Dataset Information

Encapsulation of a Porous Organic Cage into the Pores of a Metal-Organic Framework for Enhanced CO2 Separation.

ABSTRACT: We present a facile approach to encapsulate functional porous organic cages (POCs) into a robust MOF by an incipient-wetness impregnation method. Porous cucurbit[6]uril (CB6) cages with high CO2 affinity were successfully encapsulated into the nanospace of Cr-based MIL-101 while retaining the crystal framework, morphology, and high stability of MIL-101. The encapsulated CB6 amount is controllable. Importantly, as the CB6 molecule with intrinsic micropores is smaller than the inner mesopores of MIL-101, more affinity sites for CO2 are created in the resulting CB6@MIL-101 composites, leading to enhanced CO2 uptake capacity and CO2 /N2 , CO2 /CH4 separation performance at low pressures. This POC@MOF encapsulation strategy provides a facile route to introduce functional POCs into stable MOFs for various potential applications.

SUBMITTER: Liang J

PROVIDER: S-EPMC7187261 | biostudies-literature | 2020 Apr

REPOSITORIES: biostudies-literature

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Encapsulation of a Porous Organic Cage into the Pores of a Metal-Organic Framework for Enhanced CO<sub>2</sub> Separation.

Liang Jun J Nuhnen Alexander A Millan Simon S Breitzke Hergen H Gvilava Vasily V Buntkowsky Gerd G Janiak Christoph C

Angewandte Chemie (International ed. in English) 20200203 15

We present a facile approach to encapsulate functional porous organic cages (POCs) into a robust MOF by an incipient-wetness impregnation method. Porous cucurbit[6]uril (CB6) cages with high CO<sub>2</sub> affinity were successfully encapsulated into the nanospace of Cr-based MIL-101 while retaining the crystal framework, morphology, and high stability of MIL-101. The encapsulated CB6 amount is controllable. Importantly, as the CB6 molecule with intrinsic micropores is smaller than the inner mes ...[more]

PMID: 31912916

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Project description:Metal-organic frameworks (MOFs) have been an excellent platform for carbon dioxide reduction reactions (CO2RR). In this work, the feasibility of electrochemical reduction of CO2 to obtain C2-deep value-added products was investigated by the preparation of Mg-containing MOF-74 samples combined with transition metal cations (Ni2+, Co2+ and Zn2+). The prepared MOFs were used as electrocatalysts in CO2RR. Chronoamperometric analysis coupled to ATR-FTIR spectroscopy was employed to characterize the CO2 reduction products and subsequently via 1H NMR. Although an isostructural crystalline structure was observed in all synthesized MOFs, the pore diameter distribution was significantly affected due to the Mg coordination along with each transition metal nuclei with the organic ligand to form the MOF-74. Our results showed that Mg-containing MOF-74 electrocatalysts combined with Ni, Co and Zn ions successfully reduced CO2 to C2-deep products, while the monometallic Mg-MOF-74 showed only CO2 mineralization. An ester acetate, isopropyl alcohol, and formic acid were produced by Mg/Ni-MOF-74; isopropyl alcohol was provided by Mg/Co-MOF-74, and ethanol was generated by Mg/Zn-MOF-74. We observed that the change of the transition cation was a key factor in the selectivity of the obtained products, while the degree of Mg ions effectively incorporated into the MOF structure tuned the porosity and the electrocatalytic activity. Among them, Mg/Zn-MFOF-74 showed the highest Mg content loaded after synthesis and thus the most favorable electrocatalytic behavior towards CO2 reduction. Highlights • CO2-derived C2-deep reduction products were obtained by Mg-containing MOF-74 bimetallic electrocatalysts.• Mg-containing MOF-74 bimetallic electrocatalysts reduced CO2 to ester acetate, isopropanol, formic acid, and ethanol.• Mg/Zn-MOF-74 displayed the highest current density at a lower onset potential in CO2-saturated electrolyte.• The pore network could be tuned by the effective Mg content on a MOF-74 bimetallic sample.• Mg/Zn-MOF-74 showed the highest Mg content among all bimetallic electrocatalysts after the synthesis.

Dataset Information

Encapsulation of a Porous Organic Cage into the Pores of a Metal-Organic Framework for Enhanced CO2 Separation.

Publications

Encapsulation of a Porous Organic Cage into the Pores of a Metal-Organic Framework for Enhanced CO<sub>2</sub> Separation.

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