Investigating the Influence of Reaction Conditions and the Properties of Ceria for the Valorisation of Glycerol
Investigating the Influence of Reaction Conditions and the Properties of Ceria for the Valorisation of Glycerol
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DOI：
10.3390/en12071359
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发表时间：
2019-04
期刊：
影响因子：
3.2
通讯作者：
Paul J. Smith;Louise R. Smith;N. Dummer;Mark Douthwaite;D. Willock;M. Howard;D. Knight;S. Taylor-S.-Ta
中科院分区：
文献类型：
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作者：
Paul J. Smith;Louise R. Smith;N. Dummer;Mark Douthwaite;D. Willock;M. Howard;D. Knight;S. Taylor-S.-Ta
研究了甘油水溶液在一系列氧化铈催化剂上的反应，制备生物可再生甲醇。产物分布受反应温度和催化剂接触时间的影响较大。对于50重量%的甘油，实现了21%的甘油转化率。甘油溶液，在CeO 2（8 m2 g−1）上，320 °C。碳质量平衡> 99%，主要产物为羟基丙酮。相比之下，在440 °C下，转化率和碳质量平衡分别> 99.9%和76%。乙醛和甲醇是在此较高温度下的主要产物，因为两者都可以由羟基丙酮形成。甲醇在320 °C和440 °C下的时空产率（STY）分别为15.2和145 gMeOH kgcat−1 h−1。制备新鲜CeO 2并在不同温度下煅烧，测定其织构性质，并研究其对等转化率和恒定床表面积下产物分布的影响。没有注意到甘油转化率或产物选择性的明显差异。因此，我们得出结论，CeO 2的表面积似乎不会影响甲醇和甘油转化形成的其他产物的反应选择性。
The reaction of aqueous glycerol over a series of ceria catalysts is investigated, to produce bio-renewable methanol. Product distributions were greatly influenced by the reaction temperature and catalyst contact time. Glycerol conversion of 21% was achieved for a 50 wt.% glycerol solution, over CeO2 (8 m2 g−1) at 320 °C. The carbon mass balance was >99 % and the main product was hydroxyacetone. In contrast, at 440 °C the conversion and carbon mass balance were >99.9 % and 76 % respectively. Acetaldehyde and methanol were the major products at this higher temperature, as both can be formed from hydroxyacetone. The space-time yield (STY) of methanol at 320 °C and 440 °C was 15.2 and 145 gMeOH kgcat−1 h−1 respectively. Fresh CeO2 was prepared and calcined at different temperatures, the textural properties were determined and their influence on the product distribution at iso-conversion and constant bed surface area was investigated. No obvious differences to the glycerol conversion or product selectivity were noted. Hence, we conclude that the surface area of the CeO2 does not appear to influence the reaction selectivity to methanol and other products formed from the conversion of glycerol.