Continuous homogeneous asymmetric transfer hydrogenation of ketones: lessons from kinetics.
Continuous homogeneous asymmetric transfer hydrogenation of ketones: lessons from kinetics.
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酮的连续均相不对称转移氢化：动力学的教训。
DOI：
10.1002/chem.200500675
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发表时间：
2006
期刊：
影响因子：
--
通讯作者：
C. Wandrey
中科院分区：
文献类型：
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作者：
L. Greiner;Stephan Laue;A. Liese;C. Wandrey
均相催化剂的聚合物放大是一项繁琐的任务吗？使用均相催化剂的间歇操作不是均相催化的最佳性能点吗？在均相催化中，动力学建模是否不仅仅与学术问题相关？一个给定系统的所有答案都能令人满意吗？在作者看来，这些问题的答案是否定、否定、肯定和视情况而定。聚合物放大允许在化学膜反应器中连续操作转移氢化，总周转数高达2.6 x 10(3)，时空产率为0.58 kg L(-1) d(-1)，对映体比为26.8（对映体过量92.8%），转化率为80%。这是通过采用连续应用的动力学批试验模型进行的模拟预测得到的。这些对聚合物放大催化剂和未改性催化剂的模拟表明，通过批量操作无法获得相当的性能。
Is polymer enlargement of homogeneous catalysts a tedious task? Is not batch operation with homogeneous catalysts the optimum performance point for homogeneous catalysis? Is kinetic modelling relevant to more than academic questions in homogeneous catalysis? Can all answers for a given system be answered satisfactory? In the authors' view, answers to these questions are no, no, yes, and depends. Polymer enlargement allowed the continuous operation of transfer hydrogenation in a chemical membrane reactor with total turnover numbers of up to 2.6 x 10(3) and a space-time yield of 0.58 kg L(-1) d(-1) with an enantiomeric ratio of 26.8 (enantiomeric excess 92.8 %) for a conversion level of 80 %. This was predicted from simulation conducted with a model from kinetic batch experiments adopted for continuous application. These simulations for the polymer-enlarged and the unmodified catalyst show that achieving comparable performance cannot be obtained by batch operation.