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原位掺入铜(II)卟啉功能化锆金属有机框架和二氧化钛以实现高效光催化二氧化碳还原

In-situ incorporation of Copper(II) porphyrin functionalized zirconium MOF and TiO for efficient photocatalytic CO reduction.

作者信息

Wang Lei, Jin Pengxia, Duan Shuhua, She Houde, Huang Jingwei, Wang Qizhao

机构信息

College of Chemistry and Chemical Engineering, Key Laboratory of Eco-Environment-Related Polymer Materials, Ministry of Education, Northwest Normal University, Lanzhou 730070, China.

College of Chemistry and Chemical Engineering, Key Laboratory of Eco-Environment-Related Polymer Materials, Ministry of Education, Northwest Normal University, Lanzhou 730070, China; School of Environmental Science and Engineering, Chang'an University, Xi'an 710064, China.

出版信息

Sci Bull (Beijing). 2019 Jul 15;64(13):926-933. doi: 10.1016/j.scib.2019.05.012. Epub 2019 May 17.

Abstract

As one of the highly effective methods to prepare catalysts for photocatalytic reduction of CO into value-added chemicals, using metalloporphyrin as light-harvesting mixed ligand to modify metal-organic framework (MOF) is very valuable since it can greatly improve the prophyrin dispersibility and consequently inhibit its potential agglomeration. Herein, we employed a one-pot synthetic strategy to chemically immobilize Cu(II) tetra(4-carboxylphenyl)porphyrin (CuTCPP) into UiO-66 MOF structure through coordination mode. Meanwhile, in-situ growth of TiO nanoparticles onto the MOF is actualized with the generation of CuTCPP ⊂ UiO-66/TiO (CTU/TiO) composites. Under Xe lamp irradiation (λ > 300 nm), the catalytic result presents that an optimal value of 31.32 μmol g h CO evolution amount, about 7 times higher than that of pure TiO was obtained through the photocatalysis. It is supposed owning to a consistent augment of light absorption derived from chemically implanted porphyrin derivative, which is simultaneously functioning with an efficacious separation of photo-induced carries given by the newly engendered composites between MOF and TiO, an effective catalytic activity and approving recyclability of CTU/TiO can be achieved in the photocatalytic reduction of CO into CO.

摘要

作为制备用于光催化将CO还原为增值化学品催化剂的高效方法之一,使用金属卟啉作为光捕获混合配体来修饰金属有机框架(MOF)非常有价值,因为它可以大大提高卟啉的分散性,从而抑制其潜在的团聚。在此,我们采用一锅合成策略,通过配位模式将四(4-羧基苯基)卟啉铜(II)(CuTCPP)化学固定到UiO-66 MOF结构中。同时,通过生成CuTCPP⊂UiO-66/TiO(CTU/TiO)复合材料实现了TiO纳米颗粒在MOF上的原位生长。在氙灯照射(λ>300nm)下,催化结果表明,通过光催化获得的CO析出量的最佳值为31.32μmol g h,约为纯TiO的7倍。推测这归因于化学植入的卟啉衍生物导致的光吸收持续增加,其与MOF和TiO之间新生成的复合材料所实现的光生载流子有效分离同时起作用,在将CO光催化还原为CO的过程中可以实现CTU/TiO有效的催化活性和良好的可回收性。

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