4.8 Article

Interplay between oxygen doping and ultra-microporosity improves the CO2/N2 separation performance of carbons derived from aromatic polycarboxylates

Journal

CARBON
Volume 173, Issue -, Pages 989-1002

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.carbon.2020.11.080

Keywords

Porous carbons; Carbon capture; Ultra-microporosity; Oxygen doping

Funding

  1. European Union [663830]
  2. Reduce Industrial Carbon Emissions (RICE)
  3. Flexible Integrated Energy Systems (FLEXIS) - EU's European Regional Development Fund through the Welsh Government
  4. EPSRC [EP/M028267/1]
  5. European Regional Development Fund through the Welsh Government [80708]
  6. Welsh Government
  7. EPSRC [EP/M028267/1] Funding Source: UKRI

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Highly microporous carbons were prepared through two facile synthetic strategies, achieving diverse morphologies, textural properties, and oxygen contents, with assessed CO2 and N-2 sorption properties. The study found that at low pressure, the simultaneous presence of large ultra-micropore volume and high oxygen content in the sorbents contributed to competitive CO2 uptake and CO2/N-2 selectivity, suggesting the importance of interplay between ultra-microporosity and oxygen doping in determining CO2/N-2 separation properties.
Microporous carbons were prepared starting from a series of benzene polycarboxylic acids following two strategies: (i) activation- and template-free pyrolysis and (ii) ion-exchange pyrolysis. The proposed synthetic strategies are facile approaches to produce highly microporous carbons that avoid the use of large amounts of corrosive and expensive chemical activators or templates. By varying the number of carboxylic acid groups, the charge balancing species and the degree of deprotonation of the precursors, microporous carbons with diverse morphologies, textural properties and oxygen contents were obtained and their CO2 and N-2 sorption properties were assessed. The abundant micropores made the materials suitable for CO2 adsorption at low pressure and ambient temperature, achieving CO2 uptake as high as 4.4 mmol g(-1) at 25 degrees C and 1 bar, competitive with those reported for porous carbons produced using large excess of alkali metal based activating agents. It was found that high performance, in terms of CO2 uptake and CO2/N-2 selectivity, was linked to the simultaneous presence of large ultra-micropore volume and high oxygen content in the sorbents. This suggests that the interplay of ultra-microporosity and oxygen doping matters more than the two features taken singularly in determining the CO2/N-2 separation properties of porous carbons at low pressure. (C) 2020 Elsevier Ltd. All rights reserved.

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