具有定向电荷传递能力的晶态线型聚酰亚胺材料驱动光催化CO2还原

doi:10.1016/S1872-2067(23)64450-X

催化学报 ›› 2023, Vol. 49: 152-159.DOI: 10.1016/S1872-2067(23)64450-X

具有定向电荷传递能力的晶态线型聚酰亚胺材料驱动光催化CO₂还原

李慧珍^a, 陈艳蕾^a, 牛青^a, 王小凤^a, 刘哲源^a, 毕进红^b, 于岩^a^,^*(), 李留义^a^,^*()

^a福州大学材料科学与工程学院, 生态材料先进技术重点实验室, 福建福州 350108
^b福州大学环境与安全工程学院, 福建福州 350108

收稿日期:2023-02-28 接受日期:2023-04-18 出版日期:2023-06-18 发布日期:2023-06-05
通讯作者: ^*电子邮件: lyli@fzu.edu.cn (李留义),yuyan@fzu.edu.cn (于岩).
基金资助:
国家重点研发计划(2020YFA0710303);国家自然科学基金(52172188);国家自然科学基金(22272028);国家自然科学基金(U1905215);国家自然科学基金(52072076)

The crystalline linear polyimide with oriented photogenerated electron delivery powering CO₂ reduction

Huizhen Li^a, Yanlei Chen^a, Qing Niu^a, Xiaofeng Wang^a, Zheyuan Liu^a, Jinhong Bi^b, Yan Yu^a^,^*(), Liuyi Li^a^,^*()

^aKey Laboratory of Eco-materials Advanced Technology, College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, Fujian, China
^bDepartment of Environmental Science and Engineering, Fuzhou University, Fuzhou 350108, Fujian, China

Received:2023-02-28 Accepted:2023-04-18 Online:2023-06-18 Published:2023-06-05
Contact: ^*E-mail: lyli@fzu.edu.cn (L. Li),yuyan@fzu.edu.cn (Y. Yu).
Supported by:
National Key Research and Development Program of China(2020YFA0710303);National Natural Science Foundation of China(52172188);National Natural Science Foundation of China(22272028);National Natural Science Foundation of China(U1905215);National Natural Science Foundation of China(52072076)

摘要/Abstract

摘要：

利用太阳能和半导体催化材料将CO₂还原为具有高附加值的含碳化学品为解决能源危机等问题提供了一个有前景的解决方案. 目前半导体光催化CO₂还原的效率仍然很低, 这主要是光激发的载流子复合严重等问题导致的. 探索有效策略来增强半导体光催化材料光生电荷分离和传输性能被认为是提高CO₂还原效率的关键之一. 设计制备具有定向电荷传输性能的光催化材料将有助于抑制光生电荷复合, 从而实现高效光催化性能. 线型共轭有机聚合物具有直链状结构、明晰和多样的元素组成、良好的水热稳定性等优点在光催化领域受到持续的关注和研究.

本文通过均苯四甲酸二酐和二胺单体的缩合反应制备了三例晶态线型共轭聚酰亚胺材料用于光催化CO₂还原. 利用粉末X射线衍射、傅里叶红外光谱、扫描电子显微镜、透射电子显微镜、紫外可见吸收光谱和气体吸附测试等对合成的聚酰亚胺的晶态结构、光吸收性质、形貌结构和孔结构等进行了表征. 利用光电化学、电子顺磁共振波普分析、电位分析和密度泛函理论计算等研究了构筑单元的电子推拉效应对聚合物电荷分离及催化性能的影响. 结果表明, 三种结晶型聚酰亚胺均对CO₂具有良好的吸附能力且满足光催化CO₂还原电势的能带结构要求. 光生载流子的复合程度随着重复结构单元偶极距的增强而降低, 其中基于苯并噻吩砜的晶态线型聚酰亚胺(CLP-CS)具有最优的载流子分离能力. 在光催化CO₂还原反应中, CLP-CS表现出高达1700 µmol h^‒1 g_cat^‒1的CO析出效率和90%的选择性. CLP-CS在高低温和紫外灯照射等极端条件下, 仍保持良好的结构稳定性和催化活性. 实验发现, 聚合物的CO₂还原活性与重复结构单元的偶极距及方向密切有关. 局部结构的不对称性, 扩大了分子偶极, 增强了材料的内建电场驱动力. 此外, 长程有序的线型结构为光生电荷传输提供了快速迁移通道, 促进了载流子迁移. 综上, 本文报道了基于晶态线型聚合物的光催化体系, 为实现光生电荷定向传输和开发高效光催化材料提供了途径.

关键词: 光催化, 结晶聚合物, 聚酰亚胺, 二氧化碳还原, 电子定向转移

Abstract:

Orienting electron transport to suppress charge recombination is attractive for efficient photocatalysis but remains challenging. Herein, we demonstrate the synthesis of crystalline linear conjugated polyimides via the condensation of carboxylic anhydrides and amine monomers for the photocatalytic reduction of CO₂. Oriented electron transport was achieved using crystalline polyimides integrated with electronic push-pull units. Directional intramolecular electron transfer is driven by the dipole effects of the adjacent building units. The sulfone-based polyimide exhibited excellent photocatalytic performance for CO₂ reduction. Our work provides a new example photoreduction of CO₂ and a strategy for developing efficient photocatalysts with oriented electron transport.

Key words: Photocatalysis, Crystalline polymer, Polyimides, CO₂ reduction, Electron transport

李慧珍, 陈艳蕾, 牛青, 王小凤, 刘哲源, 毕进红, 于岩, 李留义. 具有定向电荷传递能力的晶态线型聚酰亚胺材料驱动光催化CO₂还原[J]. 催化学报, 2023, 49: 152-159.

Huizhen Li, Yanlei Chen, Qing Niu, Xiaofeng Wang, Zheyuan Liu, Jinhong Bi, Yan Yu, Liuyi Li. The crystalline linear polyimide with oriented photogenerated electron delivery powering CO₂ reduction[J]. Chinese Journal of Catalysis, 2023, 49: 152-159.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(23)64450-X

https://www.cjcatal.com/CN/Y2023/V49/I6/152

图/表 6

Fig. 1. Schematic illustration of functionalities of CLP-CS.

Fig. 2. (a) Schematic synthetic illustration of CLP-CS, CLP-CF, and CLP-CB. Side (b) and top (c) views of the crystal structure of CLP-CS. (d-f) PXRD patterns of experimentally observed (red), the simulated pattern (blue/orange/ purple), the profiles calculated from Le Bail fitting (green) and residual (black) for CLP-CS CLP-CF, and CLP-CB, respectively. Optical microscopy (g), SEM (h), and TEM (i) images of CLP-CS.

Fig. 3. UV-vis diffuse reflectance spectra (a), band gap structures (b), transient photocurrent responses (c), and PL spectra (d) of CLP-CS, CLP-CF, and CLP-CB.

Fig. 4. The HOMOs and LUMOs (a) and the calculated molecular dipoles (b) of model compounds for CLP-CS, CLP-CF, and CLP-CB. (c) The EPR spectra of CLP-CS and CLP-CS with [Co(bpy)3]2+ (CLP-CS and the in situ formed [Co(bpy)3]2+) under dark and light irradiation. (d) Zeta potentials of CLP-CS and [Co(bpy)3]2+.

Fig. 5. (a) Kinetic profile of CO production by CLP-CS. (b) GC-MS measurement of the gas production in isotope 13CO2 tracking experiment. (c) Catalytic performance of three polymers in an hour. (d) Recycling test of CLP-CS.

Fig. 6. Proposed photocatalytic mechanism of crystalline linear polyimide for CO2 reduction via photoinduced oriented electron transfer.

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具有定向电荷传递能力的晶态线型聚酰亚胺材料驱动光催化CO₂还原

The crystalline linear polyimide with oriented photogenerated electron delivery powering CO₂ reduction

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