穿流式电催化膜MnO_(2)@Ti的制备及催化氧化正丙醇性能  

Preparation of Flow-Through MnO_(2)@Ti Electrocatalytic Membrane and Its Catalytic Performance for Oxidation of n-Propanol

作　　者：杨明霞 樊森清 陈皎皎 陈渝 李创 肖泽仪[1] YANG Mingxia;FAN Senqing;CHEN Jiaojiao;CHEN Yu;LI Chuang;XIAO Zeyi(School of Chemical Engineering,Sichuan University,Chengdu 610065,China)

机构地区：[1]四川大学化学工程学院,四川成都610065

出　　处：《化学反应工程与工艺》2023年第5期385-393,共9页Chemical Reaction Engineering and Technology

基　　金：中国石油科技创新基金研究项目(2021DQ02-0601);四川大学科技领军人才项目(00826004151335)。

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MnO_(2)纳米颗粒,构筑了MnO_(2)@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83nm的MnO_(2)纳米颗粒。电化学表征表明,与钛膜相比,MnO_(2)@Ti电催化膜的电流密度增加了3.58mA/cm^(2),电荷转移电阻降低了26.1Ω,说明可以实现更快的电子转移。MnO_(2)@Ti电催化膜在膜通量为89.3L/(m^(2)·h)的穿流模式下,催化初始浓度为160mmol/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MnO_(2)@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。To enhance the contact and mass transfer between catalyst and reactants,MnO_(2)@Ti electrocatalytic membrane was fabricated by flowing synthesis with MnO_(2)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 MnO_(2)nanoparticles with an average size of 83 nm were successfully immobilized in 1μm membrane pores.The electrochemical characterization showed that the current density of the electrocatalytic membrane increased by 3.58 mA/cm^(2)and the charge transfer resistance decreased by 26.1Ωcompared to Ti membrane via flow-through mode,which indicated that faster electron transfer could be achieved.During the process of n-propanol oxidation by MnO_(2)@Ti electrocatalytic membrane via flow-through mode with a membrane flux of 89.3 L/(m^(2)·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 MnO_(2)@Ti electrocatalytic membrane,thus enhancing the oxidation performance of n-propanol.

关 键 词：电催化膜 流动合成 正丙醇氧化 穿流模式 

分 类 号：TQ0.32.4[化学工程]