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Selective production of arenes via direct lignin upgrading over a niobium-based catalyst

机译:通过木质素在铌基催化剂上的直接提质选择性生产芳烃

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摘要

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/Nb2O5 catalyst that enabled the complete removal of the oxygen content from lignin. The conversion of birch lignin to monomer C7–C9 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 Nb2O5 support is catalytically unique compared with other traditional oxide supports, and the disassociation energy of Caromatic–OH bonds in phenolics is significantly reduced upon adsorption on Nb2O5, resulting in its distinct selectivity to arenes. This one-pot process provides a promising approach for improved lignin valorization with general applicability.
机译:木质素是唯一大量可再生的芳香族化学物质。木质素的有效解聚和脱氧同时保持芳族官能度是有吸引力的,但极具挑战性。在这里,我们报告了在多孔Ru / Nb2O5催化剂上通过有机溶剂木质素的直接加氢脱氧选择性生产芳烃的方法,该催化剂能够从木质素中完全去除氧含量。桦木木质素向单体C7–C9烃的转化基于其单体含量几乎是定量的,总质量产率为35.5 wt%,出色的芳烃选择性为71 wt%。无弹性中子散射和DFT计算证实,Nb2O5载体与其他传统氧化物载体相比具有催化独特性,并且当吸附在Nb2O5上时,酚类中Caromatic-OH键的离解能大大降低,从而使其对芳烃的选择性显着降低。这种一锅法工艺提供了一种有希望的方法,可用于普遍应用的改进木质素增值。

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