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Microporous Lead-Organic Framework for Selective CO2 Adsorption and Heterogeneous Catalysis
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SYSNO ASEP 0498940 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title Microporous Lead-Organic Framework for Selective CO2 Adsorption and Heterogeneous Catalysis Author(s) Almáši, M. (CZ)
Zeleňák, V. (SK)
Gyepes, Robert (UFCH-W) RID, ORCID
Bourrelly, S. (FR)
Opanasenko, Maksym (UFCH-W) RID, ORCID
Llewellyn, P. L. (FR)
Čejka, Jiří (UFCH-W) RID, ORCID, SAISource Title Inorganic Chemistry. - : American Chemical Society - ISSN 0020-1669
Roč. 57, č. 4 (2018), s. 1774-1786Number of pages 13 s. Language eng - English Country US - United States Keywords secondary building units ; gas-adsorption ; carbon-dioxide ; porous materials ; base catalyst ; metal sites Subject RIV CF - Physical ; Theoretical Chemistry OECD category Physical chemistry R&D Projects GBP106/12/G015 GA ČR - Czech Science Foundation (CSF) Institutional support UFCH-W - RVO:61388955 UT WOS 000426014800013 EID SCOPUS 85042222303 DOI 10.1021/acs.inorgchem.7b02491 Annotation A novel microporous metal-organic framework, ({pb(4)(p(8)-MTB)(2)(H2O)(4)]center dot 5DMF center dot H2O}, (1, MTB = methanetetra-benzoate and DMF = N,N'-dimethylformamide), was successfully synthesized by a solvothermal reaction and structurally characterized by single-crystal X-ray diffraction. The framework exhibits a unique tetranuclear [Pb-4(mu(3)-COO)(mu(2)-COO)(6)(COO)(H2O)(4)] secondary building unit (SBU). The combination of the SBU with the tetrahedral symmetry of MTB results in a three-dimensional network structure, with one-dimensional jarlike cavities having sizes of about 14.98 x 7.88 and 14.98 x 13.17 angstrom(2) and propagating along the c axis. Due to the presence of four coordinately unsaturated sites per one metal cluster, an activated form of compound 1 (i.e., desolvated form denoted as 1') was tested in gas adsorption and catalytic experiments. The studies of gas sorption revealed that 1' exhibits a surface area (Brunauer-Emmett-Teller) of 980 m(2).g(-1). This value is the highest reported for any compound from the MTB group. Interactions of carbon dioxide (CO2) molecules with the framework, confirmed by density functional theory calculations, resulted in high CO(2)uptake and significant selectivity of CO, adsorption with respect to methane (CH4) and dinitrogen (N-2) when measured from atmospheric pressure to 21 bar. The high selectivity of CO2 over N-2 is mostly important for capturing CO2 from the atmosphere in attempts to decrease the greenhouse effect. Moreover, compound 1' was tested as a heterogeneous catalyst in Knoevenagel condensation of active methylene compounds with aldehydes. Excellent catalytic conversion and selectivity in the condensation of benzaldehyde and cyclohexanecarbaldehyde with malononitrile was observed, which suggests that accessible lead(II) sites play an important role in the heterogeneous catalytic process. Workplace J. Heyrovsky Institute of Physical Chemistry Contact Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196 Year of Publishing 2019
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