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穿流式电催化膜MnO2@Ti的制备及催化氧化正丙醇性能
Preparation of Flow-Through MnO2@Ti Electrocatalytic Membrane and Its Catalytic Performance for Oxidation of n-Propanol
【摘要】 为了增强催化剂和反应物之间的接触和传质,采用流动合成法在多孔钛膜孔道中原位固载了MnO2纳米颗粒,构筑了MnO2@Ti电催化膜,并用于电催化正丙醇氧化制备丙酸。形貌结构表征表明在1μm膜孔中成功地固定了平均尺寸为83 nm的MnO2纳米颗粒。电化学表征表明,与钛膜相比,MnO2@Ti电催化膜的电流密度增加了3.58 mA/cm2,电荷转移电阻降低了26.1Ω,说明可以实现更快的电子转移。MnO2@Ti电催化膜在膜通量为89.3 L/(m2·h)的穿流模式下,催化初始浓度为160 mmol/L的正丙醇氧化的转化率可达95%,丙酸选择性为89%,丙酸电流效率为90%。正丙醇氧化生成丙酸反应的机理分析表明,穿流模式下强化接触和传质能使MnO2@Ti电催化膜氧化过程中更多的·OH被利用,从而提高正丙醇的氧化性能。
【Abstract】 To enhance the contact and mass transfer between catalyst and reactants, MnO2@Ti electrocatalytic membrane was fabricated by flowing synthesis with MnO2 nanoparticles in situ immobilized in the pores of porous Ti membrane, and used for the production of propionic acid by electrocatalytic oxidation of n-propanol. The morphological and structural characterization showed that MnO2 nanoparticles with an average size of 83 nm were successfully immobilized in 1 μm membrane pores. The electrochemical characterization showed that the current density of the electrocatalytic membrane increased by 3.58 mA/cm2and the charge transfer resistance decreased by 26.1 Ω compared to Ti membrane via flow-through mode,which indicated that faster electron transfer could be achieved. During the process of n-propanol oxidation by MnO2@Ti electrocatalytic membrane via flow-through mode with a membrane flux of 89.3 L/(m2·h), the conversion of n-propanol with initial concentration of 160 mmol/L could reach 95%, the selectivity of propionic acid was 89% and the current efficiency of propionic acid was 90%. The mechanism analysis of n-propanol oxidation to propionic acid showed that the enhanced contact and mass transfer via flow-through mode would allow more ·OH to be utilized in the oxidation process of MnO2@Ti electrocatalytic membrane,thus enhancing the oxidation performance of n-propanol.
【Key words】 electrocatalytic membrane; flowing synthesis; n-propanol oxidation; flow-through;
- 【文献出处】 化学反应工程与工艺 ,Chemical Reaction Engineering and Technology , 编辑部邮箱 ,2023年05期
- 【分类号】TQ225.123;TQ426
- 【下载频次】16