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Proving Cooperativity of a Catalytic Reaction by Means of Nanoscale Geometry: The Case of Click Reaction

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Title
Proving Cooperativity of a Catalytic Reaction by Means of Nanoscale Geometry: The Case of Click Reaction
Author(s)
Cristóbal Quintana; Juan C. Ahumada; Guillermo Ahumada; Yaroslav Sobolev; Minju Kim; Atabay Allamyradov; Bartosz A. Grzybowski
Publication Date
2022-06
Journal
Journal of the American Chemical Society, v.144, no.25, pp.11238 - 11245
Publisher
NLM (Medline)
Abstract
Establishing whether a reaction is catalyzed by a single-metal catalytic center or cooperatively by a fleeting complex encompassing two such centers may be an arduous pursuit requiring detailed kinetic, isotopic, and other types of studies─as illustrated, for instance, by over a decade-long work on single-copper versus di-copper mechanisms of the popular click reaction. This paper describes a method to interrogate such cooperative mechanisms by a nanoparticle-based platform in which the probabilities of catalytic units being proximal can be varied systematically and, more importantly, independently of their volume concentration. The method relies on geometrical considerations rather than a detailed knowledge of kinetic equations, yet the scaling trends it yield can distinguish between cooperative and non-cooperative mechanisms.
URI
https://pr.ibs.re.kr/handle/8788114/12917
DOI
10.1021/jacs.2c02556
ISSN
0002-7863
Appears in Collections:
Center for Soft and Living Matter(첨단연성물질 연구단) > 1. Journal Papers (저널논문)
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