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Abstract

Lignin hydrogenolysis is a key step in the sustainable production of renewable bio-based chemicals and fuels. Heterogeneous metal catalysts have led to high yields but they rapidly deactivate, notably due to nanoparticle sintering and carbonaceous deposit formation. While these deposits can be removed by regeneration, sintering is irreversible and a significant barrier to commercialization. Here, simple liquid phase atomic layer deposition is used to deposit an alumina layer to protect nickel particles from sintering. In the gas phase, it is proved that alumina can prevent sintering during reduction up to 600 degrees C. This catalyst for hydrogenolysis of extracted lignin in batch and continuous operation is used. In batch, the overcoated catalyst maintains high monomer yields with little sintering over four cycles of reuse while the yield obtained with the catalyst without an overcoat reduces to half and severe sintering occurs. In a continuous flow reactor, deactivation rates are three times lower for the catalyst with the alumina overcoat. Microscopy images confirm that the alumina overcoat largely preserves nickel particle sizes after ten days of operation. The results demonstrate that catalyst overcoating with metal oxides substantially slows irreversible deactivation during lignin hydrogenolysis, which could facilitate the development of continuous lignin upgrading.

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