Core-shell metal-organic frameworks and metal functionalization to access highest efficiency in catalytic carboxylation
| Parent link: | Journal of Catalysis Vol. 371.— 2019.— [P. 106-115] |
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| Corporate Author: | |
| Other Authors: | , , , , , , , |
| Summary: | Title screen A core-shell metal-organic frameworks (MOF@MOF) based on the Zr-MOFs assembly from core-structure UiO-66 combined with shell-structure UiO-67-BPY were explored. The synthesized materials were characterized via XRD, FTIR, SEM, TEM, and surface area analysis, etc. indicating the presence of a core-shell structure of UiO-66@UiO-67-BPY. Furthermore, incorporation of the bipyridinic (BPY) group in the linker used to construct the shell layer (UiO-67-BPY) could coordinate with active metal species and thus create an advantage for site-selective metal incorporation in the core-shell structure. Silver (Ag) was selected for the selective metal incorporation and an excellent Ag-dispersion via coordination with the bipyridinic groups in the UiO-67-BPY layer of the core-shell material was obtained. The synthesized material (UiO-66@UiO-67-BPY-Ag) was successfully applied as a heterogeneous catalyst for the CO2 fixation via carboxylation of terminal alkynes. The catalytic material showed excellent yields using at a low Ag-loading under mild reaction condition (50?°C, 1?bar). Moreover, the catalyst can be recycled for at least 5 times maintaining a stable catalytic performance. Interestingly, the high catalytic activity of the synthesized material demonstrated clearly the beneficial advantage of the metalated core-shell structure over the reported routes to synthesize silver catalysts such as encapsulated Ag nanoparticles (AgNP@MOF) or Ag-bidentately coordinated on traditional MOFs applying the same reaction model. Режим доступа: по договору с организацией-держателем ресурса |
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2019
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| Subjects: | |
| Online Access: | https://doi.org/10.1016/j.jcat.2019.01.036 |
| Format: | Electronic Book Chapter |
| KOHA link: | https://koha.lib.tpu.ru/cgi-bin/koha/opac-detail.pl?biblionumber=660257 |
| Summary: | Title screen A core-shell metal-organic frameworks (MOF@MOF) based on the Zr-MOFs assembly from core-structure UiO-66 combined with shell-structure UiO-67-BPY were explored. The synthesized materials were characterized via XRD, FTIR, SEM, TEM, and surface area analysis, etc. indicating the presence of a core-shell structure of UiO-66@UiO-67-BPY. Furthermore, incorporation of the bipyridinic (BPY) group in the linker used to construct the shell layer (UiO-67-BPY) could coordinate with active metal species and thus create an advantage for site-selective metal incorporation in the core-shell structure. Silver (Ag) was selected for the selective metal incorporation and an excellent Ag-dispersion via coordination with the bipyridinic groups in the UiO-67-BPY layer of the core-shell material was obtained. The synthesized material (UiO-66@UiO-67-BPY-Ag) was successfully applied as a heterogeneous catalyst for the CO2 fixation via carboxylation of terminal alkynes. The catalytic material showed excellent yields using at a low Ag-loading under mild reaction condition (50?°C, 1?bar). Moreover, the catalyst can be recycled for at least 5 times maintaining a stable catalytic performance. Interestingly, the high catalytic activity of the synthesized material demonstrated clearly the beneficial advantage of the metalated core-shell structure over the reported routes to synthesize silver catalysts such as encapsulated Ag nanoparticles (AgNP@MOF) or Ag-bidentately coordinated on traditional MOFs applying the same reaction model. Режим доступа: по договору с организацией-держателем ресурса |
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| DOI: | 10.1016/j.jcat.2019.01.036 |