Electrocatalytically Switchable CO 2 Capture: First Principle Computational Exploration of Carbon Nanotubes with Pyridinic Nitrogen

Carbon nanotubes with specific nitrogen doping are proposed for controllable, highly selective, and reversible CO 2 capture. Using density functional theory incorporating long‐range dispersion corrections, we investigated the adsorption behavior of CO 2 on (7,7) single‐walled carbon nanotubes (CNTs) with several nitrogen doping configurations and varying charge states. Pyridinic‐nitrogen incorporation in CNTs is found to induce an increasing CO 2 adsorption strength with electron injecting, leading to a highly selective CO 2 adsorption in comparison with N 2 . This functionality could induce intrinsically reversible CO 2 adsorption as capture/release can be controlled by switching the charge carrying state of the system on/off. This phenomenon is verified for a number of different models and theoretical methods, with clear ramifications for the possibility of implementation with a broader class of graphene‐based materials. A scheme for the implementation of this remarkable reversible electrocatalytic CO 2 ‐capture phenomenon is considered.