Quantification of Active Site Density and Turnover Frequency: From Single-Atom Metal to Nanoparticle Electrocatalysts
العنوان: | Quantification of Active Site Density and Turnover Frequency: From Single-Atom Metal to Nanoparticle Electrocatalysts |
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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 |
تدمد: | 26913704 |
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