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Pd/ZrO2-Al2O3催化劑中載體制備對(duì)CH4轉(zhuǎn)化活性的影響
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1.昆明理工大學(xué) 環(huán)境科學(xué)與工程學(xué)院;2.昆明貴研新材料科技有限公司 稀貴金屬綜合利用新技術(shù)國(guó)家重點(diǎn)實(shí)驗(yàn)室

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國(guó)家自然科學(xué)基金(NO.21862010)、云南省應(yīng)用基礎(chǔ)研究計(jì)劃(NO.2017FB143)、移動(dòng)源污染排放控制技術(shù)國(guó)家工程實(shí)驗(yàn)室開放基金(NO.NELMS2017C02)、國(guó)家重點(diǎn)研發(fā)計(jì)劃(NO.2016YFC0204902) 、昆明理工大學(xué)分析測(cè)試基金(2019P20181107010)資助


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

    為推動(dòng)ZrO2-Al2O3在天然氣汽車尾氣凈化催化劑中的實(shí)際應(yīng)用,并闡明其制備條件對(duì)負(fù)載催化劑轉(zhuǎn)化活性的影響機(jī)制,文章以ZrO2-Al2O3復(fù)合氧化物為載體,采用等體積浸漬法制備了Pd/ZrO2-Al2O3催化劑,并在連續(xù)流動(dòng)固定床反應(yīng)器上研究了ZrO2-Al2O3復(fù)合氧化物的制備對(duì)催化劑低溫CH4氧化活性的影響。結(jié)果表明:制備方法中,相比于浸漬法和膠溶法,沉淀法更能提高催化劑活性;鋯源、鋁源優(yōu)選中,以Zr(NO3)4為鋯源、擬薄水鋁石為鋁源時(shí)能獲得較高的催化活性;組分配比中,以w (ZrO2): w (Al2O3)=10:90的催化活性最高。XRD、低溫N2吸附、CO脈沖吸附的結(jié)構(gòu)表征表明,ZrO2-Al2O3復(fù)合氧化物的大的比表面積、孔容、孔徑是促進(jìn)貴金屬Pd分散,提升催化劑低溫CH4轉(zhuǎn)化活性的關(guān)鍵因素。

    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,楊海瓊,張愛敏,郭淼鑫,鄭婷婷,趙云昆,羅永明,黃衛(wèi)強(qiáng). Pd/ZrO2-Al2O3催化劑中載體制備對(duì)CH4轉(zhuǎn)化活性的影響[J].稀有金屬材料與工程,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
  • 錄用日期:2019-11-29
  • 在線發(fā)布日期: 2020-11-04
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