Direct Conversion of Bio-ethanol to Isobutene on Nanosized Zn x Zr y O z Mixed Oxides with Balanced Acid–Base Sites
We report the design and synthesis of nanosized Zn x Zr y O z mixed oxides for direct and high-yield conversion of bio-ethanol to isobutene (∼83%). ZnO is addded to ZrO2 to selectively passivate zirconia’s strong Lewis acidic sites and weaken Brönsted acidic sites, while simultaneously introducing...
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| Published in | Journal of the American Chemical Society Vol. 133; no. 29; pp. 11096 - 11099 |
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| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Chemical Society
27.07.2011
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| Online Access | Get full text |
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| Abstract | We report the design and synthesis of nanosized Zn x Zr y O z mixed oxides for direct and high-yield conversion of bio-ethanol to isobutene (∼83%). ZnO is addded to ZrO2 to selectively passivate zirconia’s strong Lewis acidic sites and weaken Brönsted 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 Brönsted acidic site-catalyzed acetone-to-isobutene reaction pathway dominates on the nanosized Zn x Zr y O z mixed oxide catalyst, leading to a highly selective process for direct conversion of bio-ethanol to isobutene. |
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| AbstractList | We report the design and synthesis of nanosized Zn x Zr y O z mixed oxides for direct and high-yield conversion of bio-ethanol to isobutene (∼83%). ZnO is addded to ZrO2 to selectively passivate zirconia’s strong Lewis acidic sites and weaken Brönsted 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 Brönsted acidic site-catalyzed acetone-to-isobutene reaction pathway dominates on the nanosized Zn x Zr y O z mixed oxide catalyst, leading to a highly selective process for direct conversion of bio-ethanol to isobutene. |
| Author | Peden, Charles H. F Sun, Junming Zhu, Kake Gao, Feng Wang, Chongmin Liu, Jun Wang, Yong |
| Author_xml | – sequence: 1 givenname: Junming surname: Sun fullname: Sun, Junming – sequence: 2 givenname: Kake surname: Zhu fullname: Zhu, Kake – sequence: 3 givenname: Feng surname: Gao fullname: Gao, Feng – sequence: 4 givenname: Chongmin surname: Wang fullname: Wang, Chongmin – sequence: 5 givenname: Jun surname: Liu fullname: Liu, Jun – sequence: 6 givenname: Charles H. F surname: Peden fullname: Peden, Charles H. F – sequence: 7 givenname: Yong surname: Wang fullname: Wang, Yong email: yong.wang@pnl.gov |
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