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Microporous Lead-Organic Framework for Selective CO2 Adsorption and Heterogeneous Catalysis

SYSNO ASEP	0498940
Druh ASEP	J - Článek v odborném periodiku
Zařazení RIV	J - Článek v odborném periodiku
Poddruh J	Článek ve WOS
Název	Microporous Lead-Organic Framework for Selective CO2 Adsorption and Heterogeneous Catalysis
Tvůrce(i)	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, SAI}
Zdroj.dok.	Inorganic Chemistry. - : American Chemical Society - ISSN 0020-1669 Roč. 57, č. 4 (2018), s. 1774-1786
Poč.str.	13 s.
Jazyk dok.	eng - angličtina
Země vyd.	US - Spojené státy americké
Klíč. slova	secondary building units ; gas-adsorption ; carbon-dioxide ; porous materials ; base catalyst ; metal sites
Vědní obor RIV	CF - Fyzikální chemie a teoretická chemie
Obor OECD	Physical chemistry
CEP	GBP106/12/G015 GA ČR - Grantová agentura ČR
Institucionální podpora	UFCH-W - RVO:61388955
UT WOS	000426014800013
EID SCOPUS	85042222303
DOI	10.1021/acs.inorgchem.7b02491
Anotace	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.
Pracoviště	Ústav fyzikální chemie J.Heyrovského
Kontakt	Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196
Rok sběru	2019

Počet záznamů: 1