木质素模型化合物电化学还原裂解的产物选择性
On the product selectivity in the electrochemical reductive cleavage of lignin model compounds
摘要：
对用于燃料和能源工业的可再生化学品生产的研究发现，木质素的稳定是关键。由于木质素具有高的碳含量和芳香性，因此需要对解聚过程进行微调以将木质素转化为有价值的化学品。在上下文中，模型化合物已被用来理解模拟木质素的典型键的电催化解聚。本研究以木质素\b{eta} -O-4键的模型化合物2-苯氧基苯乙酮为研究对象，在开放式和膜式两种不同的三电极装置中进行了电催化氢化（ECH）。基于乙二醇和氯化胆碱的低共熔溶剂用于寻求溶解木质素的可持续途径。铜作为电催化剂，由于经济可行性和低活性的析氢反应（HER），一个副反应的ECH。通过改变细胞类型，我们展示了一个简单的ECH路线，从木质素产生不同的单体和低聚物。气相色谱分析的产品显示，在那些使用膜细胞的羰基含量较高，而开放的细胞产生的主要是羟基末端的化学品。针对高附加值产品，揭示了电解槽类型对木质素电化学还原解聚的影响。这种方法包括廉价的过渡金属电极和可持续的溶剂。
英文摘要：
Research towards the production of renewable chemicals for fuel and energy industries has found lignin valorization as key. With a high carbon content and aromaticity, a fine-tuning of the depolymerization process is required to convert lignin into valuable chemicals. In context, model compounds have been used to understand the electrocatalyzed depolymerization for mimicking the typical linkages of lignin. In this investigation, 2-phenoxyacetophenone, a model compound for lignin \b{eta}-O-4 linkage, was electro-catalytically hydrogenated (ECH) in distinct three-electrode setups: an open and a membrane cell. A deep eutectic solvent based on ethylene-glycol and choline chloride was used to pursue sustainable routes to dissolve lignin. Copper was used as electrocatalyst due to the economic feasibility and low activity towards hydrogen evolution reaction (HER), a side reaction of ECH. By varying the cell type, we demonstrate a simple ECH route for the generation of different monomers and oligomers from lignin. Gas chromatography of the products revealed a higher content of carbonyl groups in those using the membrane cell, whereas the open cell produced mostly hydroxyl-end chemicals. Aiming at high value-added products, our results disclose the cell type influence on electrochemical reductive depolymerization of lignin. This approach encompasses cheap transition metal electrodes and sustainable solvents.
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