Kobayashi Hirokazu, Taylor Jared M, Mitsuka Yuko, Ogiwara Naoki, Yamamoto Tomokazu, Toriyama Takaaki, Matsumura Syo, Kitagawa Hiroshi
Division of Chemistry , Graduate School of Science , Kyoto University , Kitashirakawa-Oiwakecho, Sakyo-ku , Kyoto , 606-8502 , Japan . Email:
JST , PRESTO , 4-1-8 Honcho , Kawaguchi , Saitama 332-0012 , Japan.
Chem Sci. 2019 Feb 6;10(11):3289-3294. doi: 10.1039/c8sc05441j. eCollection 2019 Mar 21.
We report the synthesis and characterization of highly active Cu nanoparticles covered with zirconium/hafnium-based metal-organic frameworks for CO hydrogenation to methanol. Compared to , , and composites, UiO-66 acts as the most active support, with producing methanol at a rate 70 times higher than that of . In addition, the replacement of Zr with Hf in UiO-66 tripled in the rate of methanol production. Furthermore, we describe a substituent effect on the catalytic activity, with providing a three-fold enhancement of methanol production, compared to that of or . The enhanced catalytic activity of Cu nanoparticles depends on the charge transfer degree from Cu nanoparticles to UiO-66 at the interface between Cu nanoparticles and UiO-66.
我们报道了用于将一氧化碳加氢制甲醇的、覆盖有锆/铪基金属有机框架的高活性铜纳米颗粒的合成与表征。与 、 、 和 复合材料相比，UiO-66作为最具活性的载体， 生成甲醇的速率比 高70倍。此外，在UiO-66中用铪替代锆使甲醇生成速率提高了两倍。此外，我们描述了取代基对催化活性的影响，与 或 相比， 使甲醇生成量提高了两倍。铜纳米颗粒催化活性的增强取决于铜纳米颗粒与UiO-66界面处从铜纳米颗粒到UiO-66的电荷转移程度。
