Charge transfer dependence on CO2 hydrogenation activity to methanol in Cu nanoparticles covered with metal-organic framework systems
Charge transfer dependence on CO2 hydrogenation activity to methanol in Cu nanoparticles covered with metal-organic framework systems
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DOI：
10.1039/c8sc05441j
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发表时间：
2019-03-21
期刊：
影响因子：
8.4
通讯作者：
Kitagawa, Hiroshi
中科院分区：
文献类型：
--
作者：
Kobayashi, Hirokazu;Taylor, Jared M.;Kitagawa, Hiroshi
我们报道了锆/铪基金属有机骨架覆盖的高活性Cu纳米颗粒的合成和表征，用于CO2加氢制甲醇。与Cu/g-Al2O3、Cu/ZIF-8、Cu/MIL-100和Cu/UiO-66复合材料相比，UiO-66是最活跃的载体，Cu/Zr-UiO-66生成甲醇的速率是Cu/ γ - al2o3的70倍。此外，在UiO-66中用Hf4+取代Zr4+使甲醇的生产速度提高了两倍。此外，我们描述了取代基对催化活性的影响，与zr - uio66或ZrUiO66- NH2相比，Cu/Zr-UiO66-COOH的甲醇产量提高了三倍。Cu纳米颗粒催化活性的增强取决于Cu纳米颗粒与UiO-66界面处Cu纳米颗粒向UiO-66的电荷转移程度。
We report the synthesis and characterization of highly active Cu nanoparticles covered with zirconium/ hafnium-based metal-organic frameworks for CO2 hydrogenation to methanol. Compared to Cu/g-Al2O3, Cu/ZIF-8, Cu/MIL-100 and Cu/UiO-66 composites, UiO-66 acts as the most active support, with Cu/Zr-UiO-66 producing methanol at a rate 70 times higher than that of Cu/gamma-Al2O3. In addition, the replacement of Zr4+ with Hf4+ in UiO-66 tripled in the rate of methanol production. Furthermore, we describe a substituent effect on the catalytic activity, with Cu/Zr-UiO66-COOH providing a three-fold enhancement of methanol production, compared to that of Zr-UiO-66 or ZrUiO66- NH2. 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.