Feedback Kinetics in Mechanochemistry: The Importance of Cohesive States

Benjamin Hutchings, Deborah Crawford, Lei Gao, Peijun Hu, Stuart James

Research output: Contribution to journalArticle

34 Citations (Scopus)
207 Downloads (Pure)

Abstract

Although mechanochemical synthesis is becoming more widely applied and even commercialised, greater basic understanding is needed if the field is to progress on less of a trial-and-error basis. We report that a mechanochemical reaction in a ball mill exhibits unusual sigmoidal feedback kinetics that differ dramatically from the simple first-order kinetics for the same reaction in solution. An induction period is followed by a rapid increase in reaction rate before the rate decreases again as the reaction goes to completion. The origin of these unusual kinetics is found to be a feedback cycle involving both chemical and mechanical factors. During the reaction the physical form of the reaction mixture changes from a powder to a cohesive rubber-like state, and this results in the observed reaction rate increase. The study reveals that non-obvious and dynamic rheological changes in the reaction mixture must be appreciated to understand how mechanochemical reactions progress.
Original languageEnglish
Pages (from-to)15252–15256
JournalAngewandte Chemie International Edition
Volume56
Issue number48
Early online date30 Oct 2017
DOIs
Publication statusPublished - 27 Nov 2017

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