4.8 Article

Direct Conversion of Bio-ethanol to Isobutene on Nanosized ZnxZryOz Mixed Oxides with Balanced Acid-Base Sites

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 133, 期 29, 页码 11096-11099

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AMER CHEMICAL SOC
DOI: 10.1021/ja204235v

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  1. US Department of Energy (DOE), Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences
  2. DOE's Office of Biological and Environmental Research
  3. DOE [DE-AC05-76RL01830]

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We report the design and synthesis of nanosized ZnxZryOz mixed oxides for direct and high-yield conversion of bio-ethanol to isobutene (similar to 83%). ZnO is addded to ZrO2 to selectively passivate zirconia's strong Lewis acidic sites and weaken Bronsted acidic sites, while simultaneously introducing basicity. As a result, the undesired reactions of bio-ethanol dehydration and acetone polymerization/coking are suppressed. Instead, a surface basic site-catalyzed ethanol dehydrogenation to acetaldehyde, acetaldehyde to acetone conversion via a complex pathway including aldol-condensation/dehydrogenation, and a Bronsted acidic site-catalyzed acetone-to-isobutene reaction pathway dominates on the nanosized ZnxZryOz mixed oxide catalyst, leading to a highly selective process for direct conversion of bio-ethanol to isobutene.

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