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      Photoinduced water oxidation by an organic ligand incorporated into the framework of a stable metal–organic framework†

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      Author(s): a , b , a , a , a ,
      Publication date (Electronic):
      Journal: Chemical Science
      Publisher: Royal Society of Chemistry

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          Abstract

          Both the chemical stability and the catalytic efficiency of an organic ligand (TTCA) can be enhanced during the photoinduced water splitting reaction by incorporating it into the framework of a stable MOF.

          Abstract

          A major challenge for the development of organic water oxidation catalysts is their low chemical stability and low catalytic efficiency. Herein, we first demonstrate that both the chemical stability and catalytic efficiency of an organic ligand for water oxidation can be improved by incorporating it into the framework of a stable MOF. This opens up a promising avenue for the development of stable and efficient organic water oxidation catalysts.

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          A rationale for the large breathing of the porous aluminum terephthalate (MIL-53) upon hydration.

          Thierry Loiseau, Christian Serre, Clarisse Huguenard … (2004)
          Aluminum 1,4-benzenedicarboxylate Al(OH)[O(2)C-C(6)H(4)-CO(2)]. [HO(2)C-C(6)H(4)-CO(2)H](0.70) or MIL-53 as (Al) has been hydrothermally synthesized by heating a mixture of aluminum nitrate, 1,4-benzenedicarboxylic acid, and water, for three days at 220 degrees C. Its 3 D framework is built up of infinite trans chains of corner-sharing AlO(4)(OH)(2) octahedra. The chains are interconnected by the 1,4-benzenedicarboxylate groups, creating 1 D rhombic-shaped tunnels. Disordered 1,4-benzenedicarboxylic acid molecules are trapped inside these tunnels. Their evacuation upon heating, between 275 and 420 degrees C, leads to a nanoporous open-framework (MIL-53 ht (Al) or Al(OH)[O(2)C-C(6)H(4)-CO(2)]) with empty pores of diameter 8.5 A. This solid exhibits a Langmuir surface area of 1590(1) m(2)g(-1) together with a remarkable thermal stability, since it starts to decompose only at 500 degrees C. At room temperature, the solid reversibly absorbs water in its tunnels, causing a very large breathing effect and shrinkage of the pores. Analysis of the hydration process by solid-state NMR ((1)H, (13)C, (27)Al) has clearly indicated that the trapped water molecules interact with the carboxylate groups through hydrogen bonds, but do not affect the hydroxyl species bridging the aluminum atoms. The hydrogen bonds between water and the oxygen atoms of the framework are responsible for the contraction of the rhombic channels. The structures of the three forms have been determined by means of powder X-ray diffraction analysis. Crystal data for MIL-53 as (Al) are as follows: orthorhombic system, Pnma (no. 62), a = 17.129(2), b = 6.628(1), c = 12.182(1) A; for MIL-53 ht (Al), orthorhombic system, Imma (no. 74), a = 6.608(1), b = 16.675(3), c = 12.813(2) A; for MIL-53 lt (Al), monoclinic system, Cc (no. 9), a = 19.513(2), b = 7.612(1), c = 6.576(1) A, beta = 104.24(1) degrees.
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            Fabrication of flexible and freestanding zinc chalcogenide single layers.

            Yongfu Sun, Zhihu Sun, Shan Gao … (2012)
            Inorganic graphene analogues (IGAs) are a conceptually new class of materials with attractive applications in next-generation flexible and transparent nanodevices. However, their species are only limited to layered compounds, and the difficulty in extension to non-layered compounds hampers their widespread applicability. Here we report the fabrication of large-area freestanding single layers of non-layered ZnSe with four-atomic thickness, using a strategy involving a lamellar hybrid intermediate. Their surface distortion, revealed by means of synchrotron radiation X-ray absorption fine structure spectroscopy, is shown to give rise to a unique electronic structure and an excellent structural stability, thus determining an enhanced solar water splitting efficiency and photostability. The ZnSe single layers exhibit a photocurrent density of 2.14 mA cm(-2) at 0.72 V versus Ag/AgCl under 300 W Xe lamp irradiation, 195 times higher than that of bulk counterpart. This work opens the door for extending atomically thick IGAs to non-layered compounds and holds promise for a wealth of innovative applications.
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              Enantiomeric differentiation of aromatic amino acids using traveling wave ion mobility-mass spectrometry

              Virginie Domalain, Marie Hubert-Roux, Vincent Tognetti … (2014)
              The present work describes the first differentiation of amino acids enantiomers using the coupling of traveling wave ion mobility and mass spectrometry. The present work describes the first differentiation of enantiomers using the coupling of traveling wave ion mobility and mass spectrometry (TWIM-MS). This study was carried out on amino acids, the building blocks of proteins, which together with nucleotides, polysaccharides or lipids, are the main constituents of all living organisms. Herein, the enantiomers of aromatic amino acids (AA) such as phenylalanine, tryptophan and tyrosine are differentiated by TWIM-MS through their cationisation with copper( II ) and multimer formation with d -proline (Pro) as a chiral reference compound. This methodology can be considered as an alternative approach to conventional methods for the separation of enantiomers. Moreover, quantification of the enantiomers can be performed easily and quickly using TWIM-MS analysis of the ionic complex [( D Pro) 2 + D/L AA+Cu II –H] + .
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                Author and article information

                Journal
                Journal ID (nlm-ta): Chem Sci
                Journal ID (iso-abbrev): Chem Sci
                Title: Chemical Science
                Publisher: Royal Society of Chemistry
                ISSN (Print): 2041-6520
                ISSN (Electronic): 2041-6539
                Publication date (Print): 1 February 2016
                Publication date (Electronic): 11 November 2015
                Volume: 7
                Issue: 2
                Pages: 1070-1075
                Affiliations
                [a ] MOE Key Laboratory of Bioinorganic and Synthetic Chemistry , State Key Laboratory of Optoelectronic Materials and Technologies , School of Chemistry and Chemical Engineering , Sun Yat-Sen University , Guangzhou 510275 , China . Email: lutongbu@ 123456mail.sysu.edu.cn
                [b ] College of Chemistry and Chemical Engineering , Gannan Normal University , Ganzhou 341000 , China
                Article
                Publisher ID: c5sc02679b
                DOI: 10.1039/c5sc02679b
                PMC ID: 5590092
                PubMed ID: 28936323
                SO-VID: 2696d9b1-5eef-4d3b-b506-275711239c87
                Copyright © This journal is © The Royal Society of Chemistry 2015
                License:

                This is an Open Access article distributed under the terms of the Creative Commons Attribution 3.0 Unported License ( http://creativecommons.org/licenses/by/3.0/) which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

                History
                Date received : 23 July 2015
                Date accepted : 2 November 2015
                Categories
                Subject: Chemistry

                Notes

                †Electronic supplementary information (ESI) available: Additional structure figures, TGA curve, adsorption isotherms, UV-vis spectra, ESR spectra, GC spectra, PXRD patterns, and an additional cyclic voltammogram. CCDC 1003764. For ESI and crystallographic data in CIF or other electronic format see DOI: 10.1039/c5sc02679b


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