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Sinter-Resistant Nickel Catalyst for Lignin Hydrogenolysis Achieved by Liquid Phase Atomic Layer Deposition of Alumina

机译:液相原子层沉积氧化铝实现木质素氢解的耐烧结镍催化剂

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摘要

Lignin hydrogenolysis is a key step in the sustainable production ofrenewable bio-based chemicals and fuels. Heterogeneous metal catalystshave led to high yields but they rapidly deactivate, notably due to nanoparticlesintering and carbonaceous deposit formation. While these deposits can beremoved by regeneration, sintering is irreversible and a significant barrier tocommercialization. Here, simple liquid phase atomic layer deposition is usedto deposit an alumina layer to protect nickel particles from sintering. In thegas phase, it is proved that alumina can prevent sintering during reductionup to 600℃. This catalyst for hydrogenolysis of extracted lignin in batch andcontinuous operation is used. In batch, the overcoated catalyst maintainshigh monomer yields with little sintering over four cycles of reuse whilethe yield obtained with the catalyst without an overcoat reduces to half andsevere sintering occurs. In a continuous flow reactor, deactivation rates arethree times lower for the catalyst with the alumina overcoat. Microscopyimages confirm that the alumina overcoat largely preserves nickel particlesizes after ten days of operation. The results demonstrate that catalyst overcoatingwith metal oxides substantially slows irreversible deactivation duringlignin hydrogenolysis, which could facilitate the development of continuouslignin upgrading.
机译:木质素氢解是可持续生产可再生生物基化学品和燃料的关键步骤。非均相金属催化剂导致了高产率,但它们会迅速失活,特别是由于纳米颗粒烧结和碳质沉积物的形成。虽然这些沉积物可以通过再生去除,但烧结是不可逆的,并且是商业化的重大障碍。在这里,使用简单的液相原子层沉积来沉积氧化铝层,以保护镍颗粒免受烧结。在气相中,证明氧化铝在还原至600°C时可以防止烧结。该催化剂用于分批和连续操作提取木质素的氢解。在批次中,包覆的催化剂在四个循环的重复使用中保持高单体收率,几乎没有烧结,而使用没有包覆的催化剂获得的产率降低到一半,并发生严重的烧结。在连续流反应器中,氧化铝涂层催化剂的失活率要低三倍。显微镜图像证实,氧化铝涂层在操作十天后在很大程度上保留了镍粒径。结果表明,催化剂与金属氧化物的覆涂可显著减缓木质素氢解过程中的不可逆失活,从而促进木质素的持续升级。

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