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Ce_xMn_(1-x)O_2复合氧化物的制备及催化湿式氧化降解高浓度有机酸的应用
引用本文:王艳敏,于超英,孟旭,赵培庆,丑凌军,陈革新.Ce_xMn_(1-x)O_2复合氧化物的制备及催化湿式氧化降解高浓度有机酸的应用[J].分子催化,2017,31(5):428-437.
作者姓名:王艳敏  于超英  孟旭  赵培庆  丑凌军  陈革新
作者单位:1. 中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室,甘肃兰州730000;中国科学院大学,北京100049;2. 中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室,甘肃兰州,730000
基金项目:国家自然科学基金项目(No.21403256,21573261)
摘    要:利用水热法制备CeO_2和一系列不同Ce/Mn原子比的Ce_xMn_(1-x)O_2复合氧化物的纳米球,对其进行XRD、XPS、SEM、H_2-TPR和N_2吸附-脱附的表征,并通过催化湿式氧化降解丁酸对催化活性进行测试,结果表明Ce_(0.2)Mn_(0.8)O_2对丁酸的降解呈现出优异的催化性能.该催化剂对高浓度的醋酸、丁酸以及两者混合酸的降解也具有高的催化活性,在185℃、0.9 MPa O_2条件下反应2 h,醋酸、丁酸以及两者混合酸COD(化学需氧量)的去除率分别高达89.8%、99.5%和99.4%.最后,对该催化剂催化湿式氧化降解丁酸、醋酸以及丁酸和醋酸的混合酸进行了动力学和稳定性方面的研究.

关 键 词:复合氧化物  催化湿式氧化  有机酸  纳米球
收稿时间:2017/7/3 0:00:00
修稿时间:2017/8/10 0:00:00

The Preparation of CexMn1-xO2 Mixed Oxides and the Applications for Catalytic Wet Air Oxidation of High Concentration Organic Acids
WANG Yan-min,YU Chao-ying,MENG Xu,ZHAO Pei-qing,CHOU Ling-jun and CHEN Ge-xin.The Preparation of CexMn1-xO2 Mixed Oxides and the Applications for Catalytic Wet Air Oxidation of High Concentration Organic Acids[J].Journal of Molecular Catalysis (China),2017,31(5):428-437.
Authors:WANG Yan-min  YU Chao-ying  MENG Xu  ZHAO Pei-qing  CHOU Ling-jun and CHEN Ge-xin
Institution:State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics(LICP), Chinese Academy of Sciences, Lanzhou 730000, China;University of Chinese Academy of Sciences, Beijing 100049, China,State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics(LICP), Chinese Academy of Sciences, Lanzhou 730000, China,State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics(LICP), Chinese Academy of Sciences, Lanzhou 730000, China,State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics(LICP), Chinese Academy of Sciences, Lanzhou 730000, China,State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics(LICP), Chinese Academy of Sciences, Lanzhou 730000, China and State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics(LICP), Chinese Academy of Sciences, Lanzhou 730000, China
Abstract:CeO2 nanospheres and CexMn1-xO2 nanospheres were prepared by PVP-assisted hydrothermal method and characterized by SEM,XPS,XRD,H2-TPR and N2 absorption-desorption.The catalytic wet air oxidation (CWAO) behavior of high concentration organic acids,including acetic acid,butyric acid and the mixture of ace tic acid and butyric acid,is tested over the Ce0.2Mn0.8O2 nanosphere,which turns out to be an efficient catalyst for the activation and degradation of high concentration organic acids.When the reaction operated at 0.9 MPa partial pressure of O2,185 ℃ for 2 h,the chemical oxygen demand (COD) removal can reach up to 89.8%,99.5% and 99.4% for acetic acid,butyric acid and the mixture of acetic acid and butyric acid,respectively.Noticeably,the kinetic studies of CWAO for three kinds of organic acids over the Ce0.2Mn0.sO2 reveal that the degradation of sole acid is easier than that of mixture acid.In addition,the Ce0.2 Mn0.8O2 oxides perform a good reusability during the cycle experiment even after six cycles.
Keywords:mixed oxides  catalytic wet air oxidation  organic acids  nanospheres
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