أعرض في EDS

Quantification of Active Site Density and Turnover Frequency: From Single-Atom Metal to Nanoparticle Electrocatalysts

التفاصيل البيبلوغرافية
العنوان: Quantification of Active Site Density and Turnover Frequency: From Single-Atom Metal to Nanoparticle Electrocatalysts
المؤلفون: Kug-Seung Lee, Hyung Suk Oh, Frédéric Jaouen, Han Chang Kwon, Pyeonghwa Jeong, Hansol Choi, Donghyun Kim, Haesol Kim, Geunsu Bae, Chang Hyuck Choi, Minkee Choi
المصدر: JACS Au, Vol 1, Iss 5, Pp 586-597 (2021)
JACS Au
بيانات النشر: American Chemical Society (ACS), 2021.
سنة النشر: 2021
مصطلحات موضوعية: Cyanide, Inorganic chemistry, Nanoparticle, chemistry.chemical_element, engineering.material, Article, Catalysis, Metal, Fe−N−C catalysts, chemistry.chemical_compound, Adsorption, QD1-999, oxygen reduction reaction, biology, Chemistry, turnover frequency, Active site, visual_art, engineering, biology.protein, visual_art.visual_art_medium, Noble metal, Platinum, active site density, Single-atom catalysts
الوصف: Single-atom catalysts (SACs) featuring atomically dispersed metal cations covalently embedded in a carbon matrix show significant potential to achieve high catalytic performance in various electrocatalytic reactions. Although considerable advances have been achieved in their syntheses and electrochemical applications, further development and fundamental understanding are limited by a lack of strategies that can allow the quantitative analyses of their intrinsic catalytic characteristics, that is, active site density (SD) and turnover frequency (TOF). Here we show an in situ SD quantification method using a cyanide anion as a probe molecule. The decrease in cyanide concentration triggered by irreversible adsorption on metal-based active sites of a model Fe-N-C catalyst is precisely measured by spectrophotometry, and it is correlated to the relative decrease in electrocatalytic activity in the model reaction of oxygen reduction reaction. The linear correlation verifies the surface-sensitive and metal-specific adsorption of cyanide on Fe-N x sites, based on which the values of SD and TOF can be determined. Notably, this analytical strategy shows versatile applicability to a series of transition/noble metal SACs and Pt nanoparticles in a broad pH range (1-13). The SD and TOF quantification can afford an improved understanding of the structure-activity relationship for a broad range of electrocatalysts, in particular, the SACs, for which no general electrochemical method to determine the intrinsic catalytic characteristics is available.
تدمد: 2691-3704
URL الوصول: https://explore.openaire.eu/search/publication?articleId=doi_dedup___::771bca7223a9cae4c1570e5421ffbfc3
https://doi.org/10.1021/jacsau.1c00074
حقوق: OPEN
رقم الأكسشن: edsair.doi.dedup.....771bca7223a9cae4c1570e5421ffbfc3
قاعدة البيانات: OpenAIRE
الوصف
تدمد:26913704