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Stalcup, Matthew A.; Nilles, Christian K.; Subramaniam, Bala; Blakemore, James D.; Leonard, Kevin C. (, Chemical Communications)We shed light on the mechanism and rate-determining steps of the electrochemical carboxylation of acetophenone as a function of CO 2 concentration by using a robust finite element analysis model that incorporates each reaction step. Specifically, we show that the first electrochemical reduction of acetophenone is followed by the homogeneous chemical addition of CO 2 . The electrochemical reduction of the acetophenone-CO 2 adduct is more facile than that of acetophenone, resulting in an Electrochemical–Chemical–Electrochemical (ECE) reaction pathway that appears as a single voltammetric wave. These modeling results provide new fundamental insights into the complex microenvironment in CO 2 -rich media that produces an optimum electrochemical carboxylation rate as a function of CO 2 pressure.more » « less
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Stalcup, Matthew A.; Nilles, Christian K.; Lee, Hyun-Jin; Subramaniam, Bala; Blakemore, James D.; Leonard, Kevin C. (, ACS Sustainable Chemistry & Engineering)null (Ed.)
