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可见光驱动增强CsPbBr量子点@二维Cu-TCPP异质结中的电子-空穴分离及高效光还原CO

Visible-light driven boosting electron-hole separation in CsPbBr QDs@2D Cu-TCPP heterojunction and the efficient photoreduction of CO.

作者信息

Zhang Na, Li Jia-Jia, Li Yang, Wang Hang, Zhang Jian-Yong, Liu Yufeng, Fang Yong-Zheng, Liu Zhifu, Zhou Min

机构信息

Shanghai Institute of Technology, Shanghai 201418, PRChina.

Shanghai Institute of Technology, Shanghai 201418, PRChina.

出版信息

J Colloid Interface Sci. 2022 Feb 15;608(Pt 3):3192-3203. doi: 10.1016/j.jcis.2021.11.045. Epub 2021 Nov 13.

DOI:10.1016/j.jcis.2021.11.045
PMID:34801238
Abstract

CsPbBr quantum dots (CPB QDs) have great potential in photoreduction of CO to chemical fuels. However, the low charge transportation efficiency and chemical instability of CPB QDs presents a considerable challenge. Herein, we describe the electrostatic assemblies of negatively charged colloidal two dimensional (2D) Cu-Tetrakis(4-carboxyphenyl) porphyrins (Cu-TCPP) nanosheets and positively CPB QDs to construct the hydride heterojunction. The photogenerated electron migration from CPB QDs to Cu-TCPP nanosheets has been witnessed, providing the supply of long-lived electrons for the reduction of CO molecules adsorbed on Cu-TCPP matrix. As a direct result, The CPB@Cu-TCPP-x (x wt% of CPB QDs) photocatalysts exhibit significantly enhanced photocatalytic conversion of CO, compared to the parent Cu-TCPP nanosheets or single CPB QDs. Especially, when with 20% CPB QDs, the heterostruture system achieves an evolution yield of 287.08 µmol g in 4 h with highly CO selectivity (99%) under visible light irradiation, which is equivalent to a 3.87-fold improvement compared to the pristine CPB QDs. Meanwhile, the CH generation rate can be up to 3.25 µmol g. This optimized construction of heterostructure could provide a platform to funnel photoinduced electrons to the reaction center, which can both act as a crucial capture and the reaction actives of CO.

摘要

CsPbBr量子点(CPB QDs)在将CO光还原为化学燃料方面具有巨大潜力。然而,CPB QDs的低电荷传输效率和化学不稳定性带来了相当大的挑战。在此,我们描述了带负电荷的二维(2D)铜-四(4-羧基苯基)卟啉(Cu-TCPP)纳米片与带正电荷的CPB QDs的静电组装,以构建氢化物异质结。已观察到光生电子从CPB QDs迁移到Cu-TCPP纳米片,为还原吸附在Cu-TCPP基质上的CO分子提供了长寿命电子。直接结果是,与母体Cu-TCPP纳米片或单一CPB QDs相比,CPB@Cu-TCPP-x(x wt%的CPB QDs)光催化剂表现出显著增强的CO光催化转化。特别是,当含有20%的CPB QDs时,该异质结构体系在可见光照射下4小时内实现了287.08 µmol g的析出产率,具有很高的CO选择性(99%),与原始CPB QDs相比提高了3.87倍。同时,CH生成速率可达3.25 µmol g。这种优化的异质结构构建可以提供一个平台,将光生电子引导到反应中心,该反应中心既可以作为关键的捕获点,又可以作为CO的反应活性点。

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