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Selective Production of Oxygenates from Carbon Dioxide Hydrogenation over a Mesoporous‐Silica‐Supported Copper‐Gallium Nanocomposite Catalyst
ChemCatChem ( IF 3.8 ) Pub Date : 2018-02-16 , DOI: 10.1002/cctc.201701679 Amol M. Hengne 1 , Kushal D. Bhatte 1 , Samy Ould-Chikh 1 , Youssef Saih 1 , Jean Marie Basset 1 , Kuo-Wei Huang 1
ChemCatChem ( IF 3.8 ) Pub Date : 2018-02-16 , DOI: 10.1002/cctc.201701679 Amol M. Hengne 1 , Kushal D. Bhatte 1 , Samy Ould-Chikh 1 , Youssef Saih 1 , Jean Marie Basset 1 , Kuo-Wei Huang 1
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The hydrogenation of CO2 to oxygenates (methanol and dimethyl ether; DME) was investigated over bifunctional supported Cu catalysts promoted with Ga. The supported Cu‐Ga nanocomposite catalysts were characterized by using XRD, TEM with energy dispersive X‐ray spectroscopy, X‐ray photoelectron spectroscopy, and H2 temperature‐programmed reduction. In comparison with Cu‐SBA‐15‐based catalysts, the Ga‐promoted catalyst prepared by the urea deposition method (Cu‐Ga/SBA‐15‐UDP) was more active and selective for CO2 hydrogenation to oxygenates. The use of Ga as the promoter led to increased acidic sites, which was confirmed by using NH3 temperature‐programmed deposition and IR spectroscopy with pyridine and 2,6‐lutidine as probe molecules. The favorable effect of Ga on the CO2 conversion and selectivity to oxygenates may come from the strong interaction of Ga with silica, which is responsible for the enhanced metal surface area, the formation of the nanocomposite, and the metal dispersion. Notably, the incorporation of Ga into Cu/SiO2 led to a several‐fold higher rate for methanol formation (13.12 μmol gCu−1 s−1) with a reasonable rate for DME formation (2.15 μmol gCu−1 s−1) compared to Cu/SiO2 catalysts.
中文翻译：
介孔二氧化硅支撑的铜镓纳米复合催化剂上二氧化碳加氢选择性生产含氧化合物
在Ga促进的双功能负载型Cu催化剂上研究了CO 2加氢为含氧化合物（甲醇和二甲醚； DME）。使用XRD，TEM和能量色散X射线光谱法，X-表征了负载型Cu-Ga纳米复合催化剂。射线光电子能谱和H 2程序升温还原。与基于Cu-SBA-15的催化剂相比，通过尿素沉积法（Cu-Ga / SBA-15-UDP）制备的Ga促进的催化剂对CO 2加氢生成氧化物的活性和选择性更高。使用Ga作为促进剂会导致酸性位点增加，这可以通过使用NH 3来证实。吡啶和2,6-二甲基吡啶为探针分子的程序升温沉积和红外光谱。Ga对CO 2转化和对含氧化合物的选择性的有利影响可能来自Ga与二氧化硅的强相互作用，这与增加的金属表面积，纳米复合材料的形成和金属分散体有关。值得注意的是，Ga掺入Cu / SiO 2导致甲醇形成速率（13.12μmolg Cu -1 s -1）高出几倍，而DME形成速率合理（2.15μmolg Cu -1 s -1））与Cu / SiO 2催化剂相比。
更新日期：2018-02-16
中文翻译：
介孔二氧化硅支撑的铜镓纳米复合催化剂上二氧化碳加氢选择性生产含氧化合物
在Ga促进的双功能负载型Cu催化剂上研究了CO 2加氢为含氧化合物（甲醇和二甲醚； DME）。使用XRD，TEM和能量色散X射线光谱法，X-表征了负载型Cu-Ga纳米复合催化剂。射线光电子能谱和H 2程序升温还原。与基于Cu-SBA-15的催化剂相比，通过尿素沉积法（Cu-Ga / SBA-15-UDP）制备的Ga促进的催化剂对CO 2加氢生成氧化物的活性和选择性更高。使用Ga作为促进剂会导致酸性位点增加，这可以通过使用NH 3来证实。吡啶和2,6-二甲基吡啶为探针分子的程序升温沉积和红外光谱。Ga对CO 2转化和对含氧化合物的选择性的有利影响可能来自Ga与二氧化硅的强相互作用，这与增加的金属表面积，纳米复合材料的形成和金属分散体有关。值得注意的是，Ga掺入Cu / SiO 2导致甲醇形成速率（13.12μmolg Cu -1 s -1）高出几倍，而DME形成速率合理（2.15μmolg Cu -1 s -1））与Cu / SiO 2催化剂相比。
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