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纳米催化剂Pd/SnO_2的制备及催化还原硝酸盐反应的调控
引用本文:吴以保,胡勇有,程建华,郭燕妮.纳米催化剂Pd/SnO_2的制备及催化还原硝酸盐反应的调控[J].环境科学学报,2010,30(12):2464-2470.
作者姓名:吴以保  胡勇有  程建华  郭燕妮
作者单位:华南理工大学环境科学与工程学院工业聚集区污染控制与生态修复教育部重点实验室,广州,510006
基金项目:国家科技重大专项 (No. 2008ZX07211-005)
摘    要:采用热分解法制备了SnO2载体,并用浸渍法制备了Pd/SnO2催化剂.同时,采用X射线衍射仪(XRD)、透射电镜(TEM)、扫描电镜(SEM)及BET比表面积仪等对所制载体和催化剂材料进行了分析表征.结果表明,热分解法和浸渍法都能够获得纳米材料,SnO2及Pd/SnO2的粒径均在9~10nm左右,比表面积分别达到144.99m·2g-1和147.36m·2g-1.在以甲酸为还原剂的Pd/SnO2催化还原硝酸盐体系中,在Pd与SnO2负载比为2%~7%,反应温度为20~50℃和甲酸投加量4.0~24.0mmol·L-1的条件下,催化活性为0.70~9.48mg·min-·1g-1,且催化活性随着负载比、温度和甲酸投加量的增大而增大,随着pH的升高先升后降,最佳pH为3.反应温度升高及pH降低都能够提高Pd/SnO2的选择性.甲酸-Pd/SnO2催化还原硝酸盐体系中还原反应的调控策略为:反应温度宜控制在40~50℃内,这样可同时获得较高的催化活性和选择性,温度过高对催化活性和选择性影响很小,温度过低则会同时降低催化活性和选择性;控制pH为3时,可以获得最大的催化活性及较好的选择性,pH升高会降低Pd/SnO2的催化活性和选择性,pH降低会导致催化活性迅速降低,但对选择性影响不大;甲酸与硝酸盐的物质的量比宜大于4:1,此时可以有效地抑制pH的上升,同时获得较高的催化活性和选择性,甲酸与硝酸盐的物质的量比小于4:1时,会同时降低Pd/SnO2的催化活性和选择性.

关 键 词:SnO2  Pd/  SnO2  纳米  甲酸  硝酸盐  催化还原
收稿时间:4/16/2010 2:47:21 PM
修稿时间:6/6/2010 1:41:07 PM

Preparation of nano-Pd/SnO2 catalyst and control of catalytic reduction reaction of nitrate
WU Yibao,HU Yongyou,CHENG Jianhua and GUO Yanni.Preparation of nano-Pd/SnO2 catalyst and control of catalytic reduction reaction of nitrate[J].Acta Scientiae Circumstantiae,2010,30(12):2464-2470.
Authors:WU Yibao  HU Yongyou  CHENG Jianhua and GUO Yanni
Institution:College of Environmental Science and Engineering, South China University of Technology, the Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, Guangzhou 510006,College of Environmental Science and Engineering, South China University of Technology, the Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, Guangzhou 510006,College of Environmental Science and Engineering, South China University of Technology, the Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, Guangzhou 510006 and College of Environmental Science and Engineering, South China University of Technology, the Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, Guangzhou 510006
Abstract:
Keywords:SnO2  Pd/SnO2  nanoparticle  formic acid  nitrate  catalytic reduction
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