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浙江大学学报(工学版)
能源工程     
Cr/TiO2催化剂汞氧化的实验
俞晋频,邱坤赞,宋浩,高翔,周劲松
浙江大学 能源清洁利用国家重点实验室,浙江 杭州 310027
Catalytic oxidation experiment of element mercury over Cr/TiO2 catalyst
YU Jin pin, QIU Kun zan, SONG Hao, GAO Xiang, ZHOU Jin song
State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, China
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摘要:

通过等体积浸渍法制备不同质量分数w(0.1%~5%)的Cr/TiO2催化剂.活性测试结果表明,Cr/TiO2催化剂在高空速、低氯条件下有很高的汞氧化活性.研究Cr负载量、反应温度、不同烟气组分对汞氧化的影响,结果表明:Cr/TiO2催化剂汞氧化活性随Cr负载量和反应温度的升高而提高.O2和HCl对Cr/TiO2催化剂上汞氧化有极强的促进作用.当只有O2存在时,Cr/TiO2催化剂上汞氧化按照Mars Maessen机理进行,Hg0首先吸附到催化剂表面,然后与晶格氧反应生成弱吸附的HgO,消耗的晶格氧由气态O2补充.当O2和HCl同时存在时,由于在催化剂表面生成活性氯物种,反应机理发生改变,汞氧化得到促进.NO也可以促进汞氧化.SO2与Hg0在催化剂表面竞争吸附从而抑制汞氧化,H2O对汞氧化也有抑制作用.

Abstract:

A series of Cr/TiO2 catalysts with different Cr loading w(0.1%~5%) were prepared using impregnation method. Cr/TiO2 catalysts exhibit excellent mercury oxidation ability in low HCl concentration even at high gas hourly space velocity. The influences of Cr loading, reaction temperature and flue gas component on mercury oxidation were studied as well. The results indicate that mercury oxidation increase together with the increase of Cr content and reaction temperature. O2 and HCl have  significant promoting effect on mercury oxidation over Cr/TiO2 catalyst. The reaction over Cr/TiO2 catalyst follows Mars Maessen mechanism when only O2 exists. Hg0  initially adsorbs on the catalyst surface, then reacts with lattice oxygen to form weakly adsorbed HgO. The consumed lattice oxygen is recovered by gas phase oxygen. When both O2 and HCl  exist, mercury oxidation is promoted due to active chlorine species generated on the catalyst surface and the mechanism alters. NO is also found to promote mercury oxidation. SO2 however inhibits the reaction due to its competitive adsorption with Hg0 on catelytic surface. H2O is also found to have a negative effect on mercury oxidation.

出版日期: 2015-11-01
:  X 701  
基金资助:

国家“863”高技术研究发展计划资助项目(2013AA065401).

通讯作者: 高翔,男,教授,博导. ORCID:0000 0002 1732 2132.     E-mail: gaox@zju.edu.cn
作者简介: 俞晋频(1990-),男,硕士生,从事燃煤电厂污染物控制研究. ORCID:0000 0002 9572 0187.E-mail: yujinpin3055@zju.edu.cn
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引用本文:

俞晋频,邱坤赞,宋浩,高翔,周劲松. Cr/TiO2催化剂汞氧化的实验[J]. 浙江大学学报(工学版), 10.3785/j.issn.1008 973X.2015.11.021.

YU Jin pin, QIU Kun zan, SONG Hao, GAO Xiang, ZHOU Jin song. Catalytic oxidation experiment of element mercury over Cr/TiO2 catalyst. JOURNAL OF ZHEJIANG UNIVERSITY (ENGINEERING SCIENCE), 10.3785/j.issn.1008 973X.2015.11.021.

链接本文:

http://www.zjujournals.com/eng/CN/10.3785/j.issn.1008 973X.2015.11.021        http://www.zjujournals.com/eng/CN/Y2015/V49/I11/2186

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