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Good electrical conductivity and high electron mobility of the sorbent materials are prerequisite for electrocatalytically switchable CO 2  capture. However, no conductive and easily synthetic sorbent materials are available until now. Here, we examined the possibility of conductive graphitic carbon nitride (g-C 4 N 3 ) nanosheets as sorbent materials for electrocatalytically switchable CO 2  capture. Using first-principle calculations, we found that the adsorption energy of CO 2  molecules on g-C 4 N 3  nanosheets can be dramatically enhanced by injecting extra electrons into the adsorbent. At saturation CO 2  capture coverage, the negatively charged g-C 4 N 3  nanosheets achieve CO 2  capture capacities up to 73.9 × 10 13  cm −2  or 42.3 wt%. In contrast to other CO 2  capture approaches, the process of CO 2  capture/release occurs spontaneously without any energy barriers once extra electrons are introduced or removed, and these processes can be simply controlled and reversed by switching on/off the charging voltage. In addition, these negatively charged g-C 4 N 3  nanosheets are highly selective for separating CO 2  from mixtures with CH 4 , H 2  and/or N 2 . These predictions may prove to be instrumental in searching for a new class of experimentally feasible high-capacity CO 2  capture materials with ideal thermodynamics and reversibility.

Conductive Graphitic Carbon Nitride as an Ideal Material for Electrocatalytically Switchable CO2 Capture