Electrocatalytically switchable CO2 capture: first principle computational exploration of carbon nanotubes with pyridinic nitrogen

ChemSusChem. 2014 Feb;7(2):435-41. doi: 10.1002/cssc.201300624.

Abstract

Carbon nanotubes with specific nitrogen doping are proposed for controllable, highly selective, and reversible CO2 capture. Using density functional theory incorporating long-range dispersion corrections, we investigated the adsorption behavior of CO2 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 CO2 adsorption strength with electron injecting, leading to a highly selective CO2 adsorption in comparison with N2 . This functionality could induce intrinsically reversible CO2 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 CO2 -capture phenomenon is considered.

Keywords: co2 capture; density functional theory; nanocarbon functionalization; nanostructures; nanotubes.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Adsorption
  • Carbon Dioxide / chemistry*
  • Computer Simulation
  • Conservation of Energy Resources
  • Electrochemistry
  • Models, Molecular*
  • Molecular Conformation
  • Nanotubes, Carbon / chemistry*
  • Nitrogen / chemistry*
  • Pyridines / chemistry*

Substances

  • Nanotubes, Carbon
  • Pyridines
  • Carbon Dioxide
  • Nitrogen
  • pyridine