Статья

Copper Nanocrystals Encapsulated in Zr-based Metal–Organic Frameworks for Highly Selective CO<sub>2</sub> Hydrogenation to Methanol

Bunyarat RungtaweevoranitDepartment of Chemistry, University of California−Berkeley, Kavli Energy NanoSciences Institute, Berkeley, California 94720, United StatesJayeon BaekDepartment of Chemistry, University of California−Berkeley, Kavli Energy NanoSciences Institute, Berkeley, California 94720, United StatesJoyce R. AraújoDepartment of Chemistry, University of California−Berkeley, Kavli Energy NanoSciences Institute, Berkeley, California 94720, United StatesBráulio S. ArchanjoMaterials Metrology Division, National Institute of Metrology, Quality, and Technology, Duque de Caxias, Rio de Janeiro 25250−020, BrazilKyung Min ChoiDepartment of Chemistry, University of California−Berkeley, Kavli Energy NanoSciences Institute, Berkeley, California 94720, United StatesOmar M. YaghiDepartment of Chemistry, University of California−Berkeley, Kavli Energy NanoSciences Institute, Berkeley, California 94720, United StatesGábor A. SomorjaiDepartment of Chemistry, University of California−Berkeley, Kavli Energy NanoSciences Institute, Berkeley, California 94720, United States

2016en

ABI

Аннотация

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.

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Идентификаторы

DOI: 10.1021/acs.nanolett.6b03637

Цитирования и источники

Цитирований: 2Использованных источников: 0

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