[{"doi":"10.1002/ange.202219314","day":"02","abstract":[{"text":"Aromatische Seitenketten sind wichtige Indikatoren für die Plastizität von Proteinen und bilden oft entscheidende Kontakte bei Protein‐Protein‐Wechselwirkungen. Wir untersuchten aromatische Reste in den beiden strukturell homologen cross‐β Amyloidfibrillen HET‐s und HELLF mit Hilfe eines spezifischen Ansatzes zur Isotopenmarkierung und Festkörper NMR mit Drehung am magischen Winkel. Das dynamische Verhalten der aromatischen Reste Phe und Tyr deutet darauf hin, dass der hydrophobe Amyloidkern starr ist und keine Anzeichen von “atmenden Bewegungen” auf einer Zeitskala von Hunderten von Millisekunden zeigt. Aromatische Reste, die exponiert an der Fibrillenoberfläche sitzen, haben zwar eine starre Ringachse, weisen aber Ringflips auf verschiedenen Zeitskalen von Nanosekunden bis Mikrosekunden auf. Unser Ansatz bietet einen direkten Einblick in die Bewegungen des hydrophoben Kerns und ermöglicht eine bessere Bewertung der Konformationsheterogenität, die aus einem NMR‐Strukturensemble einer solchen Cross‐β‐Amyloidstruktur hervorgeht.","lang":"ger"}],"date_updated":"2024-01-23T12:23:35Z","citation":{"mla":"Becker, Lea Marie, et al. “Der starre Kern und die flexible Oberfläche von Amyloidfibrillen – Magic‐Angle‐Spinning NMR Spektroskopie von aromatischen Resten.” <i>Angewandte Chemie</i>, vol. 135, no. 19, e202219314, Wiley, 2023, doi:<a href=\"https://doi.org/10.1002/ange.202219314\">10.1002/ange.202219314</a>.","short":"L.M. Becker, M. Berbon, A. Vallet, A. Grelard, E. Morvan, B. Bardiaux, R. Lichtenecker, M. Ernst, A. Loquet, P. Schanda, Angewandte Chemie 135 (2023).","ista":"Becker LM, Berbon M, Vallet A, Grelard A, Morvan E, Bardiaux B, Lichtenecker R, Ernst M, Loquet A, Schanda P. 2023. Der starre Kern und die flexible Oberfläche von Amyloidfibrillen – Magic‐Angle‐Spinning NMR Spektroskopie von aromatischen Resten. Angewandte Chemie. 135(19), e202219314.","apa":"Becker, L. M., Berbon, M., Vallet, A., Grelard, A., Morvan, E., Bardiaux, B., … Schanda, P. (2023). Der starre Kern und die flexible Oberfläche von Amyloidfibrillen – Magic‐Angle‐Spinning NMR Spektroskopie von aromatischen Resten. <i>Angewandte Chemie</i>. Wiley. <a href=\"https://doi.org/10.1002/ange.202219314\">https://doi.org/10.1002/ange.202219314</a>","ama":"Becker LM, Berbon M, Vallet A, et al. Der starre Kern und die flexible Oberfläche von Amyloidfibrillen – Magic‐Angle‐Spinning NMR Spektroskopie von aromatischen Resten. <i>Angewandte Chemie</i>. 2023;135(19). doi:<a href=\"https://doi.org/10.1002/ange.202219314\">10.1002/ange.202219314</a>","ieee":"L. M. Becker <i>et al.</i>, “Der starre Kern und die flexible Oberfläche von Amyloidfibrillen – Magic‐Angle‐Spinning NMR Spektroskopie von aromatischen Resten,” <i>Angewandte Chemie</i>, vol. 135, no. 19. Wiley, 2023.","chicago":"Becker, Lea Marie, Mélanie Berbon, Alicia Vallet, Axelle Grelard, Estelle Morvan, Benjamin Bardiaux, Roman Lichtenecker, Matthias Ernst, Antoine Loquet, and Paul Schanda. “Der starre Kern und die flexible Oberfläche von Amyloidfibrillen – Magic‐Angle‐Spinning NMR Spektroskopie von aromatischen Resten.” <i>Angewandte Chemie</i>. Wiley, 2023. <a href=\"https://doi.org/10.1002/ange.202219314\">https://doi.org/10.1002/ange.202219314</a>."},"year":"2023","volume":135,"acknowledgement":"Wir danken Albert A. Smith (Leipzig) für aufschlussreiche Diskussionen. Diese Arbeit wurde mit Mitteln des Europäischen Forschungsrats (StG-2012-311318 an P.S.) unterstützt und nutzte die Plattformen des Grenoble Instruct-ERIC Center (ISBG; UMS 3518 CNRS-CEA-UJF-EMBL) im Rahmen der Grenoble Partnership for Structural Biology (PSB) sowie die Einrichtungen und das Fachwissen der Biophysical and Structural Chemistry Platform (BPCS) am IECB, CNRS UAR3033, INSERM US001 und der Universität Bordeaux.","ddc":["540"],"publication_status":"published","department":[{"_id":"PaSc"}],"article_processing_charge":"Yes (in subscription journal)","date_created":"2024-01-18T10:01:01Z","title":"Der starre Kern und die flexible Oberfläche von Amyloidfibrillen – Magic‐Angle‐Spinning NMR Spektroskopie von aromatischen Resten","intvolume":"       135","_id":"14835","license":"https://creativecommons.org/licenses/by-nc/4.0/","author":[{"id":"36336939-eb97-11eb-a6c2-c83f1214ca79","full_name":"Becker, Lea Marie","orcid":"0000-0002-6401-5151","last_name":"Becker","first_name":"Lea Marie"},{"full_name":"Berbon, Mélanie","first_name":"Mélanie","last_name":"Berbon"},{"full_name":"Vallet, Alicia","first_name":"Alicia","last_name":"Vallet"},{"last_name":"Grelard","first_name":"Axelle","full_name":"Grelard, Axelle"},{"full_name":"Morvan, Estelle","first_name":"Estelle","last_name":"Morvan"},{"last_name":"Bardiaux","first_name":"Benjamin","full_name":"Bardiaux, Benjamin"},{"first_name":"Roman","last_name":"Lichtenecker","full_name":"Lichtenecker, Roman"},{"first_name":"Matthias","last_name":"Ernst","full_name":"Ernst, Matthias"},{"full_name":"Loquet, Antoine","last_name":"Loquet","first_name":"Antoine"},{"id":"7B541462-FAF6-11E9-A490-E8DFE5697425","full_name":"Schanda, Paul","orcid":"0000-0002-9350-7606","last_name":"Schanda","first_name":"Paul"}],"issue":"19","publisher":"Wiley","article_type":"original","quality_controlled":"1","file_date_updated":"2024-01-23T08:57:01Z","publication_identifier":{"eissn":["1521-3757"],"issn":["0044-8249"]},"oa":1,"tmp":{"name":"Creative Commons Attribution-NonCommercial 4.0 International (CC BY-NC 4.0)","image":"/images/cc_by_nc.png","short":"CC BY-NC (4.0)","legal_code_url":"https://creativecommons.org/licenses/by-nc/4.0/legalcode"},"date_published":"2023-05-02T00:00:00Z","type":"journal_article","file":[{"access_level":"open_access","relation":"main_file","success":1,"creator":"dernst","file_id":"14876","file_size":1004676,"checksum":"98e68d370159f7be52a3d7c8a8ee1198","date_created":"2024-01-23T08:57:01Z","file_name":"2023_AngewChem_Becker.pdf","content_type":"application/pdf","date_updated":"2024-01-23T08:57:01Z"}],"user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","status":"public","oa_version":"Published Version","month":"05","article_number":"e202219314","publication":"Angewandte Chemie","has_accepted_license":"1","language":[{"iso":"ger"}],"keyword":["General Medicine"]},{"ddc":["540","541"],"volume":132,"year":"2020","citation":{"ista":"Bouchal R, Li Z, Bongu C, Le Vot S, Berthelot R, Rotenberg B, Favier F, Freunberger SA, Salanne M, Fontaine O. 2020. Competitive salt precipitation/dissolution during free‐water reduction in water‐in‐salt electrolyte. Angewandte Chemie. 132(37), 16047–16051.","mla":"Bouchal, Roza, et al. “Competitive Salt Precipitation/Dissolution during Free‐water Reduction in Water‐in‐salt Electrolyte.” <i>Angewandte Chemie</i>, vol. 132, no. 37, Wiley, 2020, pp. 16047–51, doi:<a href=\"https://doi.org/10.1002/ange.202005378\">10.1002/ange.202005378</a>.","short":"R. Bouchal, Z. Li, C. Bongu, S. Le Vot, R. Berthelot, B. Rotenberg, F. Favier, S.A. Freunberger, M. Salanne, O. Fontaine, Angewandte Chemie 132 (2020) 16047–16051.","chicago":"Bouchal, Roza, Zhujie Li, Chandra Bongu, Steven Le Vot, Romain Berthelot, Benjamin Rotenberg, Frederic Favier, Stefan Alexander Freunberger, Mathieu Salanne, and Olivier Fontaine. “Competitive Salt Precipitation/Dissolution during Free‐water Reduction in Water‐in‐salt Electrolyte.” <i>Angewandte Chemie</i>. Wiley, 2020. <a href=\"https://doi.org/10.1002/ange.202005378\">https://doi.org/10.1002/ange.202005378</a>.","ieee":"R. Bouchal <i>et al.</i>, “Competitive salt precipitation/dissolution during free‐water reduction in water‐in‐salt electrolyte,” <i>Angewandte Chemie</i>, vol. 132, no. 37. Wiley, pp. 16047–16051, 2020.","apa":"Bouchal, R., Li, Z., Bongu, C., Le Vot, S., Berthelot, R., Rotenberg, B., … Fontaine, O. (2020). Competitive salt precipitation/dissolution during free‐water reduction in water‐in‐salt electrolyte. <i>Angewandte Chemie</i>. Wiley. <a href=\"https://doi.org/10.1002/ange.202005378\">https://doi.org/10.1002/ange.202005378</a>","ama":"Bouchal R, Li Z, Bongu C, et al. Competitive salt precipitation/dissolution during free‐water reduction in water‐in‐salt electrolyte. <i>Angewandte Chemie</i>. 2020;132(37):16047-16051. doi:<a href=\"https://doi.org/10.1002/ange.202005378\">10.1002/ange.202005378</a>"},"date_updated":"2023-09-05T15:47:50Z","abstract":[{"lang":"eng","text":"Water-in-salt electrolytes based on highly concentrated bis(trifluoromethyl)sulfonimide (TFSI) promise aqueous electrolytes with stabilities approaching 3 V. However, especially with an electrode approaching the cathodic (reductive) stability, cycling stability is insufficient. While stability critically relies on a solid electrolyte interphase (SEI), the mechanism behind the cathodic stability limit remains unclear. Here, we reveal two distinct reduction potentials for the chemical environments of ‘free’ and ‘bound’ water and that both contribute to SEI formation. Free-water is reduced ~1V above bound water in a hydrogen evolution reaction (HER) and responsible for SEI formation via reactive intermediates of the HER; concurrent LiTFSI precipitation/dissolution establishes a dynamic interface. The free-water population emerges, therefore, as the handle to extend the cathodic limit of aqueous electrolytes and the battery cycling stability."}],"day":"07","doi":"10.1002/ange.202005378","file_date_updated":"2020-09-17T08:59:43Z","quality_controlled":"1","page":"16047-16051","article_type":"original","publisher":"Wiley","issue":"37","author":[{"full_name":"Bouchal, Roza","first_name":"Roza","last_name":"Bouchal"},{"full_name":"Li, Zhujie","first_name":"Zhujie","last_name":"Li"},{"last_name":"Bongu","first_name":"Chandra","full_name":"Bongu, Chandra"},{"last_name":"Le Vot","first_name":"Steven","full_name":"Le Vot, Steven"},{"full_name":"Berthelot, Romain","first_name":"Romain","last_name":"Berthelot"},{"full_name":"Rotenberg, Benjamin","last_name":"Rotenberg","first_name":"Benjamin"},{"first_name":"Frederic","last_name":"Favier","full_name":"Favier, Frederic"},{"orcid":"0000-0003-2902-5319","full_name":"Freunberger, Stefan Alexander","first_name":"Stefan Alexander","last_name":"Freunberger","id":"A8CA28E6-CE23-11E9-AD2D-EC27E6697425"},{"full_name":"Salanne, Mathieu","first_name":"Mathieu","last_name":"Salanne"},{"full_name":"Fontaine, Olivier","last_name":"Fontaine","first_name":"Olivier"}],"scopus_import":"1","_id":"8057","intvolume":"       132","title":"Competitive salt precipitation/dissolution during free‐water reduction in water‐in‐salt electrolyte","department":[{"_id":"StFr"}],"article_processing_charge":"No","date_created":"2020-06-29T16:15:49Z","publication_status":"published","status":"public","user_id":"c635000d-4b10-11ee-a964-aac5a93f6ac1","file":[{"file_id":"8401","creator":"dernst","success":1,"access_level":"open_access","relation":"main_file","date_updated":"2020-09-17T08:59:43Z","content_type":"application/pdf","file_name":"2020_AngChemieDE_Bouchal.pdf","date_created":"2020-09-17T08:59:43Z","checksum":"7dd0a56f6bd5de08ea75b1ec388c91bc","file_size":1904552}],"type":"journal_article","date_published":"2020-09-07T00:00:00Z","tmp":{"legal_code_url":"https://creativecommons.org/licenses/by/4.0/legalcode","short":"CC BY (4.0)","image":"/images/cc_by.png","name":"Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)"},"oa":1,"publication_identifier":{"issn":["0044-8249"],"eissn":["1521-3757"]},"language":[{"iso":"eng"}],"has_accepted_license":"1","publication":"Angewandte Chemie","month":"09","oa_version":"Published Version"}]