In this paper, nitrogen and sulfur co-doped carbon nanotubes composites were prepared by coal pyrolysis with the aim of applying them to carbon dioxide adsorption. Compared with previous carbon nanotubes modification methods, this study increased the specific surface area, microporosity and the number of adsorption sites of the materials through structural modification and surface modification, thus improving the adsorption capacity. Notably, secondary KOH activation modification was employed to increase the N and S elemental content in the adsorbent. Without leading to the loss of specific surface area, the specific surface area after modification was increased by 29% to 1875 m2/g, and the N content in the adsorbent could be reasonably regulated. The IAST calculations revealed that the prepared adsorbent had a high selectivity for CO2/N2 in binary gas mixtures, which is of practical significance for the treatment of flue gas streams. In addition, the isocratic heat of adsorption of the adsorbent was calculated to be less than 40kJ/mol using the Clasius-Clapeyron equation, which indicates that the adsorbent is easy to desorb and can be used several times. After five consecutive CO2 adsorption experiments, the adsorbent retained 98.22% of its CO2 adsorption capacity. Overall, this study not only provides a new idea for the high value-added utilization of low-rank bituminous coal. It also provides an important reference for the large-scale doping of N and S elements in coal-based carbon materials, which has certain theoretical and applied values.
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