载体性质对Pt催化剂H2选择催化还原NOx活性和选择性的影响

doi:10.1016/S1872-2067(14)60197-2

催化学报 ›› 2015, Vol. 36 ›› Issue (2): 197-203.DOI: 10.1016/S1872-2067(14)60197-2

载体性质对Pt催化剂H₂选择催化还原NO_x活性和选择性的影响

李新燕, 张肖肖, 徐永贞, 柳叶, 王新平

大连理工大学环境科学与技术学院, 工业生态学和环境工程重点实验室和精细化工重点实验室, 辽宁大连116024

收稿日期:2014-07-05 修回日期:2014-07-16 出版日期:2015-01-21 发布日期:2015-01-21
通讯作者: 王新平
基金资助:
国家自然科学基金(21177016, 21277019).

Influence of support properties on H₂ selective catalytic reduction activities and N₂ selectivities of Pt catalysts

Xinyan Li, Xiaoxiao Zhang, Yongzhen Xu, Ye Liu, Xinping Wang

Key Laboratory of Industrial Ecology and Enironmental Engineering (MOE) and State Key Laboratory of Fine Chemical, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, Liaoning, China

Received:2014-07-05 Revised:2014-07-16 Online:2015-01-21 Published:2015-01-21
Supported by:
This work was supported by the National Natural Science Foundation of China (21177016, 21277019).

摘要/Abstract

摘要：

研究了Pt/MgO, Pt/γ-Al₂O₃, Pt/ZrO₂和Pt/HZSM-5催化剂上H₂选择催化还原消除NO_x(H₂-SCR)反应. 结果发现, H₂-SCR活性和N₂生成选择性受催化剂中Pt的金属性以及载体的氮氧化物吸附能力影响很大. HZSM-5的表面酸性使载体对NO_x吸附能力较小, 使担载Pt以较高的金属性存在, 从而导致Pt/HZSM-5催化剂的高活性和高选择性. 相反, Pt/MgO和Pt/γ-Al₂O₃催化剂较差的活性和选择性可归因于其载体的碱性表面、催化剂中Pt较低的金属性以及载体对氮氧化物较大的吸附能力. 结合反应的原位红外光谱结果可以认为, 在Pt/载体界面处亚硝酸根/硝酸根物种被还原为N₂或N₂O, 取决于该处参与反应的活性H与这些含氮物种的相对数目.

关键词: 氢气活化, 氮氧化物吸附, 选择性催化还原, 氮气选择性, 氢溢流

Abstract:

The selective catalytic reduction of NO_x by H₂ (H₂-SCR) was studied over Pt/MgO, Pt/γ-Al₂O₃, Pt/ZrO₂, and Pt/HZSM-5 catalysts. The H₂-SCR activities and N₂ selectivities of the catalysts were strongly influenced by the amounts of Pt metal in the catalysts and the NO_x adsorption capacities of the supports. The acidic surface of HZSM-5 increased the amount of metallic Pt on the support, decreasing the NO_x adsorption capacity, resulting in much higher H₂-SCR activity and N₂ selectivity. The inferior activities of Pt/MgO and Pt/γ-Al₂O₃ are ascribed to the low amounts of metallic Pt and large NO_x adsorption capacities of the supports as a result of their basic surfaces. Based on these results and in situ Fourier transform infrared spectroscopic studies of the reaction, it is proposed that the reduction products of nitrite/nitrate species at the Pt/support interface are N₂ or N₂O, depending on the relative amounts of active hydrogen and nitrous species involved in the reduction.

Key words: Hydrogen activation, Nitrogen oxide adsorption, Selective catalytic reduction, Nitrogen selectivity, Hydrogen-spillover

李新燕, 张肖肖, 徐永贞, 柳叶, 王新平. 载体性质对Pt催化剂H₂选择催化还原NO_x活性和选择性的影响[J]. 催化学报, 2015, 36(2): 197-203.

Xinyan Li, Xiaoxiao Zhang, Yongzhen Xu, Ye Liu, Xinping Wang. Influence of support properties on H₂ selective catalytic reduction activities and N₂ selectivities of Pt catalysts[J]. Chinese Journal of Catalysis, 2015, 36(2): 197-203.

×
扫码分享

导出引用管理器 EndNote|Ris|BibTeX

链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(14)60197-2

https://www.cjcatal.com/CN/Y2015/V36/I2/197

参考文献

[1] Liu Z M, Woo S I. Catal Rev-Sci Eng, 2006, 48: 43
[2] Choo S T, Lee Y G, Nam I S, Ham S, Lee J B. Appl Catal A, 2000, 200: 177
[3] Nakajima F, Hamada I. Catal Today, 1996, 29: 109
[4] Gutberlet H, Schallert B. Catal Today, 1993, 16: 207
[5] Costa C N, Savva P G, Fierro J L G, Efstathiou A M. Appl Catal B, 2007, 75: 147
[6] Obuchi A, Ohi A, Nakamura M, Ogata A, Mizuno K, Ohuchi H. Appl Catal B, 1993, 2: 71
[7] Liu Z M, Woo S I, Lee W S. J Phys Chem B, 2006, 110: 26019
[8] Yu Q, Wang X P, Xing N, Yang H L, Zhang S X. J Catal, 2007, 245: 124
[9] Shelef M, Jones J H, Kummer J T, Otto K, Weaver E E. Environ Sci Technol, 1971, 5: 790
[10] Frank B, Emig G, Renken A. Appl Catal B, 1998, 19: 45
[11] Salama T M, Ohnishi R, Ichikawa M. Chem Commun, 1997: 105
[12] Costa C N, Efstathiou A M. Appl Catal B, 2007, 72: 240
[13] Itoh M, Motoki K, Saito M, Iwamoto J, Machida K. Bull Chem Soc Jpn, 2009, 82: 1197
[14] Machida M, Watanabe T. Appl Catal B, 2004, 52: 281
[15] Olympiou G G, Efstathiou A M. Chem Eng J, 2011, 170: 424
[16] Park S M, Kim M Y, Kim E S, Han H S, Seo G. Appl Catal A, 2011, 395: 120
[17] Hamada S, Hibarino S, Ikeue K, Machida M. Appl Catal B, 2007, 74: 197
[18] Hamada S, Ikeue K, Machida M. Appl Catal B, 2007, 71: 1
[19] Schott F J P, Balle P, Adler J, Kureti S. Appl Catal B, 2009, 87: 18
[20] Li L D, Wu P, Yu Q, Wu G J, Guan N J. Appl Catal B, 2010, 94: 254
[21] Machida M, Ikeda S, Kurogi D, Kijima T. Appl Catal B, 2001, 35: 107
[22] Costa C N, Efstathiou A M. J Phys Chem C, 2007, 111: 3010
[23] Burch R, Coleman M D. J Catal, 2002, 208: 435
[24] Satsuma A, Hashimoto M, Shibata J, Yoshida H, Hattori T. Chem Commun, 2003: 1698
[25] Shibata J, Hashimoto M, Shimizu K, Yoshida H, Hattori T, Satsuma A. J Phys Chem B, 2004, 108: 18327
[26] Wu P, Li L D, Yu Q, Wu G J, Guan N J. Catal Today, 2010, 158: 228
[27] Burch R, Shestov A A, Sullivan J A. J Catal, 1999, 186: 353
[28] Yang J I, Jung H. Chem Eng J, 2009, 146: 11
[29] Burch R, Millington P J, Walker A P. Appl Catal B, 1994, 4: 65
[30] Marina O A, Yentekakis I V, Vayenas C G, Palermo A, Lambert R M. J Catal, 1997, 166: 218
[31] Li J, Wu G J, Guan N J, Li L D. Catal Commum, 2012, 24: 38
[32] Pitchon V, Fritz A. J Catal, 1999, 186: 64
[33] Yazawa Y, Takagi N, Yoshida H, Komai S, Satsuma A, Tanaka T, Yoshida S, Hattori T. Appl Catal A, 2002, 233: 103
[34] Yoshida H, Yazawa Y, Hattori T. Catal Today, 2003, 87: 19
[35] Si Z C, Weng D, Wu X D, Li J, Li G. J Catal, 2010, 271: 43
[36] Kantcheva M, Vakkasoglu A S. J Catal, 2004, 223: 352
[37] Savva P G, Efstathiou A M. J Catal, 2008, 257: 324

载体性质对Pt催化剂H₂选择催化还原NO_x活性和选择性的影响

Influence of support properties on H₂ selective catalytic reduction activities and N₂ selectivities of Pt catalysts

PDF

可视化

摘要/Abstract

引用本文

使用本文

扫码分享

参考文献

相关文章 15

编辑推荐

Metrics

[1]	孙传智, 陈葳, 贾轩轩, 刘安鼐, 高飞, 冯帅, 董林. Sm掺杂对Fe₂O₃催化剂NH₃-SCR反应活性及抗水抗硫性作用[J]. 催化学报, 2021, 42(3): 417-430.
[2]	刘晓娜, 曹毅, 闫娜娜, 马超, 曹磊, 郭鹏, 田鹏, 刘中民. Cu-SAPO-17:一种新颖的NO_x选择性催化还原催化剂[J]. 催化学报, 2020, 41(11): 1715-1722.
[3]	张祎旸, 曾慧, 贾斌, 王智华, 刘志明. Pd/TiO₂催化剂上氢气选择性催化还原NO_x的研究[J]. 催化学报, 2019, 40(6): 849-855.
[4]	姚小江, 曹俊, 陈丽, 亢科科, 陈阳, 田密, 杨复沫. MnO_x/CeO₂纳米棒催化剂在低温NH₃-SCR反应中的阳离子(Zr⁴⁺,Al³⁺,Si⁴⁺)掺杂效应[J]. 催化学报, 2019, 40(5): 733-743.
[5]	明淑君, 庞磊, 范驰, 郭文, 董亚浩, 刘鹏, 陈真, 李涛. 柴油机尾气中的碱性无机污染物引起Cu-SAPO-18脱硝催化剂的化学失活[J]. 催化学报, 2019, 40(4): 590-599.
[6]	曹俊, 姚小江, 杨复沫, 陈丽, 傅敏, 汤常金, 董林. Ce⁴⁺,Zr⁴⁺共掺杂提高V₂O₅-WO₃/TiO₂催化剂脱硝性能及抗K中毒能力[J]. 催化学报, 2019, 40(1): 95-104.
[7]	陈传敏, 曹悦, 刘松涛, 陈建猛, 贾文波. 改性钒钛基SCR催化剂的研究进展[J]. 催化学报, 2018, 39(8): 1347-1365.
[8]	方亚蓉, 郭彦炳. 铜基非贵金属异相催化剂在环境修复中的应用[J]. 催化学报, 2018, 39(4): 566-582.
[9]	文叶轩, 曹爽, 费晓琦, 王海强, 吴忠标. 一步水热法合成具有(001)高能晶面的SO₄^2--TiO₂及其NH₃-SCR脱硝性能[J]. 催化学报, 2018, 39(4): 771-778.
[10]	盛重义, 麻丁仁, 俞丹青, 肖香, 黄冰洁, 杨柳, 王圣. 低温NH₃-SCR新型MnO_x@TiO₂纳米棒核壳结构催化剂的合成及抗SO₂性能研究[J]. 催化学报, 2018, 39(4): 821-830.
[11]	李伟, 张成, 李鑫, 谭鹏, 周安鹂, 方庆艳, 陈刚. Ho改性的Mn-Ce/TiO₂催化剂低温脱硝性能的评价和表征[J]. 催化学报, 2018, 39(10): 1653-1663.
[12]	许文晋, 张光旭, 陈晗炜, 张国孟, 韩洋, 常意川, 龚鹏. Mn/beta与Mn/ZSM-5催化剂对氨选择性催化还原NO的低温催化活性比较:锰前驱体的影响[J]. 催化学报, 2018, 39(1): 118-127.
[13]	周调云, 苑青, 潘秀莲, 包信和. 碳化硅上生长Cu/SSZ-13分子筛及其NH₃-SCR催化性能[J]. 催化学报, 2018, 39(1): 71-78.
[14]	沈行加, 吴先元, 江大好, 李小年, 倪珺. 利用原位红外光谱确证Ru/SBA-15的加氢活性位点[J]. 催化学报, 2017, 38(9): 1597-1602.
[15]	齐凯, 谢峻林, 方德, 李凤祥, 何峰. N₂气氛下焙烧制备的Mn基催化剂催化NO_x脱除性能的提升机理:低MnO_x结晶度与氧化度[J]. 催化学报, 2017, 38(5): 845-852.