Efficient carboxylation of styrene and carbon dioxide by single-atomic copper electrocatalyst.

[Display omitted] Electrocarboxylation of olefins with carbon dioxide (CO 2) is a potential approach to produce carboxylates as synthetic intermediates of polymer and pharmaceuticals. Nonetheless, due to the intrinsic inertness of CO 2 at ambient conditions, the electrocarboxylation efficiency has been quite limited, typically with high applied potentials and low current densities. In this work, we demonstrate that nitrogen-coordinated single-atomic copper sites on carbon framework (Cu/N C) served as an excellent electrocatalyst for electrocarboxylation of styrene with CO 2. The Cu/N C catalyst allowed to efficiently activate CO 2 , followed by nucleophilic attack to carboxylate styrene to produce phenylsuccinic acid, thus leading the reaction toward the CO 2 activation pathway. The enhanced CO 2 activation capability enabled increased selectivity and activity for electrocarboxylation of styrene. The Faradaic efficiency of electrocarboxylation was 92%, suggesting most of the activated CO 2 proceeded to react with styrene rather than direct reduction to CO or CH 4. The electrocarboxylation exhibited almost 100% product selectivity toward phenylsuccinic acid, with a high partial current density of 58 mA·cm−2 at −2.2 V (vs. Ag/AgI), corresponding to an outstanding production rate of 216 mg·cm−2·h−1, substantially exceeding previously reported works. Our work suggests an exciting perspective in electrocarboxylation of olefins by rational design of CO 2 activation electrocatalysts. [ABSTRACT FROM AUTHOR]