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光催化CO2静电纺丝MOF膜的制备与性能

作者：林鹏飞，何欣平，吴东云，董晨曦，赵磊，伊春海，郭佳鑫

单位： 1 西安交通大学化学工程与技术学院，西安 710049；2陕西延长石油（集团）有限责任公司研究院，西安 710065；3盐城职业技术学院纺织服装学院，盐城 224005

关键词： MOFs；ZIF-67；热稳定；静电纺丝；膜；光催化；CO2还原

DOI号：

分类号： X701

出版年,卷(期):页码： 2024,44(4):17-27

摘要：

金属有机骨架(MOFs)因其在多相催化中的应用而受到广泛的关注，但是与反应混合物的分离效果差限制了其实际应用。MOFs薄膜在光催化分解污染物方面有着广泛的应用，但在光催化CO2领域很少有报道，所以制备适合光催化CO2高效还原的MOFs薄膜十分有必要。本研究通过静电纺丝将ZIF-67混纺在聚丙烯腈(PAN)纳米纤维膜(NFMs)内，再进行热稳定处理，得到SZIF-67/PAN NFMs，表征了形貌特征、化学成分、光催化性能以及光电性能等。结果表明，SZIF-67/PAN NFMs由于可见光响应的改善、光热转化能力和耐溶剂能力的提高，对CO2的还原表现出优异的可见光驱动光催化活性，CO生成速率达到12000μmol/(g.h)，重复使用3次后光催化性能仍保持在85.4%。此外，还提出了CO2全面光还原的可能机理：光敏剂通过可见光激发产生电子注入SZIF-67/PAN NFMs中Co活性点位，吸附在Co活性点位上的电子进一步转移到CO2上并与质子形成CO。最后CO从NFMs上解吸，实现光催化CO2到CO的转化。

Metal-organic frameworks (MOFs) have garnered considerable attention for their applications in heterogeneous catalysis. However, their practical utility is hindered by subpar separation efficiency from reaction mixtures. While MOF membranes find widespread application in photocatalytic decomposition of pollutants, their utilization in the photocatalytic CO2 reduction domain is notably underexplored. Consequently, the preparation of MOF membranes tailored for efficient photocatalytic CO2 reduction becomes imperative. In this study, ZIF-67 was blended into polyacrylonitrile (PAN) nanofiber membranes (NFMs) by electrospinning, and then heat stabilized to obtain SZIF-67/PAN NFMs. The morphology, chemical composition, photocatalytic properties and photoelectric properties were characterized. The results demonstrate that SZIF-67/PAN NFMs exhibit outstanding visible light-driven photocatalytic activity for CO2 reduction, attributed to improvements in visible light responsiveness, photothermal conversion capability, and solvent resistance. The CO generation rate reached 12000 μmol/(g.h), with photocatalytic performance maintaining at 85.4% after three repeated uses. In addition, the possible mechanism of total CO2 photoreduction is proposed: the photosensitizers generate electrons through visible light excitation into the Co active site in SZIF-67/PAN NFMs, and the electrons adsorbing at the Co active site are further transferred to CO2 and form CO with protons. Finally, CO is desorbed from NFMs to achieve the photocatalytic conversion of CO2 to CO.

基金项目：

陕西省自然科学基金（2023-JC-ZD-26）

作者简介：

林鹏飞（1992-），男，山东潍坊人，博士研究生，从事静电纺丝先进光催化纳米纤维膜的制备与应用，E-mail：linpengfei@stu.xjtu.edu.cn

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