EELS Studies of Cerium Electrolyte Reveal Substantial Solute Concentration Effects in Graphene Liquid Cells.

التفاصيل البيبلوغرافية
العنوان:	EELS Studies of Cerium Electrolyte Reveal Substantial Solute Concentration Effects in Graphene Liquid Cells.
المؤلفون:	Crook MF; Department of Chemistry, University of California, Berkeley, California 94720, United States., Moreno-Hernandez IA; Department of Chemistry, University of California, Berkeley, California 94720, United States., Ondry JC; Department of Chemistry, University of California, Berkeley, California 94720, United States.; Kavli Energy NanoScience Institute, Berkeley, California 94720, United States., Ciston J; National Center for Electron Microscopy Facility, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States., Bustillo KC; National Center for Electron Microscopy Facility, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States., Vargas A; Department of Chemical and Biomolecular Engineering, University of California, Berkeley, California 94720, United States., Alivisatos AP; Department of Chemistry, University of California, Berkeley, California 94720, United States.; Kavli Energy NanoScience Institute, Berkeley, California 94720, United States.; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.; Department of Materials Science and Engineering, University of California, Berkeley, California 94720, United States.
المصدر:	Journal of the American Chemical Society [J Am Chem Soc] 2023 Mar 29; Vol. 145 (12), pp. 6648-6657. Date of Electronic Publication: 2023 Mar 20.
نوع المنشور:	Journal Article
اللغة:	English
بيانات الدورية:	Publisher: American Chemical Society Country of Publication: United States NLM ID: 7503056 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1520-5126 (Electronic) Linking ISSN: 00027863 NLM ISO Abbreviation: J Am Chem Soc Subsets: PubMed not MEDLINE; MEDLINE
أسماء مطبوعة:	Publication: Washington, DC : American Chemical Society Original Publication: Easton, Pa. [etc.]
مستخلص:	Graphene liquid cell transmission electron microscopy is a powerful technique to visualize nanoscale dynamics and transformations at atomic resolution. However, the solution in liquid cells is known to be affected by radiolysis, and the stochastic formation of graphene liquid cells raises questions about the solution chemistry in individual pockets. In this study, electron energy loss spectroscopy (EELS) was used to evaluate a model encapsulated solution, aqueous CeCl 3 . First, the ratio between the O K-edge and Ce M-edge was used to approximate the concentration of cerium salt in the graphene liquid cell. It was determined that the ratio between oxygen and cerium was orders of magnitude lower than what is expected for a dilute solution, indicating that the encapsulated solution is highly concentrated. To probe how this affects the chemistry within graphene liquid cells, the oxidation of Ce ³⁺ was measured using time-resolved parallel EELS. It was determined that Ce ³⁺ oxidizes faster under high electron fluxes, but reaches the same steady-state Ce ⁴⁺ concentration regardless of flux. The time-resolved concentration profiles enabled direct comparison to radiolysis models, which indicate rate constants and g -values of certain molecular species are substantially different in the highly concentrated environment. Finally, electron flux-dependent gold nanocrystal etching trajectories showed that gold nanocrystals etch faster at higher electron fluxes, correlating well with the Ce ³⁺ oxidation kinetics. Understanding the effects of the highly concentrated solution in graphene liquid cells will provide new insight on previous studies and may open up opportunities to systematically study systems in highly concentrated solutions at high resolution.
تواريخ الأحداث:	Date Created: 20230320 Date Completed: 20230329 Latest Revision: 20230329
رمز التحديث:	20240628
DOI:	10.1021/jacs.2c07778
PMID:	36939571
قاعدة البيانات:	MEDLINE

Find this issue from the American Chemical Society

الوصف
تدمد:	1520-5126
DOI:	10.1021/jacs.2c07778