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Epoxidation of Propene by High-Throughput Screening Method Over Combinatorially Prepared Cu Catalysts Supported on High and Low Surface Area Silica

机译:高通量筛选法在高表面积和低表面积二氧化硅负载的组合制备的铜催化剂上丙烯环氧化

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摘要

Gas phase epoxidation of propene using molecular oxygen was studied by use of a high-throughput testing technique. A large number of catalysts including promoted and un-promoted Cu were synthesized in a much faster combinatorial fashion using a sol-gel method. Metal catalysts supported on high and low surface area silica were tested and ranked in a high-throughput activity and selectivity testing apparatus at different experimental conditions such as reaction temperature and reactant gas ratio. The amount of Cu loading and the addition of alkali promoters such as K and Li resulted in different tendencies in consumption rate for both silica materials. The maximum PO production rate was obtained as 25.82 μmol/g/ cat/min (2.90 % conv. and 20.49 % selectivity) for 3 % Cu-2.25 % K catalyst supported on high surface area silica. There was no noticeable difference in structural and chemical properties of catalysts after modification with K when examined by XRD and TEM; however, the overall activation energy of un-modified catalysts (92 kJ/mol) decreased to 71 kJ/mol for K-modined catalyst. There was negligible difference between the activation energies calculated for PO production (75 vs. 77 kJ/mol).
机译:通过使用高通量测试技术研究了使用分子氧的丙烯气相环氧化。使用溶胶-凝胶法以更快的组合方式合成了包括促进和未促进的Cu在内的大量催化剂。测试了负载在高和低表面积二氧化硅上的金属催化剂,并在不同的实验条件下(例如反应温度和反应气体比)在高通量活性和选择性测试设备中进行了排名。两种硅材料的铜负载量和碱助剂(如K和Li)的添加导致了不同的消耗速率趋势。对于负载在高表面积二氧化硅上的3%Cu-2.25%K催化剂,最大PO生产率为25.82μmol/ g / cat / min(2.90%转化率和20.49%选择性)。用XRD和TEM观察,用K改性后,催化剂的结构和化学性质无明显差异。然而,未改性催化剂的总活化能(92 kJ / mol)降低至K改性催化剂的71 kJ / mol。计算出的PO生成的活化能之间的差异可以忽略不计(75对77 kJ / mol)。

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