N2O在Au/Co3O4和Au/ZnCo2O4催化剂上的分解反应

窦喆 冯鸣 徐秀峰

引用本文: 窦喆, 冯鸣, 徐秀峰. N2O在Au/Co3O4和Au/ZnCo2O4催化剂上的分解反应[J]. 燃料化学学报, 2013, 41(10): 1234-1240. shu
Citation:  DOU Zhe, FENG Ming, XU Xiu-feng. Catalytic decomposition of N2O over Au/Co3O4 and Au/ZnCo2O4 catalysts[J]. Journal of Fuel Chemistry and Technology, 2013, 41(10): 1234-1240. shu

N2O在Au/Co3O4和Au/ZnCo2O4催化剂上的分解反应

    通讯作者: XU Xiu-feng,E-mail:xxf@ytu.edu.cn。
摘要: 通过调变HAuCl4溶液的pH值和Au负载量,用沉积-沉淀法制备了一系列Au/Co3O4催化剂,并采用AES、BET、XRD、SEM、XPS和H2-TPR等技术对催化剂的结构和组成进行了表征,考察了制备条件对其在有氧气氛中催化N2O分解反应性能的影响规律,得到了催化剂最佳制备条件:HAuCl4溶液pH值为9,Au负载量为0.29%。催化测试结果表明:虽然ZnCo2O4的催化活性优于Co3O4,但0.31%Au/ZnCo2O4的活性和稳定性低于0.29%Au/Co3O4。500℃、在含氧气氛中连续反应10 h, 两者均可完全分解N2O,但在含氧、含水气氛中0.29%Au/Co3O4和0.31%Au/ZnCo2O4上的N2O转化率分别为92%和63%。究其原因,发现Au/Co3O4中Au和Co组分间存在协同效应,而Au/ZnCo2O4中Au和Co组分间则没有协同效应。

English

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    1. [1] WOOD B R, REIMER J A, BELL A T. Studies of N2O adsorption and decomposition on Fe-ZSM-5[J]. J Catal, 2002, 209(1): 151-158.[1] WOOD B R, REIMER J A, BELL A T. Studies of N2O adsorption and decomposition on Fe-ZSM-5[J]. J Catal, 2002, 209(1): 151-158.

    2. [2] WACLAW A, NOWINSKA K, SCHWIEGER W, ZIELINSKA A. N2O decomposition over iron modified zeolites ZSM-5[J]. Catal Today, 2004, 90(1/2): 21-25.[2] WACLAW A, NOWINSKA K, SCHWIEGER W, ZIELINSKA A. N2O decomposition over iron modified zeolites ZSM-5[J]. Catal Today, 2004, 90(1/2): 21-25.

    3. [3] PIRNGRUBER G D, LUECHINGER M, ROY P K, CECCHETTO A, SMIRNIOTIS P. N2O decomposition over iron-containing zeolites prepared by different methods: A comparison of the reaction mechanism[J]. J Catal, 2004, 224(2): 429-440.[3] PIRNGRUBER G D, LUECHINGER M, ROY P K, CECCHETTO A, SMIRNIOTIS P. N2O decomposition over iron-containing zeolites prepared by different methods: A comparison of the reaction mechanism[J]. J Catal, 2004, 224(2): 429-440.

    4. [4] PIETERSE J A Z, BOONEVELD S, VAN DEN BRINK R W. Evaluation of Fe-zeolite catalysts prepared by different methods for the decomposition of N2O[J]. Appl Catal B: Environ, 2004, 51(4): 215-228.[4] PIETERSE J A Z, BOONEVELD S, VAN DEN BRINK R W. Evaluation of Fe-zeolite catalysts prepared by different methods for the decomposition of N2O[J]. Appl Catal B: Environ, 2004, 51(4): 215-228.

    5. [5] JÍÑA K, NOVÁKOVÁ J, SCHWARZE M, VONDROVÁ A, SKLENÁK S, SOBALIK Z. Role of the Fe-zeolite structure and iron state in the N2O decomposition: Comparison of Fe-FER, Fe-BEA, and Fe-MFI catalysts[J]. J Catal, 2009, 262(1): 27-34.[5] JÍÑA K, NOVÁKOVÁ J, SCHWARZE M, VONDROVÁ A, SKLENÁK S, SOBALIK Z. Role of the Fe-zeolite structure and iron state in the N2O decomposition: Comparison of Fe-FER, Fe-BEA, and Fe-MFI catalysts[J]. J Catal, 2009, 262(1): 27-34.

    6. [6] OHNISHI C, ASANO K, IWAMOTO S, CHIKAMA K, INOUE M. Alkali-doped Co3O4 catalysts for direct decomposition of N2O in the presence of oxygen[J]. Catal Today, 2007, 120(2): 145-150.[6] OHNISHI C, ASANO K, IWAMOTO S, CHIKAMA K, INOUE M. Alkali-doped Co3O4 catalysts for direct decomposition of N2O in the presence of oxygen[J]. Catal Today, 2007, 120(2): 145-150.

    7. [7] ASANO K, OHNISHI C, IWAMOTO S, SHIOYA Y, INOUE M. Potassium-doped Co3O4 catalyst for direct decomposition of N2O[J]. Appl Catal B: Environ, 2008, 78(3/4): 242-249.[7] ASANO K, OHNISHI C, IWAMOTO S, SHIOYA Y, INOUE M. Potassium-doped Co3O4 catalyst for direct decomposition of N2O[J]. Appl Catal B: Environ, 2008, 78(3/4): 242-249.

    8. [8] STELMACHOWSKI P, MANIAK G, KOTARBA A, SOJKA Z. Strong electronic promotion of Co3O4 towards N2O decomposition by surface alkali dopants[J]. Catal Commun, 2009, 10(7): 1062-1065.[8] STELMACHOWSKI P, MANIAK G, KOTARBA A, SOJKA Z. Strong electronic promotion of Co3O4 towards N2O decomposition by surface alkali dopants[J]. Catal Commun, 2009, 10(7): 1062-1065.

    9. [9] PASHA N, LINGAIAH N, BABU N S, REDDY P S S, PRASAD P S S. Studies on cesium doped cobalt oxide catalysts for direct N2O decomposition in the presence of oxygen and steam[J]. Catal Commun, 2008, 10(2): 132-136.[9] PASHA N, LINGAIAH N, BABU N S, REDDY P S S, PRASAD P S S. Studies on cesium doped cobalt oxide catalysts for direct N2O decomposition in the presence of oxygen and steam[J]. Catal Commun, 2008, 10(2): 132-136.

    10. [10] SHEN Q, LI L D, LI J J, TIAN H, HAO Z P. A study on N2O catalytic decomposition over Co/MgO catalysts[J]. J Hazard Mater, 2009, 163(2/3): 1332- 1337.[10] SHEN Q, LI L D, LI J J, TIAN H, HAO Z P. A study on N2O catalytic decomposition over Co/MgO catalysts[J]. J Hazard Mater, 2009, 163(2/3): 1332- 1337.

    11. [11] 武海鹏, 李文静, 郭丽, 潘燕飞, 徐秀峰. 碱金属助剂类型及前驱物对改性NiAl复合氧化物催化分解N2O活性的影响[J]. 燃料化学学报, 2011, 39(7): 550-555.[11] 武海鹏, 李文静, 郭丽, 潘燕飞, 徐秀峰. 碱金属助剂类型及前驱物对改性NiAl复合氧化物催化分解N2O活性的影响[J]. 燃料化学学报, 2011, 39(7): 550-555.

    12. [12]

      (WU Hai-peng, LI Wen-jing, GUO Li, PAN Yan-fei, XU Xiu-feng. The effect of promoter species and precursors on catalytic activity of alkali metal promoted NiAl mixed oxides for N2O decomposition[J]. Journal of Fuel Chemistry and Technology, 2011, 39(7): 550-555.)(WU Hai-peng, LI Wen-jing, GUO Li, PAN Yan-fei, XU Xiu-feng. The effect of promoter species and precursors on catalytic activity of alkali metal promoted NiAl mixed oxides for N2O decomposition[J]. Journal of Fuel Chemistry and Technology, 2011, 39(7): 550-555.)

    13. [12] 武海鹏, 钱振英, 徐晓玲, 徐秀峰. K改性NiAl类水滑石衍生复合氧化物催化分解N2O[J]. 燃料化学学报, 2011, 39(2): 115-121.[12] 武海鹏, 钱振英, 徐晓玲, 徐秀峰. K改性NiAl类水滑石衍生复合氧化物催化分解N2O[J]. 燃料化学学报, 2011, 39(2): 115-121.

    14. [14]

      (WU Hai-peng, XU Zhen-ying, XU Xiao-ling, XU Xiu-feng. N2O decomposition over K-promoted NiAl mixed oxides derived from hydrotalcite-like compounds[J]. Journal of Fuel Chemistry and Technology, 2011, 39(2): 115-121.)(WU Hai-peng, XU Zhen-ying, XU Xiao-ling, XU Xiu-feng. N2O decomposition over K-promoted NiAl mixed oxides derived from hydrotalcite-like compounds[J]. Journal of Fuel Chemistry and Technology, 2011, 39(2): 115-121.)

    15. [13] CHENG H K, HUANG Y Q, WANG A Q, LI L, WANG X D, ZHANG T. N2O decomposition over K-promoted Co-Al catalysts prepared from hydrotalcite-like precursors[J]. Appl Catal B: Environ, 2009, 89(3/4): 391-397.[13] CHENG H K, HUANG Y Q, WANG A Q, LI L, WANG X D, ZHANG T. N2O decomposition over K-promoted Co-Al catalysts prepared from hydrotalcite-like precursors[J]. Appl Catal B: Environ, 2009, 89(3/4): 391-397.

    16. [14] ABU-ZIED B M. 碱促进的钴酸镁催化剂上的氧化亚氮分解[J]. 催化学报, 2011, 32(2): 264-272.[14] ABU-ZIED B M. 碱促进的钴酸镁催化剂上的氧化亚氮分解[J]. 催化学报, 2011, 32(2): 264-272.

    17. [17]

      (ABU-ZIED B M. Nitrous oxide decomposition over alkali-promoted magnesium cobaltite catalysts[J]. Chinese Journal of Catalysis, 2011, 32(2): 264-272.)(ABU-ZIED B M. Nitrous oxide decomposition over alkali-promoted magnesium cobaltite catalysts[J]. Chinese Journal of Catalysis, 2011, 32(2): 264-272.)

    18. [15] PARRES-ESCLAPEZ S, ILLÁN-GÓMEZ M J, SALINAS-MARTÍNEZ DE LECEA C, BUENO-LPEZ A. On the importance of the catalyst redox properties in the N2O decomposition over alumina and ceria supported Rh, Pd and Pt[J]. Appl Catal B: Environ, 2010, 96(3/4): 370-378.[15] PARRES-ESCLAPEZ S, ILLÁN-GÓMEZ M J, SALINAS-MARTÍNEZ DE LECEA C, BUENO-LPEZ A. On the importance of the catalyst redox properties in the N2O decomposition over alumina and ceria supported Rh, Pd and Pt[J]. Appl Catal B: Environ, 2010, 96(3/4): 370-378.

    19. [16] BOISSEL V, TAHIR S, KOH C A. Catalytic decomposition of N2O over monolithic supported noble metal-transition metal oxides[J]. Appl Catal B: Environ, 2006, 64(3/4): 234-242.[16] BOISSEL V, TAHIR S, KOH C A. Catalytic decomposition of N2O over monolithic supported noble metal-transition metal oxides[J]. Appl Catal B: Environ, 2006, 64(3/4): 234-242.

    20. [17] YAN L, ZHANG X M, REN T, ZHANG H P, WANG X L, SUO J S. Superior performance of nano-Au supported over Co3O4 catalyst in direct N2O decomposition[J]. Chem Commun, 2002, (8): 860-861.[17] YAN L, ZHANG X M, REN T, ZHANG H P, WANG X L, SUO J S. Superior performance of nano-Au supported over Co3O4 catalyst in direct N2O decomposition[J]. Chem Commun, 2002, (8): 860-861.

    21. [18] 徐晓玲, 徐秀峰, 张国涛, 牛宪军. 钴铝复合氧化物负载金催化剂的制备及催化分解N2O[J]. 燃料化学学报, 2009, 37(5): 595-600.[18] 徐晓玲, 徐秀峰, 张国涛, 牛宪军. 钴铝复合氧化物负载金催化剂的制备及催化分解N2O[J]. 燃料化学学报, 2009, 37(5): 595-600.

    22. [22]

      (XU Xiao-ling, XU Xiu-feng, ZHANG Guo-tao, NIU Xian-jun. Preparation of Co-Al mixed oxide supported gold catalysts and their catalytic activity for N2O decomposition[J]. Journal of Fuel Chemistry and Technology, 2009, 37(5): 595-600.)(XU Xiao-ling, XU Xiu-feng, ZHANG Guo-tao, NIU Xian-jun. Preparation of Co-Al mixed oxide supported gold catalysts and their catalytic activity for N2O decomposition[J]. Journal of Fuel Chemistry and Technology, 2009, 37(5): 595-600.)

    23. [19] LEE S J, GAVRIILIDIS A. Supported Au catalysts for low-temperature CO oxidation prepared by impregnation[J]. J Catal, 2002, 206(2): 305-313.[19] LEE S J, GAVRIILIDIS A. Supported Au catalysts for low-temperature CO oxidation prepared by impregnation[J]. J Catal, 2002, 206(2): 305-313.

    24. [20] KUNG H H, KUNG M C, COSTELLO C K. Supported Au catalysts for low temperature CO oxidation[J]. J Catal, 2003, 216(1/2): 425-432.[20] KUNG H H, KUNG M C, COSTELLO C K. Supported Au catalysts for low temperature CO oxidation[J]. J Catal, 2003, 216(1/2): 425-432.

    25. [21] MANIAK G, STELMACHOWSKI P, KOTARBA A, SOJKA Z, RICO-PÉREZ V, BUENO-LÓPEZ A. Rationales for the selection of the best precursor for potassium doping of cobalt spinel based deN2O catalyst[J]. Appl Catal B: Environ, 2013, 136-137: 302-307.[21] MANIAK G, STELMACHOWSKI P, KOTARBA A, SOJKA Z, RICO-PÉREZ V, BUENO-LÓPEZ A. Rationales for the selection of the best precursor for potassium doping of cobalt spinel based deN2O catalyst[J]. Appl Catal B: Environ, 2013, 136-137: 302-307.

    26. [22] LIN J N, CHEN J H, HSIAO C Y, KANG Y M, WAN B Z. Gold supported on surface acidity modified Y-type and iron/Y-type zeolite for CO oxidation[J]. Appl Catal B: Environ, 2002, 36(1): 19-29.[22] LIN J N, CHEN J H, HSIAO C Y, KANG Y M, WAN B Z. Gold supported on surface acidity modified Y-type and iron/Y-type zeolite for CO oxidation[J]. Appl Catal B: Environ, 2002, 36(1): 19-29.

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  • 收稿日期:  2013-04-08
  • 网络出版日期:  2013-06-12
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