首页|期刊导航|物理化学学报|具有高传质和亲和表面的NH2-UIO-66基疏水多孔液体用于增强CO2光还原

具有高传质和亲和表面的NH2-UIO-66基疏水多孔液体用于增强CO2光还原OA北大核心CSTPCD

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

中文摘要英文摘要

增加光催化剂表面的CO2浓度有助于提高光催化还原CO2的反应动力学速率.然而,CO2在水相中的低溶解度和较差的传质严重阻碍了CO2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(NH2-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(NH2-UIO-66 PL).研究发现,具有永久孔隙率的NH2-UIO-66 PL能够使大量CO2富集在多孔液体的空腔中,便于CO2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CO2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CO2能力.NH2-UIO-66 PL的CO产率为24.70 μmol∙g-1∙h-1,CH4产率为7.93 μmol∙g-1∙h-1,分别是亲水性NH2-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CO2吸附和还原提供了工业应用的可能性.

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.

徐阳锐;任叶炜;刘馨琳;李宏平;逯子扬

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江苏大学能源与动力工程学院,江苏 镇江 212013江苏大学能源研究院,江苏 镇江 212013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||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

化学

多孔液体UIO-66疏水表面CO2传输通道CO2光还原

Porous liquidsUIO-66Hydrophobic surfaceCO2 transport channelCO2 photoreduction

《物理化学学报》 2024 (11)

29-30,2

The project was 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),and the Special Scientific Research Project of School of Emergency Management of Jiangsu University(KY-C-12). 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)

10.3866/PKU.WHXB202403032

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