Charge-modulated CO2 capture

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Recently, the concept of using charge-modulation to manipulate the interaction of adsorbate molecules such as CO2 on certain sorbent materials has been advanced through a series of first principle computational predictions. The interactions switched on through charge-modulation shifting the Fermi level are in part, but by no means exclusively, electrostatic. In addition to electrostatics, the Fermi level shifting can be viewed as a way to modulate not only the position but also the identity and character of the frontier orbitals on the sorbent materials that engage with the adsorbate molecules. Thus, a rich new space for electrochemical modulation of surface-molecular interactions—guided by first principle computational modeling—suggests itself. Here we summarize the growing computational literature on switchable CO2 capture strategies. We also provide some new insights into contrasting electrostatic versus chemical responses to charge-modulation as exemplified by water versus CO2 on N-doped graphene surfaces, which suggest that this CO2 capture strategy could be water tolerant.