Shanghai Key Laboratory of Functional Materials Chemistry, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China.
School of Chemistry, University of Manchester, Manchester M13 9PL, UK.
Nat Commun. 2017 Jul 24;8:16104. doi: 10.1038/ncomms16104.
Lignin is the only large-volume renewable source of aromatic chemicals. Efficient depolymerization and deoxygenation of lignin while retaining the aromatic functionality are attractive but extremely challenging. Here we report the selective production of arenes via direct hydrodeoxygenation of organosolv lignin over a porous Ru/NbO catalyst that enabled the complete removal of the oxygen content from lignin. The conversion of birch lignin to monomer C-C hydrocarbons is nearly quantitative based on its monomer content, with a total mass yield of 35.5 wt% and an exceptional arene selectivity of 71 wt%. Inelastic neutron scattering and DFT calculations confirm that the NbO support is catalytically unique compared with other traditional oxide supports, and the disassociation energy of C-OH bonds in phenolics is significantly reduced upon adsorption on NbO, resulting in its distinct selectivity to arenes. This one-pot process provides a promising approach for improved lignin valorization with general applicability.
木质素是唯一一种大宗可再生芳香族化学品资源。高效地将木质素解聚和脱氧，同时保留芳香族功能，这是极具吸引力但极具挑战性的。在此，我们报告了通过在多孔 Ru/NbO 催化剂上直接加氢脱氧，从有机溶剂木质素中选择性地生产芳烃。该催化剂能够使木质素中的氧含量完全去除。基于其单体含量，桦木木质素转化为单体 C-C 烃类的转化率几乎达到定量，总质量收率为 35.5wt%，芳烃选择性达到 71wt%。非弹性中子散射和 DFT 计算证实，与其他传统氧化物载体相比，NbO 载体具有独特的催化性能，酚类化合物中 C-OH 键的离解能在吸附到 NbO 上时显著降低，导致其对芳烃具有独特的选择性。该一锅法工艺为提高木质素的增值利用提供了一种很有前景的方法，具有广泛的适用性。
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