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Effects of zirconia phase on the synthesis of methanol over zirconia-supported copper

Journal Article · · Catalysis Letters
OSTI ID:819461

A study has been conducted to identify the influence of zirconia phase and copper to zirconia surface area on the activity of Cu/ZrO2 catalysts for the synthesis of methanol from either CO/H2 or CO2/H2. To determine the effects of zirconia phase, a pair of Cu/ZrO2 catalysts were prepared on tetragonal (t-) and monoclinic (m-) zirconia. The zirconia surface area and the Cu dispersion were essentially identical for these two catalysts. At 548 K, 0.65 MPa, and H 2/COx (x=1,2)=3, the catalysts prepared on m-ZrO2 was 4.5 times more active for methanol synthesis from CO2/H2 than that prepared on t-ZrO2, and 7.5 times more active when CO/H2 was used as the feed. Increasing the surface area of m-ZrO2 and the ration of Cu to ZrO2 surface areas further increased the methanol synthesis activity. In situ infrared spectroscopy and transient-response experiments indicate that the higher rate of methanol synthesis from Co2/H2 over Cu/m-ZrO2 is due solely to the higher concentration of active intermediates. By contrast, the higher rate of methanol synthesis from Co/H2 is due to both a higher concentration of surface intermediates and the more rapid dynamics of their transformation over Cu/ZrO2.

Research Organization:
Ernest Orlando Lawrence Berkeley National Laboratory, Berkeley, CA (US)
Sponsoring Organization:
USDOE Director, Office of Science. Office of Basic Energy Sciences. Division of Chemical Sciences (US)
DOE Contract Number:
AC03-76SF00098
OSTI ID:
819461
Report Number(s):
LBNL--49410
Journal Information:
Catalysis Letters, Journal Name: Catalysis Letters Journal Issue: 1-2 Vol. 80; ISSN CALEER; ISSN 1011-372X
Country of Publication:
United States
Language:
English