期刊
ACS CATALYSIS
卷 8, 期 9, 页码 7809-7819出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b01396
关键词
CO2 hydrogenation; Methanol synthesis; Copper; Zirconia; Amorphous; Mixed oxide
资金
- Japan Society for the Promotion of Science (JSPS) [15J10157]
- Grants-in-Aid for Scientific Research [15J10157] Funding Source: KAKEN
We examined the formation mechanism of active sites on Cu/ZrO2 specific toward CO2-to-methanol hydrogenation. The active sites on Cu/a-ZrO2 (a-: amorphous) were more suitable for CO2-to-methanol hydrogenation than those on Cu/t-ZrO2 (t-: tetragonal) and Cu/m-ZrO2 (m-: monoclinic). When a-ZrO2 was impregnated with a Cu(NO3)(2)center dot 3H(2)O solution and then calcined under air, most of the Cu species entered a-ZrO2, leading to the formation of a Cu-Zr mixed oxide (CuaZr1-aOb). The H-2 reduction of the thus-formed CuaZr1-aOb led to the formation of Cu nano-particles on a-ZrO2, which can be dedicated to CO2-to-methanol hydrogenation. We concluded that the selective synthesis of CuaZr1-aOb, especially amorphous CuaZr1-aOb, is a key feature of the catalyst preparation. The preparation conditions of the amorphous CuaZr1-aOb specific toward CO2-to-methanol hydrogenation is as follows: (i) Cu(NO3)(2)center dot 3H(2)O/a-ZrO2 is calcined at low temperature (350 degrees C in this study) and (ii) the Cu loading is low (6 and 8 wt % in this study). Via these preparation conditions, the characteristics of a-ZrO2 for the catalysts remained unchanged during the reaction at 230 degrees C. The latter preparation condition is related to the solubility limit of Cu species in a-ZrO2. Accordingly, we obtained the amorphous CuaZr1-aOb without forming crystalline CuO particles.
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