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Production of renewable alcohols from maple wood using supercritical methanol hydrodeoxygenation in a semi-continuous flowthrough reactor
Green Chemistry ( IF 9.8 ) Pub Date : 2020-11-10 , DOI: 10.1039/d0gc03218b
Peter H. Galebach 1, 2, 3, 4 , Jimmy K. Soeherman 1, 2, 3, 4 , Elise Gilcher 1, 2, 3, 4 , Ashley M. Wittrig 4, 5, 6 , Jillian Johnson 4, 5, 6 , Thomas Fredriksen 4, 5, 6 , Chengrong Wang 4, 5, 6 , Michael P. Lanci 4, 5, 6 , James A. Dumesic 1, 2, 3, 4 , George W. Huber 1, 2, 3, 4
Affiliation  

Biomass conversion to alcohols using supercritical methanol depolymerization and hydrodeoxygenation (SCM-DHO) with CuMgAl mixed metal oxide is a promising process for biofuel production. We demonstrate how maple wood can be converted at high weight loadings and product concentrations in a batch and a semi-continuous reactor to a mixture of C2–C10 linear and cyclic alcohols. Maple wood was solubilized semi-continuously in supercritical methanol and then converted to a mixture of C2–C9 alcohols and aromatics over a packed bed of CuMgAlOx catalyst. Up to 95 wt% of maple wood can be solubilized in the methanol by using four temperature holds at 190, 230, 300, and 330 °C. Lignin was solubilized at 190 and 230 °C to a mixture of monomers, dimers, and trimers while hemicellulose and cellulose solubilized at 300 and 330 °C to a mixture of oligomeric sugars and liquefaction products. The hemicellulose, cellulose, and lignin were converted to C2–C10 alcohol fuel precursors over a packed bed of CuMgAlOx catalyst with 70–80% carbon yield of the entire maple wood. The methanol reforming activity of the catalyst decreased by 25% over four beds of biomass, which corresponds to 5 turnovers for the catalyst, but was regenerable after calcination and reduction. In batch reactions, maple wood was converted at 10 wt% in methanol with 93% carbon yield to liquid products. The product concentration can be increased to 20 wt% by partially replacing the methanol with liquid products. The yield of alcohols in the semi-continuous reactor was approximately 30% lower than in batch reactions likely due to degradation of lignin and cellulose during solubilization. These results show that solubilization of whole biomass can be separated from catalytic conversion of the intermediates while still achieving a high yield of products. However, close contact of the catalyst and the biomass during solubilization is critical to achieve the highest yields and concentration of products.

中文翻译:

在半连续流通式反应器中使用超临界甲醇加氢脱氧从枫木生产可再生醇

使用超临界甲醇解聚和加氢脱氧(SCM-DHO)与CuMgAl混合金属氧化物将生物质转化为醇是一种有前途的生物燃料生产方法。我们展示了枫木如何在一批和一个半连续反应器中以高重量负荷和产品浓度转化为C 2 -C 10线性和环状醇的混合物。枫木在超临界甲醇中半连续溶解,然后在填充的CuMgAlO x床上转化为C 2 -C 9醇和芳烃的混合物催化剂。通过在190、230、300和330°C下保持四个温度,最多可将95%(重量)的枫木溶解在甲醇中。木质素在190和230℃下增溶为单体,二聚体和三聚体的混合物,而半纤维素和纤维素在300和330℃下增溶为低聚糖和液化产物的混合物。在CuMgAlO x的填充床上,将半纤维素,纤维素和木质素转化为C 2 –C 10酒精燃料前体。整个枫木的碳产率为70-80%的催化剂。在四个生物质床上,催化剂的甲醇重整活性降低了25%,相当于催化剂的5次转化,但在煅烧和还原后可再生。在分批反应中,将枫木在甲醇中的含量为10 wt%,碳产率为93%,转化为液体产品。通过用液体产物部分代替甲醇,产物浓度可以增加到20wt%。半连续反应器中的醇收率比间歇反应中的醇收率低约30%,这可能是由于增溶过程中木质素和纤维素的降解。这些结果表明,可以从中间体的催化转化中分离出整个生物质的增溶,同时仍然获得高产率的产物。然而,
更新日期:2020-11-17
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