence of PbS at 450 °C to produce doped nanocrystal-based composites with embedded Cs4PbBr6 nanoprecipitates. We show that PbBr2 is extracted from CsPbBr3 and diffuses into the PbS lattice with a consequent increase in the concentration of free charge carriers. This new doping strategy enables the adjustment of the density of charge carriers between 1019 and 1020 cm–3, and it may serve as a general strategy for doping other nanocrystal-based semiconductors."}],"author":[{"first_name":"Mariano","full_name":"Calcabrini, Mariano","last_name":"Calcabrini","id":"45D7531A-F248-11E8-B48F-1D18A9856A87"},{"first_name":"Aziz","full_name":"Genc, Aziz","last_name":"Genc"},{"first_name":"Yu","orcid":"0000-0001-7313-6740","full_name":"Liu, Yu","last_name":"Liu","id":"2A70014E-F248-11E8-B48F-1D18A9856A87"},{"first_name":"Tobias","last_name":"Kleinhanns","full_name":"Kleinhanns, Tobias","id":"8BD9DE16-AB3C-11E9-9C8C-2A03E6697425"},{"id":"BB243B88-D767-11E9-B658-BC13E6697425","orcid":"0000-0002-6962-8598","last_name":"Lee","full_name":"Lee, Seungho","first_name":"Seungho"},{"first_name":"Dmitry N.","last_name":"Dirin","full_name":"Dirin, Dmitry N."},{"full_name":"Akkerman, Quinten A.","last_name":"Akkerman","first_name":"Quinten A."},{"last_name":"Kovalenko","full_name":"Kovalenko, Maksym V.","first_name":"Maksym V."},{"full_name":"Arbiol, Jordi","last_name":"Arbiol","first_name":"Jordi"},{"id":"43C61214-F248-11E8-B48F-1D18A9856A87","last_name":"Ibáñez","full_name":"Ibáñez, Maria","orcid":"0000-0001-5013-2843","first_name":"Maria"}],"publication_status":"published","citation":{"apa":"Calcabrini, M., Genc, A., Liu, Y., Kleinhanns, T., Lee, S., Dirin, D. N., … Ibáñez, M. (2021). Exploiting the lability of metal halide perovskites for doping semiconductor nanocomposites. <i>ACS Energy Letters</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/acsenergylett.0c02448\">https://doi.org/10.1021/acsenergylett.0c02448</a>","ieee":"M. Calcabrini <i>et al.</i>, “Exploiting the lability of metal halide perovskites for doping semiconductor nanocomposites,” <i>ACS Energy Letters</i>, vol. 6, no. 2. American Chemical Society, pp. 581–587, 2021.","chicago":"Calcabrini, Mariano, Aziz Genc, Yu Liu, Tobias Kleinhanns, Seungho Lee, Dmitry N. Dirin, Quinten A. Akkerman, Maksym V. Kovalenko, Jordi Arbiol, and Maria Ibáñez. “Exploiting the Lability of Metal Halide Perovskites for Doping Semiconductor Nanocomposites.” <i>ACS Energy Letters</i>. American Chemical Society, 2021. <a href=\"https://doi.org/10.1021/acsenergylett.0c02448\">https://doi.org/10.1021/acsenergylett.0c02448</a>.","mla":"Calcabrini, Mariano, et al. “Exploiting the Lability of Metal Halide Perovskites for Doping Semiconductor Nanocomposites.” <i>ACS Energy Letters</i>, vol. 6, no. 2, American Chemical Society, 2021, pp. 581–87, doi:<a href=\"https://doi.org/10.1021/acsenergylett.0c02448\">10.1021/acsenergylett.0c02448</a>.","ama":"Calcabrini M, Genc A, Liu Y, et al. Exploiting the lability of metal halide perovskites for doping semiconductor nanocomposites. <i>ACS Energy Letters</i>. 2021;6(2):581-587. doi:<a href=\"https://doi.org/10.1021/acsenergylett.0c02448\">10.1021/acsenergylett.0c02448</a>","short":"M. Calcabrini, A. Genc, Y. Liu, T. Kleinhanns, S. Lee, D.N. Dirin, Q.A. Akkerman, M.V. Kovalenko, J. Arbiol, M. Ibáñez, ACS Energy Letters 6 (2021) 581–587.","ista":"Calcabrini M, Genc A, Liu Y, Kleinhanns T, Lee S, Dirin DN, Akkerman QA, Kovalenko MV, Arbiol J, Ibáñez M. 2021. Exploiting the lability of metal halide perovskites for doping semiconductor nanocomposites. ACS Energy Letters. 6(2), 581–587."},"related_material":{"record":[{"id":"12885","relation":"dissertation_contains","status":"public"}]},"ddc":["540"],"tmp":{"image":"/images/cc_by.png","legal_code_url":"https://creativecommons.org/licenses/by/4.0/legalcode","name":"Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)","short":"CC BY (4.0)"},"isi":1,"external_id":{"isi":["000619803400036"]},"title":"Exploiting the lability of metal halide perovskites for doping semiconductor nanocomposites","year":"2021","doi":"10.1021/acsenergylett.0c02448","ec_funded":1,"issue":"2","publication":"ACS Energy Letters","page":"581-587","file_date_updated":"2021-02-17T07:36:52Z","intvolume":"         6","status":"public","day":"20","type":"journal_article","date_created":"2021-02-14T23:01:14Z","file":[{"checksum":"6fa7374bf8b95fdfe6e6c595322a6689","date_created":"2021-02-17T07:36:52Z","file_size":5071201,"file_name":"2021_ACSEnergyLetters_Calcabrini.pdf","access_level":"open_access","date_updated":"2021-02-17T07:36:52Z","success":1,"file_id":"9155","creator":"dernst","relation":"main_file","content_type":"application/pdf"}],"has_accepted_license":"1","department":[{"_id":"MaIb"}],"publisher":"American Chemical Society","scopus_import":"1","language":[{"iso":"eng"}],"month":"01","article_type":"original","date_published":"2021-01-20T00:00:00Z"}]