Naphthaleneimide functionalized NU-1000 as an efficient donor-acceptor photo-catalyst for the visible-light-driven oxidation of benzylamine coupling

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials Pub Date : 2025-06-04 DOI:10.1016/j.micromeso.2025.113724

Chunyu Liu, Mingxue Shao, Huadong Guo, Jiaping Cao, Rao Bao, Xianmin Guo

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引用次数: 0

Abstract

Metal-organic frameworks provided an advantageous platform for photo-catalysis owing to their designable structure and tunable photo-electric characteristic. However, the catalytic performance of MOFs often suffered from poor chem-stability, low visible light absorption and inefficient photogenerated charge separation. In this work, through the solvent-assisted ligand incorporation method, a carboxylate-derivatized naphthaleneimide moiety (HBNDI) was successfully integrated into pyrene-cored NU-1000 to establish a mixed-ligand BNDI-NU-1000. Photo-electric measurements and DFT calculations revealed that BNDI-NU-1000 was a typical donor-acceptor system owing to the rapid charge transfer between electron-rich pyrene and electron-deficient naphthaleneimide. Due to the synergetic effect of efficient photo-induced electron transfer and energy transfer, BNDI-NU-1000 displayed high catalytic activity in the visible-light-driven aerobic oxidation of benzylamine coupling. This study opened up a promising avenue to develop viable donor-acceptor photo-catalysts for organic transformation.

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萘酰亚胺功能化NU-1000作为一种高效的供-受体光催化剂用于可见光驱动氧化苄胺偶联反应

金属有机骨架具有可设计的结构和可调谐的光电特性，为光催化提供了有利的平台。然而，mof的催化性能往往存在化学稳定性差、可见光吸收低、光生电荷分离效率低等问题。本研究通过溶剂辅助配体掺入法，将羧酸衍生物化萘酰亚胺（HBNDI）部分成功整合到芘核的NU-1000中，建立了混合配体BNDI-NU-1000。光电测量和DFT计算表明，BNDI-NU-1000是一个典型的供体-受体体系，其电荷在富电子芘和缺电子萘酰亚胺之间快速转移。由于高效的光诱导电子转移和能量转移的协同作用，BNDI-NU-1000在可见光驱动的苯胺偶联有氧氧化中表现出较高的催化活性。本研究为开发可行的有机转化供受体光催化剂开辟了一条有前途的途径。

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来源期刊

Microporous and Mesoporous Materials 化学-材料科学：综合

CiteScore

10.70

自引率

5.80%

发文量

649

审稿时长

26 days

期刊介绍： Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.