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Supported cobalt catalysts for the selective hydrogenation of ethyl levulinate to various chemicals

机译:用于将乙酰丙酸乙酯选择性加氢为各种化学品的负载钴催化剂

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A highly active and selective cobalt catalyst was developed for the hydrogenation of biomass-derived ethyl levulinate (EL) to γ-valerolactone (GVL), ethyl 4-hydroxypentanoate (EHP), 1,4-pentanediol (1,4-PDO) and 2-methyltetrahydrofuran (2-MTHF), which are considered to be value-added chemicals and important biofuels. The effects of reaction time, reaction temperature, catalyst amount and solvent on its catalytic performance were investigated. In addition, the reaction pathway was studied as well. It was found that the selectivity of GVL, 1,4-PDO and 2-MTHF on Co/ZrO _(2) can be easily tuned by changing reaction conditions, and can reach as high as 94%, 78% and 77%, respectively. The product selectivity is also significantly affected by the catalyst support. With SBA-15 as the support, the selectivity of EHP can reach 90%. Moreover, Co/ZrO _(2) gave an extraordinarily high GVL productivity of 1.50 mol g _(metal) ~(?1) h ~(?1) and displayed excellent stability and reusability. Interestingly, coke has a positive effect on the enhancement of GVL yield. AL dimers and trimers were identified as the coke species in the hydrogenation of EL. As far as we know, this is the first work conducting the flexible transformation of EL on cobalt catalysts.
机译:开发了一种高活性和选择性的钴催化剂,用于将生物质衍生的乙酰丙酸乙酯(EL)加氢成γ-戊内酯(GVL),4-羟基戊酸乙酯(EHP),1,4-戊二醇(1,4-PDO)和2-甲基四氢呋喃(2-MTHF)被认为是增值化学品和重要的生物燃料。研究了反应时间,反应温度,催化剂用量和溶剂对其催化性能的影响。另外,还研究了反应途径。发现通过改变反应条件可以很容易地调节GVL,1,4-PDO和2-MTHF对Co / ZrO _(2)的选择性,最高可达94%,78%和77%,分别。催化剂载体还显着影响产物的选择性。以SBA-15为载体,EHP的选择性可达到90%。此外,Co / ZrO _(2)具有1.50 mol g _(金属)〜(?1)h〜(?1)的极高的GVL生产率,并显示出极好的稳定性和可重复使用性。有趣的是,焦炭对提高GVL产量有积极作用。 AL二聚体和三聚体被确定为EL加氢过程中的焦炭。据我们所知,这是在钴催化剂上进行EL柔性转化的第一项工作。

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