Depolymerization and hydrodeoxygenation of lignin to aromatic hydrocarbons with a Ru catalyst on a variety of Nb-based supports
Depolymerization and hydrodeoxygenation of lignin to aromatic hydrocarbons with a Ru catalyst on a variety of Nb-based supports
复制标题
在各种铌基载体上使用 Ru 催化剂将木质素解聚和加氢脱氧为芳香烃
DOI：
10.1016/s1872-2067(19)63317-6
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发表时间：
2019-04-01
影响因子：
16.5
通讯作者：
Wang, Yanqin
中科院分区：
文献类型：
--
作者：
Ma, Di;Lu, Shenglu;Wang, Yanqin
通过解聚和随后的加氢脱氧有效地将木质素转化为芳香烃是很重要的。以前，我们发现NbOX物种在木质素及其模型化合物中C-O键的活化和断裂中起着关键作用。本研究以商品铌酸(HY-340)、磷酸铌(NBPO-CBMM)和自制的层状氧化铌层(Nb2Os-Layer)为载体，研究了Bronsted酸和Lewis酸对木素转化过程中C-O键活化的影响。制备了不同Ru颗粒大小的负载Ru的Nb基催化剂，并将其用于对甲酚的转化。结果表明，所有Ru/Nb基催化剂都能产生较高的C-7-C-9烃的摩尔产率(82.3%-99.1%)。此外，Ru/Nb2O5-层对C-7-C-9烃的摩尔产率和对C-7-C-9芳香烃的选择性最高，分别达到99.1%和88.0%。此外，还发现Lewis酸中心在酶木素解聚为酚类单体和酚的C-O键断裂过程中起着重要作用。此外，Ru的电子态和颗粒大小是影响芳香烃选择性的重要因素。金属Ru表面的部分正电荷和较小的Ru颗粒尺寸有利于提高芳香烃的选择性。(C)2019年，中国科学院大连化学物理研究所。爱思唯尔出版，版权所有。
Efficient conversion of lignin to aromatic hydrocarbons via depolymerization and subsequent hydrodeoxygenation is important. Previously, we found that NbOX species played a key role in the activation and cleavage of C-O bonds in lignin and its model compounds. In this study, commercial niobic acid (HY-340), niobium phosphate (NbPO-CBMM) and lab-made layered niobium oxide (Nb2Os-Layer) were chosen as supports to study the effect of Bronsted and Lewis acids on the activation of C-O bonds in lignin conversion. A variety of Ru-loaded, Nb-based catalysts with different Ru particle sizes were prepared and applied to the conversion of p-cresol. The results show that all the Ru/Nb-based catalysts produce high mole yields of C-7-C-9 hydrocarbons (82.3%-99.1%). What's more, Ru/Nb2O5-Layer affords the best mole yield of C-7-C-9 hydrocarbons and selectivity for C-7-C-9 aromatic hydrocarbons, of up to 99.1% and 88.0%, respectively. Moreover, it was found that Lewis acid sites play important roles in the depolymerization of enzymatic lignin into phenolic monomers and the cleavage of the C-O bond of phenols. Additionally, the electronic state and particle size of Ru are significant factors which influence the selectivity for aromatic hydrocarbons. A partial positive charge on the metallic Ru surface and a smaller Ru particle size are beneficial in improving the selectivity for aromatic hydrocarbons. (C) 2019, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.