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化学工业与工程 2014, Vol. 31 Issue (6) :13-17    DOI: doi: 10.13353/j.issn.1004.9533.2014.06.003
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Mn-M-O/TiO2-Al2O3催化超临界水氧化氨氮废水
胡紫芳1,2,姜浩锡1,2,李桂明1,2
1.天津大学石油化工技术开发中心,天津 300072; 2.天津大学绿色合成与转化教育部重点实验室,天津 300072
Oxidation of NH3 Wastewater in Supercritical Water over Mn-M-O/TiO2-Al2O3 Catalyst
 HU  Zi-Fang1,2, JIANG  Hao-Xi1,2, LI  Gui-Ming1,2
1R&D Center for Petrochemical Technology, Tianjin University, Tianjin 300072, China; 2Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University, Tianjin 300072, China

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摘要 以Mn和M(Ce、Cu、Co)的氧化物为活性组分、TiO2-Al2O3(TA)为载体,分别制备了3种不同Mn/M物质的量之比的双金属负载型Mn-M-O/TA催化剂。在连续超临界水氧化装置上及460 ℃、26 MPa、停留时间4~5 s和氧化剂剂量为化学剂量3倍的条件下,考察了各催化剂对氨的降解活性,结果表明Mn-Cu-O/TA催化剂具有较好的氨降解性能,Mn-Cu-O/TA-55催化剂氨转化率为55.8%。采用XRD、XPS、TPR等方法对Mn-M-O/TA催化剂进行了表征,添加铜后催化剂还原性能的提高,有利于氨转化率的提高。
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胡紫芳
姜浩锡
李桂明
关键词氧化锰;   二氧化钛;   超临界水氧化;   氨;   催化     
Abstract: Ammonia is one of the most refractory pollutants in coking wastewater. The degradation effect of traditional biochemical methods is not obvious. However, supercritical water oxidation technology as a novel and highly efficient method can completely remove ammonia in coking wastewater after the introduction of manganese based catalysts. In this work, supported manganesebased catalysts doped with additives Mn-M-O/TA of three different Mn/M molar ratio were prepared separately by incipient impregnation with oxides of Mn and M(Ce, Co, Cu) as active components and TiO2-Al2O3 (TA) as the support. The oxidation reaction of NH3 in supercritical water was carried out in a continuous flow reactor at 460 ℃, 26 MPa, and the residence time of 4—5 s with the oxidant dose of 3 times the stoichiometric amount. The results showed that the Mn-Cu-O/TA catalysts had a preferable performance of ammonia degradation, Mn-Cu-O/TA-55 exhibited the highest activity and the conversion of ammonia was 55.8%. The catalysts were characterized by XRD, XPS, TPR and other methods. The results showed that the reduction properties of the catalysts after adding Cu improved fast, which was good for the increase of conversion of ammonia.
Keywordsmanganese oxide;   titanium dioxide;   supercritical water oxidation;   ammonia;   catalysis     
Received 2013-04-17;
Fund:

天津大学自主创新基金资助项目(2012XZ-095)。

Corresponding Authors: 李桂明,电话:(022)27406119,E-mail:liguiming@tju.edu.cn。     Email: liguiming@tju.edu.cn
About author: 胡紫芳(1987-),女,硕士研究生,从事超临界流体技术与应用催化研究。
引用本文:   
胡紫芳, 姜浩锡, 李桂明.Mn-M-O/TiO2-Al2O3催化超临界水氧化氨氮废水[J].  化学工业与工程, 2014,31(6): 13-17
HU Zi-Fang, JIANG Hao-Xi, LI Gui-Ming.Oxidation of NH3 Wastewater in Supercritical Water over Mn-M-O/TiO2-Al2O3 Catalyst[J].  Chemcial Industry and Engineering, 2014,31(6): 13-17
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