具有高传质和亲和表面的NH_(2)-UIO-66基疏水多孔液体用于增强CO_(2)光还原  

NH_(2)-UIO-66 Based Hydrophobic Porous Liquid with High Mass Transfer and Affinity Surface for Enhancing CO_(2) Photoreduction

作　　者：徐阳锐 任叶炜 刘馨琳[2] 李宏平 逯子扬[1,4] Yangrui Xu;Yewei Ren;Xinlin Liu;Hongping Li;Ziyang Lu(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;School of Energy and Power Engineering,Jiangsu University,Zhenjiang 212013,Jiangsu Province,China;Institute for Energy Research,Jiangsu University,Jiangsu,Zhenjiang 212013,Jiangsu Province,China;Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment,Suzhou University of Science and Technology,Suzhou 215009,Jiangsu Province,China)

机构地区：[1]江苏大学环境健康与生态安全研究所,应急管理学院,环境与安全工程学院,江苏镇江212013 [2]江苏大学能源与动力工程学院,江苏镇江212013 [3]江苏大学能源研究院,江苏镇江212013 [4]苏州科技大学江苏省水处理技术与材料协同创新中心,江苏苏州215009

出　　处：《物理化学学报》2024年第11期29-30,共2页Acta Physico-Chimica Sinica

基　　金：国家自然科学基金项目(22278190);镇江市碳达峰碳中和科技创新专项—产业前瞻与共性关键技术攻关项目(CQ2022009);结构化学国家重点实验室开放项目(20230022);江苏省青蓝工程人才项目(2023);江苏水处理技术与材料协同创新中心、江苏大学应急管理学院教育教改研究和人才培养专项项目(JG-03-11);江苏大学应急管理学院专项科研项目(KY-C-12)。

摘　　要：增加光催化剂表面的CO_(2)浓度有助于提高光催化还原CO_(2)的反应动力学速率。然而,CO_(2)在水相中的低溶解度和较差的传质严重阻碍了CO_(2)在活性位点的吸附和转化。在本工作中,将疏水性液体端长链(PDMS)接枝到金属有机骨架(NH_(2)-UIO-66)的氨基位点上,合成了具有强疏水性的多孔液体光催化剂(NH_(2)-UIO-66 PL)。研究发现,具有永久孔隙率的NH_(2)-UIO-66 PL能够使大量CO_(2)富集在多孔液体的空腔中,便于CO_(2)的快速运输并扩散到光催化剂表面。通过接枝疏水性PDMS形成具有高正电位的CO_(2)亲和表面和活化还原反应的关键中间体,从而形成更强的电子富集Zr活性位点,增强整体的光还原CO_(2)能力。NH_(2)-UIO-66 PL的CO产率为24.70μmol·g^(-1)·h^(-1),CH_(4)产率为7.93μmol·g^(-1)·h^(-1),分别是亲水性NH_(2)-UIO-66的2.3倍和2.7倍。这项研究提供了一种新颖的疏水性多孔液体的设计,为高CO_(2)吸附和还原提供了工业应用的可能性。Increasing the CO_(2)concentration on the surface of the photocatalysts helps to increase the reaction dynamic rate of the photocatalytic CO_(2)reduction.However,the low solubility and poor mass transfer of CO_(2)in aqueous phase seriously hinder the adsorption and conversion of CO_(2)at the active site.In this work,the porous liquid photocatalyst(NH_(2)-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(NH_(2)-UIO-66).It is found that the NH_(2)-UIO-66 PL with permanent porosity causes a large amount of CO_(2)to be concentrated in the porous liquid cavity for transporting and diffusing CO_(2)onto the photocatalyst surface rapidly,and then the CO_(2)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 CO_(2)reduction ability.As a result,NH_(2)-UIO-66 PL achieved CO_(2)photoreduction with a CO yield of 24.70μmol∙g^(-1)∙h^(-1)and CH_(4)yield of 7.93μmol∙g^(-1)∙h^(-1),which is 2.3-fold and 2.7-fold compared to hydrophilic NH_(2)-UIO-66,respectively.This research provides a novel design of hydrophobic porous liquids to provide industrial possibilities for high CO_(2)adsorption and reduction.

关 键 词：多孔液体 UIO-66 疏水表面 CO_(2)传输通道 CO_(2)光还原 

分 类 号：O643[理学—物理化学]