Direct deoxygenation of lignin model compounds into aromatic hydrocarbons through hydrogen transfer reaction

Direct deoxygenation of lignin model compounds into aromatic hydrocarbons through hydrogen transfer reaction
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木质素模型化合物通过氢转移反应直接脱氧生成芳香烃

DOI:
10.1016/j.apcata.2017.07.050
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发表时间:
2017-10
期刊:
Applied Catalysis A: General
影响因子:
--
通讯作者:
Wang Yanqin
Wang Yanqin
中科院分区:
其他
文献类型:
--
作者:
Guo Tianye;Xia Qineng;Shao Yi;Liu Xiaohui;Wang Yanqin

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以2-PrOH为氢供体,Ru/Nb 2 O 5-SiO2为催化剂,通过催化氢转移反应将木质素模型化合物直接脱氧为芳烃。结果表明,Ru/Nb_2O_5-SiO_2催化剂在230 °C下对甲酚的加氢脱氧反应具有良好的催化活性,转化率为98.5%,甲苯收率为84.0%,这是由于Nb_2O_5物种对C-单键-O键断裂的显著促进作用和Ru具有适当的转移加氢活性所致。此外,Ru/Nb 2 O 5-SiO2催化剂在2-PrOH供氢下,对各种木质素模型化合物如2-甲氧基-4-甲基苯酚、苄基苯基醚(α-O-4模型化合物)、2-(2-甲氧基苯基)氧基-1-苯乙醇(β-O-4模型化合物)以及从桦树中提取的真实的木质素的加氢脱氧反应中也表现出了优异的性能。对这些模型化合物的反应路径研究表明,在2-PrOH存在下,Ru/Nb 2 O 5-SiO2催化剂上的反应主要是直接脱氧(DDO)反应。在这里,发现使用2-PrOH作为氢源比使用分子氢对芳烃更有选择性。本工作为可再生木质素催化氢转移反应高选择性生产芳烃提供了新的途径。
A new route is reported for the direct deoxygenation of lignin model compounds to aromatic hydrocarbons via the catalytic hydrogen transfer reactions over Ru/Nb2O5-SiO2catalyst with 2-PrOH as a hydrogen donor. It is found that Ru/Nb2O5-SiO2catalyst is active for the hydrodeoxygenation ofp-cresol with 98.5% conversion and 84.0% yield of toluene at 230 °C, owing to the significant promotion effect of NbOxspecies on Csingle bondO bond cleavage and the proper transfer hydrogenation activity of Ru. Furthermore, Ru/Nb2O5-SiO2catalyst also shows excellent performances in the transfer hydrodeoxygenation of various lignin model compounds such as 2-methoxy-4-methyl phenol, benzyl phenyl ether (α-O-4 model compound), 2-(2-methoxyphenyl)oxy-1-phenethanol (β-O-4 model compound) and even the real lignin extracted from birch, into aromatic hydrocarbons with 2-PrOH as the hydrogen donor. The reaction pathway studies of these model compounds demonstrate that the direct deoxygenation (DDO) is the main reaction route over Ru/Nb2O5-SiO2catalyst in the presence of 2-PrOH. Here, using 2-PrOH as a hydrogen source is found to be more selective to aromatic hydrocarbons than using molecular hydrogen. This work provides a new way for the high selective production of aromatic hydrocarbons from renewable ligninviathe catalytic hydrogen transfer reactions.
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