SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2022, Vol. 42 ›› Issue (2): 104-111.DOI: 10.1016/j.cjche.2021.07.010

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Light-responsive adsorbents with tunable adsorbent-adsorbate interactions for selective CO2 capture

Peng Tan1, Yao Jiang1, Qiurong Wu1, Chen Gu1, Shichao Qi1, Qiang Zhang2, Xiaoqin Liu1, Linbing Sun1   

  1. 1. State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China;
    2. Department of Chemistry, Washington State University, Pullman, WA 99163, United States
  • Received:2021-05-18 Revised:2021-07-14 Online:2022-03-30 Published:2022-02-28
  • Contact: Linbing Sun,E-mail:lbsun@njtech.edu.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (22078155, 21808110, 21878149, and 21676138), and China Postdoctoral Science Foundation (2020M681567). We are also grateful to the High Performance Computing Center of Nanjing Tech University for supporting the computational resources.

Light-responsive adsorbents with tunable adsorbent-adsorbate interactions for selective CO2 capture

Peng Tan1, Yao Jiang1, Qiurong Wu1, Chen Gu1, Shichao Qi1, Qiang Zhang2, Xiaoqin Liu1, Linbing Sun1   

  1. 1. State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China;
    2. Department of Chemistry, Washington State University, Pullman, WA 99163, United States
  • 通讯作者: Linbing Sun,E-mail:lbsun@njtech.edu.cn
  • 基金资助:
    This work was supported by the National Natural Science Foundation of China (22078155, 21808110, 21878149, and 21676138), and China Postdoctoral Science Foundation (2020M681567). We are also grateful to the High Performance Computing Center of Nanjing Tech University for supporting the computational resources.

Abstract: Amines in porous materials have been employed as active species for the selective CO2 adsorption from natural gas because of their target-specific interactions. Nevertheless, it is difficult to modulate such strong interactions to reach a high efficiency in the adsorption processes. Herein, we fabricated light-responsive adsorbents with tunable adsorbent-adsorbate interactions for CO2 capture. The adsorbents were synthesized by introducing primary and secondary amines into a mesoporous silica that had been grafted with azobenzene groups on the surfaces. The target-specific amine sites render the adsorbents significantly selective in the uptake of CO2 over CH4, and the azobenzene groups were used as light-responsive switches to influence the adsorbent-adsorbate interactions. The adsorbents can freely adsorb CO2 when the azobenzene groups are in the trans state. Ultraviolet-light irradiation makes the azobenzene groups transform to the cis configuration, which greatly hinders amines in the uptake of CO2. The caused difference of adsorption capacity can reach 34.9%. The alternative irradiation by ultraviolet- and visible-light can lead to a recyclable regulation on adsorption performance. The changes of the electrostatic potentials of amines are responsible for the light-induced regulation on adsorption.

Key words: Adsorbents, CO2 capture, Selectivity, Light responsiveness, Azobenzene

摘要: Amines in porous materials have been employed as active species for the selective CO2 adsorption from natural gas because of their target-specific interactions. Nevertheless, it is difficult to modulate such strong interactions to reach a high efficiency in the adsorption processes. Herein, we fabricated light-responsive adsorbents with tunable adsorbent-adsorbate interactions for CO2 capture. The adsorbents were synthesized by introducing primary and secondary amines into a mesoporous silica that had been grafted with azobenzene groups on the surfaces. The target-specific amine sites render the adsorbents significantly selective in the uptake of CO2 over CH4, and the azobenzene groups were used as light-responsive switches to influence the adsorbent-adsorbate interactions. The adsorbents can freely adsorb CO2 when the azobenzene groups are in the trans state. Ultraviolet-light irradiation makes the azobenzene groups transform to the cis configuration, which greatly hinders amines in the uptake of CO2. The caused difference of adsorption capacity can reach 34.9%. The alternative irradiation by ultraviolet- and visible-light can lead to a recyclable regulation on adsorption performance. The changes of the electrostatic potentials of amines are responsible for the light-induced regulation on adsorption.

关键词: Adsorbents, CO2 capture, Selectivity, Light responsiveness, Azobenzene