Huan Dai, Zichen Xu, Ke Yang, Jianchao Zhou, Jing Wang, Ya Zhang, Yudong Shen, Xiaolan Liu, Yue Jiang and Wei Xu*,
{"title":"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","authors":"Huan Dai, Zichen Xu, Ke Yang, Jianchao Zhou, Jing Wang, Ya Zhang, Yudong Shen, Xiaolan Liu, Yue Jiang and Wei Xu*, ","doi":"10.1021/acs.inorgchem.4c0435310.1021/acs.inorgchem.4c04353","DOIUrl":null,"url":null,"abstract":"<p >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 CO<sub>2</sub> 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]<sub><i>n</i></sub> (Tb-MOF) (H<sub>3</sub>L = 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 CO<sub>2</sub> 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 Tb<sup>3+</sup> site as Lewis acidic centers makes Tb-MOF achieve efficiently catalytic conversion for CO<sub>2</sub> 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.</p>","PeriodicalId":40,"journal":{"name":"Inorganic Chemistry","volume":"63 51","pages":"24351–24362 24351–24362"},"PeriodicalIF":4.7000,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A Multifunctional Tb(III)-Based Metal–Organic Framework for Chemical Conversion of CO2, Fluorescence Sensing of Trace Water and Metamitron\",\"authors\":\"Huan Dai, Zichen Xu, Ke Yang, Jianchao Zhou, Jing Wang, Ya Zhang, Yudong Shen, Xiaolan Liu, Yue Jiang and Wei Xu*, \",\"doi\":\"10.1021/acs.inorgchem.4c0435310.1021/acs.inorgchem.4c04353\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >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 CO<sub>2</sub> 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]<sub><i>n</i></sub> (Tb-MOF) (H<sub>3</sub>L = 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 CO<sub>2</sub> 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 Tb<sup>3+</sup> site as Lewis acidic centers makes Tb-MOF achieve efficiently catalytic conversion for CO<sub>2</sub> 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. 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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.
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.