用于CO2化学转化、痕量水和变氮荧光传感的多功能Tb(III)基金属-有机骨架

IF 4.7 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Huan Dai, Zichen Xu, Ke Yang, Jianchao Zhou, Jing Wang, Ya Zhang, Yudong Shen, Xiaolan Liu, Yue Jiang and Wei Xu*, 
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引用次数: 0

摘要

利用金属-有机框架(MOFs)作为荧光传感器来检测环境和化学试剂污染物以及用于二氧化碳转化的多相催化是一个重要的研究途径,对保护人类健康具有重要意义。本文利用单晶x射线晶体学方法,构造了一种基于Tb(III)的三维金属有机骨架[Tb(L)·4DMF]n (Tb- mof) (H3L = 5′-(4-羧基-3-羟基苯基)-3,3″-二羟基-[1,1′:3′,1″-terphenyl]-4,4″-二羧酸)。它具有沿[010]方向的一维菱形通道,孔径为6.02 × 9.13 Å。Tb-MOF是一种多功能的荧光传感器材料和CO2环加成非均相催化剂材料。荧光传感研究表明,Tb-MOF具有较高的灵敏度、选择性和良好的再生性能,是一种有效的化学传感器,可用于检测有机溶剂中的农药和痕量水。结合XRD、紫外-可见吸收光谱、红外光谱、理论计算和荧光寿命分析,对MMT和水猝灭荧光的机理进行了分析。该材料还被用于感应MMT和纸条中的水。此外,开放的Tb3+位点作为刘易斯酸中心,使Tb-MOF能够有效地催化二氧化碳和环氧化物转化为环状碳酸盐。此外,通过原位漫反射红外傅里叶变换光谱(DRIFTS)实验,提出了二氧化碳转化为环状碳酸盐的可能催化机理。它还表现出可回收性长达五个周期,而没有注意到传感或催化效率的明显损失。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

A Multifunctional Tb(III)-Based Metal–Organic Framework for Chemical Conversion of CO2, Fluorescence Sensing of Trace Water and Metamitron

A Multifunctional Tb(III)-Based Metal–Organic Framework for Chemical Conversion of CO2, Fluorescence Sensing of Trace Water and Metamitron

The utilization of metal–organic frameworks (MOFs) as fluorescent sensors for the detection of environmental and chemical reagent pollutants as well as heterogeneous catalysis for CO2 conversion represents a crucial avenue of research with significant implications for the protection of human health. In this work, a Tb(III)-based three-dimensional metal–organic framework, [Tb(L)·4DMF]n (Tb-MOF) (H3L = 5′-(4-carboxy-3-hydroxyphenyl)-3,3″-dihydroxy-[1,1′:3′,1″-terphenyl]-4,4″-dicarboxylic acid), has been structurally conformed by single-crystal X-ray crystallography. It possesses a 1D rhombus channel along the [010] direction, featuring a pore size of 6.02 × 9.13 Å. Tb-MOF was proved to be a multifunctional material for a fluorescent sensor and CO2 cycloaddition heterogeneous catalyst material. Fluorescence sensing studies revealed that Tb-MOF demonstrates high sensitivity, selectivity, and favorable regeneration properties, making it an effective chemosensor for detecting the metamitron (MMT) pesticide and trace water in organic solvents. The mechanism of fluorescence quenching by MMT and water was elucidated by a combination of XRD, UV–vis absorption spectra, IR spectra, theoretical calculations, and fluorescence lifetimes. The material was also utilized for the sensing of MMT and water in paper strips. Additionally, the open Tb3+ site as Lewis acidic centers makes Tb-MOF achieve efficiently catalytic conversion for CO2 and epoxides to cyclic carbonates. Moreover, a possible catalytic mechanism for the conversion of carbon dioxide to cyclic carbonates was proposed by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments. It also exhibited recyclability for up to five cycles without noticing an appreciable loss in sensing or catalytic efficiency.

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来源期刊
Inorganic Chemistry
Inorganic Chemistry 化学-无机化学与核化学
CiteScore
7.60
自引率
13.00%
发文量
1960
审稿时长
1.9 months
期刊介绍: Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.
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