Copper Nanocrystals Encapsulated in Zr-based Metal–Organic Frameworks for Highly Selective CO2 Hydrogenation to Methanol

详细信息    查看全文

• 作者：Bunyarat Rungtaweevoranit ; Jayeon Baek ; Joyce R. Araujo ; Braulio S. Archanjo ; Kyung Min Choi ; Omar M. Yaghi ; Gabor A. Somorjai
• 刊名：Nano Letters
• 出版年：2016
• 出版时间：December 14, 2016
• 年：2016
• 卷：16
• 期：12
• 页码：7645-7649
• 全文大小：352K
• ISSN：1530-6992

文摘

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.