mevalonolactone;
isoprene;
ring opening;
decarboxylation;
aluminosilicates;
GAMMA-VALEROLACTONE;
BIOMASS;
ACID;
SITES;
D O I:
10.1021/acscatal.0c01438
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
Isoprene production from biomass via solely biochemical processes is inherently limited by the low yields of the biological pathways. In this work, we demonstrate that isoprene can be efficiently produced via a hybrid bio/thermochemical process, combining the efficient fermentation of cellulosic sugars to mevalonolactone (MVL) with the acid-catalyzed MVL decarboxylation to isoprene. We report herein the thermochemical conversion of MVL to isoprene over inexpensive amorphous SiO2/Al2O3. A detailed investigation into the reaction conditions and the Si/AI ratio shows that isoprene formation is maximized over high-SiO2-content samples at mild temperatures (225-250 degrees C) that prevent its secondary oligomerization to alkylated aromatics and cyclic olefins. The highest isoprene yield is attained over SiO2/Al2O3 with 90 wt % SiO2 at 250 degrees C and 1.4 h(-1), corresponding to similar to 60% of the theoretical maximum. Acidity-performance correlations reveal the key role of Bronsted acidity in the reaction.
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Abdelrahman, Omar A.
Park, Dae Sung
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h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Natl Sci Fdn Ctr Chem Innovat, Ctr Sustainable Polymers, 209 Smith Hall,207 Pleasant St SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Park, Dae Sung
Vinter, Katherine P.
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h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Vinter, Katherine P.
Spanjers, Charles S.
论文数: 0引用数: 0
h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Natl Sci Fdn Ctr Chem Innovat, Ctr Sustainable Polymers, 209 Smith Hall,207 Pleasant St SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Spanjers, Charles S.
Ren, Limin
论文数: 0引用数: 0
h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Ren, Limin
论文数: 引用数:
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机构:
Cho, Hong Je
Zhang, Kechun
论文数: 0引用数: 0
h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Natl Sci Fdn Ctr Chem Innovat, Ctr Sustainable Polymers, 209 Smith Hall,207 Pleasant St SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Zhang, Kechun
Fan, Wei
论文数: 0引用数: 0
h-index: 0
机构:
Univ Massachusetts, Dept Chem Engn, 686 North Pleasant St, Amherst, MA 01003 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Fan, Wei
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机构:
Tsapatsis, Michael
Dauenhauer, Paul J.
论文数: 0引用数: 0
h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Natl Sci Fdn Ctr Chem Innovat, Ctr Sustainable Polymers, 209 Smith Hall,207 Pleasant St SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Abdelrahman, Omar A.
Park, Dae Sung
论文数: 0引用数: 0
h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Natl Sci Fdn Ctr Chem Innovat, Ctr Sustainable Polymers, 209 Smith Hall,207 Pleasant St SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Park, Dae Sung
Vinter, Katherine P.
论文数: 0引用数: 0
h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Vinter, Katherine P.
Spanjers, Charles S.
论文数: 0引用数: 0
h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Natl Sci Fdn Ctr Chem Innovat, Ctr Sustainable Polymers, 209 Smith Hall,207 Pleasant St SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Spanjers, Charles S.
Ren, Limin
论文数: 0引用数: 0
h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Ren, Limin
论文数: 引用数:
h-index:
机构:
Cho, Hong Je
Zhang, Kechun
论文数: 0引用数: 0
h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Natl Sci Fdn Ctr Chem Innovat, Ctr Sustainable Polymers, 209 Smith Hall,207 Pleasant St SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Zhang, Kechun
Fan, Wei
论文数: 0引用数: 0
h-index: 0
机构:
Univ Massachusetts, Dept Chem Engn, 686 North Pleasant St, Amherst, MA 01003 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Fan, Wei
论文数: 引用数:
h-index:
机构:
Tsapatsis, Michael
Dauenhauer, Paul J.
论文数: 0引用数: 0
h-index: 0
机构:
Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
Natl Sci Fdn Ctr Chem Innovat, Ctr Sustainable Polymers, 209 Smith Hall,207 Pleasant St SE, Minneapolis, MN 55455 USAUniv Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA