Microporous Lead-Organic Framework for Selective CO2 Adsorption and Heterogeneous Catalysis
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F18%3A00498940" target="_blank" >RIV/61388955:_____/18:00498940 - isvavai.cz</a>
Result on the web
<a href="http://dx.doi.org/10.1021/acs.inorgchem.7b02491" target="_blank" >http://dx.doi.org/10.1021/acs.inorgchem.7b02491</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1021/acs.inorgchem.7b02491" target="_blank" >10.1021/acs.inorgchem.7b02491</a>
Alternative languages
Result language
angličtina
Original language name
Microporous Lead-Organic Framework for Selective CO2 Adsorption and Heterogeneous Catalysis
Original language description
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.
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10403 - Physical chemistry
Result continuities
Project
<a href="/en/project/GBP106%2F12%2FG015" target="_blank" >GBP106/12/G015: Intelligent design of nanoporous adsorbents and catalysts</a><br>
Continuities
P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)
Others
Publication year
2018
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
Inorganic Chemistry
ISSN
0020-1669
e-ISSN
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Volume of the periodical
57
Issue of the periodical within the volume
4
Country of publishing house
US - UNITED STATES
Number of pages
13
Pages from-to
1774-1786
UT code for WoS article
000426014800013
EID of the result in the Scopus database
2-s2.0-85042222303