具有高传质和亲和表面的NH<sub>2</sub>-UIO-66基疏水多孔液体用于增强CO<sub>2</sub>光还原

引用本文: 徐阳锐, 任叶炜, 刘馨琳, 李宏平, 逯子扬. 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[J]. 物理化学学报, 2024, 40(11): 240303. doi: 10.3866/PKU.WHXB202403032 shu

Citation: Yangrui Xu, Yewei Ren, Xinlin Liu, Hongping Li, Ziyang Lu. NH₂-UIO-66 Based Hydrophobic Porous Liquid with High Mass Transfer and Affinity Surface for Enhancing CO₂ Photoreduction[J]. Acta Physico-Chimica Sinica, 2024, 40(11): 240303. doi: 10.3866/PKU.WHXB202403032 shu

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

徐阳锐 ^1, ,
任叶炜 ^1, ,
刘馨琳 ^{2,
,} ,
李宏平 ^3, ,
逯子扬 ^{1, 4,
,}

1.
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, 江苏大学, 江苏镇江 212013
2.
能源与动力工程学院, 江苏大学, 江苏镇江 212013
3.
能源研究院, 江苏大学, 江苏镇江 212013
4.
江苏省水处理技术与材料协同创新中心, 苏州科技大学, 江苏苏州 215009

通讯作者: 刘馨琳, liuxl@ujs.edu.cn; 逯子扬, luziyang126@126.com

基金项目:
22278190

CQ2022009

20230022

2023

JG-03-11

KY-C-12

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)嫁接到金属有机骨架(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。通过嫁接疏水性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。

关键词:

English

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

Yangrui Xu ^1, ,
Yewei Ren ^1, ,
Xinlin Liu ^{2,
,} ,
Hongping Li ^3, ,
Ziyang Lu ^{1, 4,
,}

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

Corresponding author: Email: liuxl@ujs.edu.cn (X.L.); Email: luziyang126@126.com (Z.L.)

Received Date: 28 March 2024
Accepted Date: 06 May 2024
Revised Date: 02 May 2024
Available Online: 15 November 2024
Fund Project:
the National Natural Science Foundation of China

Zhenjiang Carbon Emissions Peak/Carbon Neutrality Science and Technology Innovation Special Fund Project

Open Project of State Key Laboratory of Structural Chemistry

Qing Lan Project of Jiangsu Province

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

the Special Scientific Research Project of School of Emergency Management of Jiangsu University

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:

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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

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

通讯作者: 刘馨琳, liuxl@ujs.edu.cn; 逯子扬, luziyang126@126.com

English

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

Corresponding author: Email: liuxl@ujs.edu.cn (X.L.); Email: luziyang126@126.com (Z.L.)

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CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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

通讯作者: 刘馨琳, liuxl@ujs.edu.cn; 逯子扬, luziyang126@126.com

English

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

Corresponding author: Email: liuxl@ujs.edu.cn (X.L.); Email: luziyang126@126.com (Z.L.)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

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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

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

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