制备方法对Ni/CeO2-Al2O3催化剂甲烷部分氧化催化性能的影响

余长林; 胡久彪; 杨凯; 周晓春

制备方法对Ni/CeO₂-Al₂O₃催化剂甲烷部分氧化催化性能的影响

1.
江西理工大学冶金与化学工程学院, 江西赣州 341000;
2.
福州大学福建省光催化重点实验室-省部共建国家重点实验室培育基地, 福建福州 350002

基金项目: 国家自然科学基金(21067004,21263005);江西省教育厅科技基金(GJJ12344);江西省青年科学家培养项目(20122BCB23015);国家留学基金(2011836054)。

详细信息

通讯作者:
余长林 (1974-), 湖南炎陵人, 男, 博士, 副教授, 主要从事纳米催化新材料研究。Tel: 0797-8312334; E-mail: yuchanglinjx@163.com。

中图分类号: O643
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出版历程
- 收稿日期: 2012-11-21
- 修回日期: 2013-02-04
- 刊出日期: 2013-06-30

Effects of preparation methods on the catalytic performance of Ni/CeO₂-Al₂O₃ catalyst in methane partial oxidation

1.
School of Metallurgy and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, China;
2.
Fujian Provincial Key Laboratory of Photocatalysis-State Key Laboratory Breeding Base, Fuzhou University, Fuzhou 350002, China

摘要

摘要: 采用浸渍-沉淀法、水热合成法、共沉淀法和柠檬酸络合法制备了Ni/CeO₂-Al₂O₃催化剂,考察了制备方法对该催化剂的物理结构和甲烷部分氧化(POM)催化性能的影响。利用N₂物理吸附、X射线粉末衍射(XRD)、H₂-程序升温还原(H₂-TPR)、NH₃-程序升温脱附(NH₃-TPD)、热重(TG)分析等手段对反应前后催化剂的物理化学性质进行了表征。实验结果表明,浸渍-沉淀法制备催化剂的活性和产物H₂和CO的选择性最低。而柠檬酸络合法制备的Ni/CeO₂-Al₂O₃表现出最大的CH₄转化率和最高的CO、H₂选择性。BET和XRD表征结果表明,柠檬酸络合法制备的Ni/CeO₂-Al₂O₃的比表面积最大,且CeO₂晶粒粒径小、分散均匀;H₂-TPR测试表明,该催化剂负载的Ni物种和Ni与Al₂O₃相互作用产生的尖晶石NiAl₂O₄都较容易被还原成金属Ni,产生更多的活性中心;NH₃-TPD和TG分析表明,该催化剂具有较多酸性位点和表面积炭,但相比较于它的高反应活性,积炭速率较低、稳定性较高。
- 甲烷 /
- 部分氧化 /
- 镍 /
- 制备方法 /
- 尖晶石
Abstract: A series of Ni/CeO₂-Al₂O₃ catalysts were prepared by the methods of impregnation-precipitation, hydrothermal synthesis, co-precipitation and citric acid complexation. The effects of preparation method on the physical structures and catalytic performance of the resultant catalysts in partial oxidation of methane (POM) were investigated. The fresh and spent catalysts were characterized by N₂ physical adsorption, X-ray diffraction (XRD), temperature-programmed reduction by hydrogen (H₂-TPR), temperature programmed desorption of ammonia (NH₃-TPD) and thermogravimetry (TG) analysis. The results show that Ni/CeO₂-Al₂O₃ prepared by impregnation-precipitation method exhibits the lowest activity and selectivity to H₂ and CO; the highest catalytic performance is achieved by the catalyst prepared through citric acid complexation. The Ni/CeO₂-Al₂O₃ catalyst prepared by citric acid complexation has the largest specific surface area and the smallest CeO₂ crystals with good dispersion. Both Ni species and NiAl₂O₄ spinel in Ni/CeO₂-Al₂O₃ prepared by citric acid complexation are prone to being reduced to metal Ni, which can produce more active sites for methane partial oxidation reaction. There is more acidic sites and deposited carbon over the catalyst prepared by citric acid complexation; however, taking its high activity into account, its stability is relatively high with low carbon deposition rate.
- methane /
- partial oxidation /
- nickel /
- preparation method /
- spinel

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制备方法对Ni/CeO₂-Al₂O₃催化剂甲烷部分氧化催化性能的影响

通讯作者:
余长林 (1974-), 湖南炎陵人, 男, 博士, 副教授, 主要从事纳米催化新材料研究。Tel: 0797-8312334; E-mail: yuchanglinjx@163.com。

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Effects of preparation methods on the catalytic performance of Ni/CeO₂-Al₂O₃ catalyst in methane partial oxidation

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