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

Kód výsledku v 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>

Výsledek na webu

<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>

Jazyk výsledku

angličtina

Název v původním jazyce

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

Popis výsledku v původním jazyce

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.

Název v anglickém jazyce

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

Popis výsledku anglicky

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.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/GBP106%2F12%2FG015" target="_blank" >GBP106/12/G015: Vývoj nových nanoporézních adsorbentů a katalyzátorů</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2018

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Inorganic Chemistry

ISSN

0020-1669

e-ISSN

—

Svazek periodika

57

Číslo periodika v rámci svazku

4

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

13

Strana od-do

1774-1786

Kód UT WoS článku

000426014800013

EID výsledku v databázi Scopus

2-s2.0-85042222303