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Published on: December 6, 2021
Copper Nanocrystals Encapsulated in Zr-based Metal-Organic Frameworks for Highly Selective CO2 Hydrogenation to
Bunyarat Rungtaweevoranit1, Jayeon Baek1, Joyce R Araujo1,2
1Department of Chemistry, University of California-Berkeley, Kavli Energy NanoSciences Institute , Berkeley, California 94720, United States.
Abstract:
We show that the activity and selectivity of Cu catalyst can be promoted by a Zr-based metal-organic framework (MOF), Zr6O4(OH)4(BDC)6 (BDC = 1,4-benzenedicarboxylate), UiO-66, to have a strong interaction with Zr oxide [Zr6O4(OH)4(-CO2)12] secondary building units (SBUs) of the MOF for CO2 hydrogenation to methanol. These interesting features are achieved by a catalyst composed of 18 nm single Cu nanocrystal (NC) encapsulated within single crystal UiO-66 (Cu⊂UiO-66). The performance of this catalyst construct exceeds the benchmark Cu/ZnO/Al2O3 catalyst and gives a steady 8-fold enhanced yield and 100% selectivity for methanol. The X-ray photoelectron spectroscopy data obtained on the surface of the catalyst show that Zr 3d binding energy is shifted toward lower oxidation state in the presence of Cu NC, suggesting that there is a strong interaction between Cu NC and Zr oxide SBUs of the MOF to make a highly active Cu catalyst.
