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Tungsten-Based Bimetallic Catalysts for Selective Cleavage of Lignin C-O Bonds

机译:基于钨的双金属催化剂,用于木质素C-O键的选择性切割

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摘要

Tungsten-based bimetallic catalysts M-W/AC (M=Ru, Pt, and Pd; AC=activated carbon) exhibited high activity and selectivity in the hydrogenolysis of typical -O-4 model compounds and deconstruction of lignin feedstock for the production of aromatic chemicals. Synergy effect was observed between tungsten and noble-metal species, which on the one hand modulated the hydrogenolysis activity of tungsten and improved the activity of catalyst, and on the other hand suppressed overhydrogenation that avoided the formation of cycloalkanes. The conversion of -O-4 model compounds with different substituents showed that electronic effects play an important role in stabilizing the reaction intermediates, and the electron-donating methoxy group on the aromatic ring accelerated the hydrogenolysis efficiency. Solvent effect was another factor that determined hydrogenolysis efficiency; dipolar aprotic solvents such as n-hexane provided the high yields of target aromatics. In the conversion of realistic lignins, the bimetallic catalyst showed excellent activity not only in -O-4 cleavage but also in the hydrogenolysis of other major linkages such as -O-4 and - between aromatic units, so that a high yield of liquid oil was obtained from lignin.
机译:基于钨的双金属催化剂MW / AC(M = Ru,Pt和Pd; Ac =活性炭)在典型-O-4模型化合物的氢解中表现出高活性和选择性,用于生产芳香化学品的木质素原料的解构。在钨和贵金属物种之间观察到协同效应,这在一方面调节钨的氢解活性并改善催化剂的活性,另一方面,抑制过氢化,避免形成环烷烃。 -O-4模型化合物与不同取代基的转化表明,电子效应在稳定反应中间体中发挥着重要作用,并且芳环上的电子给甲氧基加速了氢解效率。溶剂效应是确定氢解效率的另一个因素;诸如N-己烷的偶极非质子溶剂提供了高产率芳族的产量。在逼真的木质素的转化中,双金属催化剂不仅在-4-4裂解中表现出优异的活性,而且在其他主要键的氢解中出现,例如-O-4和 - 在芳族单元之间,因此高产液体油从木质素获得。

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