Core-shell metal-organic frameworks and metal functionalization to access highest efficiency in catalytic carboxylation

Yanyan Gong, Ye Yuan, Cheng Chen, Pan Zhang, Jichao Wang, Serge Zhuiykov, Somboon Chaemchuen, Francis Verpoort

Research output: Contribution to journalArticlepeer-review

7 Citations (Scopus)

Abstract

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.

Original languageEnglish
Pages (from-to)106-115
Number of pages10
JournalJournal of Catalysis
Volume371
DOIs
Publication statusPublished - 1 Mar 2019

Keywords

  • Carboxylation
  • CO fixation
  • Core-shell structure
  • Heterogeneous catalysis
  • MOF@MOF
  • Propiolic acids

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

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