Acta Phys. -Chim. Sin. ›› 2024, Vol. 40 ›› Issue (11): 2403032.doi: 10.3866/PKU.WHXB202403032

• ARTICLE • Previous Articles     Next Articles

NH2-UIO-66 Based Hydrophobic Porous Liquid with High Mass Transfer and Affinity Surface for Enhancing CO2 Photoreduction

Yangrui Xu1, Yewei Ren1, Xinlin Liu2,*(), Hongping Li3, Ziyang Lu1,4,*()   

  1. 1 Institute of Environmental Health and Ecological Security, School of Emergency Management, School of the Environment and Safety Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu Province, China
    2 School of Energy and Power Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu Province, China
    3 Institute for Energy Research, Jiangsu University, Jiangsu, Zhenjiang 212013, Jiangsu Province, China
    4 Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Suzhou University of Science and Technology, Suzhou 215009, Jiangsu Province, China
  • Received:2024-03-28 Revised:2024-05-02 Accepted:2024-05-06 Published:2024-10-14
  • Contact: Email: liuxl@ujs.edu.cn (Xinlin Liu)luziyang126@126.com (Ziyang Lu)
  • Supported by:
    the National Natural Science Foundation of China(22278190); Zhenjiang Carbon Emissions Peak/Carbon Neutrality Science and Technology Innovation Special Fund Project(CQ2022009); Open Project of State Key Laboratory of Structural Chemistry(20230022); Qing Lan Project of Jiangsu Province(2023); Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Project of Research on Educational Reform and Talent Development of School of Emergency Management of Jiangsu University(JG-03-11); the Special Scientific Research Project of School of Emergency Management of Jiangsu University(KY-C-12)

Abstract:

Increasing the CO2 concentration on the surface of the photocatalysts helps to increase the reaction dynamic rate of the photocatalytic CO2 reduction. However, the low solubility and poor mass transfer of CO2 in aqueous phase seriously hinder the adsorption and conversion of CO2 at the active site. In this work, the porous liquid photocatalyst (NH2-UIO-66 PL) with strong hydrophobicity has been synthesized by grafting the hydrophobic liquid end long-chain (PDMS) onto the amino site of metal-organic framework (NH2-UIO-66). It is found that the NH2-UIO-66 PL with permanent porosity causes a large amount of CO2 to be concentrated in the porous liquid cavity for transporting and diffusing CO2 onto the photocatalyst surface rapidly, and then the CO2 affinity surface with high positive potential and key intermediates for activation reduction reactions are formed with the grafting of hydrophobic PDMS, leading to stronger electron enrichment Zr active sites for enhancement of the overall CO2 reduction ability. As a result, NH2-UIO-66 PL achieved CO2 photoreduction with a CO yield of 24.70 μmol∙g−1∙h−1 and CH4 yield of 7.93 μmol∙g−1∙h−1, which is 2.3-fold and 2.7-fold compared to hydrophilic NH2-UIO-66, respectively. This research provides a novel design of hydrophobic porous liquids to provide industrial possibilities for high CO2 adsorption and reduction.

Key words: Porous liquids, UIO-66, Hydrophobic surface, CO2 transport channel, CO2 photoreduction