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Electrochemistry for the generation of renewable chemicals electrochemical conversion of levulinic acid

机译:用于产生可再生化学品的电化学电化学转化乙酰酸

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The oxidative and reductive electrochemical conversion of levulinic acid to its primary products valeric acid, γ-valerolactone, 2,7-octanedione, 4-hydroxy-2-butanone and 3-buten-2-one is studied in detail. The reactions were performed in aqueous solutions and at ambient temperature, following the principles of green chemistry. The obtained primary reaction products were studied with respect to the oxidative and reductive electrochemical formation of secondary products, such as n -octane, 1-butanol and 1,3-butanediol. It is shown that the choice of electrolyte composition, educt concentration and the nature of the electrode material has a strong influence on the selectivity of product formation. For instance it is demonstrated that in alkaline solutions γ-valerolactone can be gained from levulinic acid at iron electrodes with similar Coulombic efficiency (~20%) but higher selectivity ( S = 70%) than on lead ( S = 50%). Furthermore, for the first time the electrochemical two-step reaction of levulinic acid to 1-butanol via 4-hydroxy-2-butanone is reported. For some of the reaction pathways the main product is water insoluble, which allows a direct separation of the product and the potential electrolyte reuse in a semi-continuous process. Especially the use of the electrocatalytic hydrogenation may provide a path for the storage of electricity into liquid organic fuels as shown by a basic energetic assessment of all electrochemical conversions.
机译:详细地研究了乙酰丙酸对其初级产物戊酸,γ-戊酮,2,7-辛烷酮,4-羟基-2-丁酮和3-丁烯-2-酮的氧化和还原电化学转化。通过绿色化学原理,在水溶液中和环境温度下进行反应。研究了所得初级反应产物,相对于仲产物的氧化和还原电化学形成,例如N-氧辛烷,1-丁醇和1,3-丁二醇。结果表明,电解质组合物的选择,内脏浓度和电极材料的性质对产品形成的选择性有很大影响。例如,证明,在碱性溶液中,γ-戊酮可以从具有相似的库仑效率(〜20%)的铁电极处的紫水酸中获得,但选择性更高(S = 70%),而不是在铅(S = 50%)。此外,首次据报道乙酰丙酸对1-丁醇的电化学两步反应通过4-羟基-2-丁酮。对于一些反应途径,主要产物是水不溶性,其允许在半连续过程中直接分离产品和电解电解质再利用。特别是使用电催化氢化可以提供用于将电力储存到液体有机燃料中的路径,如所有电化学转换的基本能量评估所示。

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