Real-Time Observation of “Soft” Magic-Size Clusters during Hydrolysis of the Model Metallodrug Bismuth Disalicylate

Daniel Szczerba; Davin Tan; Jean-Louis Do; Hatem M. Titi; Siham Mouhtadi; Denis Chaumont; Maria del Carmen Marco de Lucas; Nicolas Geoffroy; Michel Meyer; Yoann Rousselin; Jessica M. Hudspeth; Valerie Schwanen; Petra Spörk-Erdely; Ann-Christin Dippel; Oleh Ivashko; Olof Gutowski; Philipp Glaevecke; Vasilii Bazhenov; Mihails Arhangelskis; Ivan Halasz; Tomislav Friscic; Simon A.J. Kimber

doi:10.1021/jacs.1c07186

Real-Time Observation of “Soft” Magic-Size Clusters during Hydrolysis of the Model Metallodrug Bismuth Disalicylate

Daniel Szczerba, Davin Tan, Jean-Louis Do, Hatem M. Titi, Siham Mouhtadi, Denis Chaumont, Maria del Carmen Marco de Lucas, Nicolas Geoffroy, Michel Meyer, Yoann Rousselin, Jessica M. Hudspeth, Valerie Schwanen, Petra Spörk-Erdely, Ann-Christin Dippel, Oleh Ivashko, Olof Gutowski, Philipp Glaevecke, Vasilii Bazhenov, Mihails Arhangelskis, Ivan HalaszTomislav Friscic, Simon A.J. Kimber

Lehrstuhl für Metallkunde (420)

Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Begutachtung

Abstract

Colloidal bismuth therapeutics have been used for hundreds of years, yet remain mysterious. Here we report an X-ray pair distribution function (PDF) study of the solvolysis of bismuth disalicylate, a model for the metallodrug bismuth subsalicylate (Pepto-Bismol). This reveals catalysis by traces of water, followed by multistep cluster growth. The ratio of the two major species, {Bi9O7} and {Bi38O44}, depends on exposure to air, time, and the solvent. The solution-phase cluster structures are of significantly higher symmetry in comparison to solid-state analogues, with reduced off-center Bi3+ displacements. This explains why such "magic-size"clusters can be both stable enough to crystallize and sufficiently labile for further growth.

Originalsprache	Englisch
Seiten (von - bis)	16332-16336
Seitenumfang	5
Fachzeitschrift	Journal of the American Chemical Society
Jahrgang	143.2021
Ausgabenummer	40
Frühes Online-Datum	28 Sept. 2021
DOIs	https://doi.org/10.1021/jacs.1c07186
Publikationsstatus	Veröffentlicht - 13 Okt. 2021

Bibliographische Notiz

Funding Information:
We acknowledge the European Synchrotron Radiation Facility for provision of synchrotron beam time on ID15B. We acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at P21.1. We thank Sakura Pascarelli for her kind help in Hamburg and the staff of ID15 at the ESRF for assistance with consumables. Agnieszka Poulain is acknowledged for support on the beamline. V.S. and P.S.-E. were funded by the ESRF-ILL International Summer Student Program. This work was supported by the EIPHI Graduate School (contract ANR-17-EURE-0002). Ce travail a été soutenu par le programme ”Investissements d’Avenir”, ISITE-BFC project (contract ANR- 15-IDEX-0003). We thank Agnès Birot for administrative support.

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Szczerba, D., Tan, D., Do, J.-L., Titi, H. M., Mouhtadi, S., Chaumont, D., Marco de Lucas, M. D. C., Geoffroy, N., Meyer, M., Rousselin, Y., Hudspeth, J. M., Schwanen, V., Spörk-Erdely, P., Dippel, A.-C., Ivashko, O., Gutowski, O., Glaevecke, P., Bazhenov, V., Arhangelskis, M., ... Kimber, S. A. J. (2021). Real-Time Observation of “Soft” Magic-Size Clusters during Hydrolysis of the Model Metallodrug Bismuth Disalicylate. Journal of the American Chemical Society, 143.2021(40), 16332-16336. https://doi.org/10.1021/jacs.1c07186

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abstract = "Colloidal bismuth therapeutics have been used for hundreds of years, yet remain mysterious. Here we report an X-ray pair distribution function (PDF) study of the solvolysis of bismuth disalicylate, a model for the metallodrug bismuth subsalicylate (Pepto-Bismol). This reveals catalysis by traces of water, followed by multistep cluster growth. The ratio of the two major species, {Bi9O7} and {Bi38O44}, depends on exposure to air, time, and the solvent. The solution-phase cluster structures are of significantly higher symmetry in comparison to solid-state analogues, with reduced off-center Bi3+ displacements. This explains why such {"}magic-size{"}clusters can be both stable enough to crystallize and sufficiently labile for further growth.",

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Szczerba, D, Tan, D, Do, J-L, Titi, HM, Mouhtadi, S, Chaumont, D, Marco de Lucas, MDC, Geoffroy, N, Meyer, M, Rousselin, Y, Hudspeth, JM, Schwanen, V, Spörk-Erdely, P, Dippel, A-C, Ivashko, O, Gutowski, O, Glaevecke, P, Bazhenov, V, Arhangelskis, M, Halasz, I, Friscic, T & Kimber, SAJ 2021, 'Real-Time Observation of “Soft” Magic-Size Clusters during Hydrolysis of the Model Metallodrug Bismuth Disalicylate', Journal of the American Chemical Society, Jg. 143.2021, Nr. 40, S. 16332-16336. https://doi.org/10.1021/jacs.1c07186

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AU - Mouhtadi, Siham

AU - Chaumont, Denis

AU - Marco de Lucas, Maria del Carmen

AU - Geoffroy, Nicolas

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AU - Rousselin, Yoann

AU - Hudspeth, Jessica M.

AU - Schwanen, Valerie

AU - Spörk-Erdely, Petra

AU - Dippel, Ann-Christin

AU - Ivashko, Oleh

AU - Gutowski, Olof

AU - Glaevecke, Philipp

AU - Bazhenov, Vasilii

AU - Arhangelskis, Mihails

AU - Halasz, Ivan

AU - Friscic, Tomislav

AU - Kimber, Simon A.J.

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