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Pd/ZrO2-Al2O3催化剂中载体制备对CH4转化活性的影响
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1.昆明理工大学 环境科学与工程学院;2.昆明贵研新材料科技有限公司 稀贵金属综合利用新技术国家重点实验室

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国家自然科学基金(NO.21862010)、云南省应用基础研究计划(NO.2017FB143)、移动源污染排放控制技术国家工程实验室开放基金(NO.NELMS2017C02)、国家重点研发计划(NO.2016YFC0204902) 、昆明理工大学分析测试基金(2019P20181107010)资助


Effect of Support Preparation on CH4 Conversion Activity over Pd/ZrO2-Al2O3 Catalysts
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    摘要:

    为推动ZrO2-Al2O3在天然气汽车尾气净化催化剂中的实际应用,并阐明其制备条件对负载催化剂转化活性的影响机制,文章以ZrO2-Al2O3复合氧化物为载体,采用等体积浸渍法制备了Pd/ZrO2-Al2O3催化剂,并在连续流动固定床反应器上研究了ZrO2-Al2O3复合氧化物的制备对催化剂低温CH4氧化活性的影响。结果表明:制备方法中,相比于浸渍法和胶溶法,沉淀法更能提高催化剂活性;锆源、铝源优选中,以Zr(NO3)4为锆源、拟薄水铝石为铝源时能获得较高的催化活性;组分配比中,以w (ZrO2): w (Al2O3)=10:90的催化活性最高。XRD、低温N2吸附、CO脉冲吸附的结构表征表明,ZrO2-Al2O3复合氧化物的大的比表面积、孔容、孔径是促进贵金属Pd分散,提升催化剂低温CH4转化活性的关键因素。

    Abstract:

    Through the preparation of Pd/ZrO2-Al2O3 catalysts supported by ZrO2-Al2O3 composite oxides, the influence of the preparation of ZrO2-Al2O3 composite oxides on the low temperature CH4 oxidation activity of the catalysts were studied in a continuous flow fixed bed reactor, in order to promote the practical application of ZrO2-Al2O3 in the catalyst for natural gas vehicle exhaust purification, and to clarify the mechanism of the influence of preparation conditions on the conversion activity of the supported catalyst. The results show that the precipitation method can improve the activity of catalyst more than the impregnation method and the peptizing method; When Zr(NO3)4 is used as zirconium precursor and boehmite as aluminum precursor, high catalytic activity can be obtained; The activity of w (ZrO2): w (Al2O3)=10:90 is the highest in series of catalysts with different proportions. The structure characterization of XRD, N2 adsorption-desorption and CO pulse adsorption show that the large specific surface area, pore volume and pore diameter of ZrO2-Al2O3 composite oxides are the key factors to promote the dispersion of noble metal Pd and the conversion activity of catalyst CH4 at low temperature.

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杜君臣,杨海琼,张爱敏,郭淼鑫,郑婷婷,赵云昆,罗永明,黄卫强. Pd/ZrO2-Al2O3催化剂中载体制备对CH4转化活性的影响[J].稀有金属材料与工程,2020,49(10):3505~3509.[du jun chen, Yang Haiqiong, Zhang Aimin, Guo Miaoxin, Zheng Tingting, Zhao Yunkun, Luo Yongming, Huang Weiqiang. Effect of Support Preparation on CH4 Conversion Activity over Pd/ZrO2-Al2O3 Catalysts[J]. Rare Metal Materials and Engineering,2020,49(10):3505~3509.]
DOI:10.12442/j. issn.1002-185X.20190856

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  • 收稿日期:2019-10-16
  • 最后修改日期:2019-11-25
  • 录用日期:2019-11-29
  • 在线发布日期: 2020-11-04
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