MnO2的晶相结构和表面性质对低温NH3-SCR反应的影响
采用水热法合成了两种具有相同形貌但是不同物相结构的MnO2纳米棒，分别为隧道状和层状结构。考察其低温NH。选择性催化还原NOx（NH3-SCR）的性能．结果表明MnO2纳米棒的比表面积不是影响活性的主要因素，催化剂的晶相结构和表面性质对催化活性有很大影响，隧道状a-MnO2纳米棒的低温NH3-SCR活性明显高于层状5-MnO2纳米棒．结构分析和NH。程序升温脱附（NH3-TPD）实验表明，a-MnO2纳米棒的暴露晶面（110）面存在大量的配位不饱和Mn离子，形成较多的Lewis酸性位点，而且a-MnO2较弱的Mn—O键和隧道结构都有利于NH。的吸附：而δ-MnO2纳米棒的暴露晶面（001）面上...
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| Published in | 物理化学学报 Vol. 28; no. 7; pp. 1771 - 1776 |
|---|---|
| Main Author | |
| Format | Journal Article |
| Language | Chinese |
| Published |
清华大学环境学院,环境模拟与污染控制国家重点联合实验室,北京100084%复旦大学环境科学与工程系,上海,200433
2012
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| Subjects | |
| Online Access | Get full text |
| ISSN | 1000-6818 |
| DOI | 10.3866/PKU.WHXB201204175 |
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| Abstract | 采用水热法合成了两种具有相同形貌但是不同物相结构的MnO2纳米棒，分别为隧道状和层状结构。考察其低温NH。选择性催化还原NOx（NH3-SCR）的性能．结果表明MnO2纳米棒的比表面积不是影响活性的主要因素，催化剂的晶相结构和表面性质对催化活性有很大影响，隧道状a-MnO2纳米棒的低温NH3-SCR活性明显高于层状5-MnO2纳米棒．结构分析和NH。程序升温脱附（NH3-TPD）实验表明，a-MnO2纳米棒的暴露晶面（110）面存在大量的配位不饱和Mn离子，形成较多的Lewis酸性位点，而且a-MnO2较弱的Mn—O键和隧道结构都有利于NH。的吸附：而δ-MnO2纳米棒的暴露晶面（001）面上的Mn离子已达到配位饱和，所以其表面Lewis酸性位点较少．X射线光电子能谱（XPS）和热重（TG）分析表明a-MnO2纳米棒的表面更有利于NH3和NOX的活化．具有有利于吸附NH3和活化NH3和N0x的表面性质和晶型结构，是a-MnO：纳米棒活性高的主要原因． |
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| AbstractList | 采用水热法合成了两种具有相同形貌但是不同物相结构的MnO2纳米棒，分别为隧道状和层状结构。考察其低温NH。选择性催化还原NOx（NH3-SCR）的性能．结果表明MnO2纳米棒的比表面积不是影响活性的主要因素，催化剂的晶相结构和表面性质对催化活性有很大影响，隧道状a-MnO2纳米棒的低温NH3-SCR活性明显高于层状5-MnO2纳米棒．结构分析和NH。程序升温脱附（NH3-TPD）实验表明，a-MnO2纳米棒的暴露晶面（110）面存在大量的配位不饱和Mn离子，形成较多的Lewis酸性位点，而且a-MnO2较弱的Mn—O键和隧道结构都有利于NH。的吸附：而δ-MnO2纳米棒的暴露晶面（001）面上的Mn离子已达到配位饱和，所以其表面Lewis酸性位点较少．X射线光电子能谱（XPS）和热重（TG）分析表明a-MnO2纳米棒的表面更有利于NH3和NOX的活化．具有有利于吸附NH3和活化NH3和N0x的表面性质和晶型结构，是a-MnO：纳米棒活性高的主要原因． O643; 采用水热法合成了两种具有相同形貌但是不同物相结构的MnO2纳米棒,分别为隧道状和层状结构,考察其低温NH3选择性催化还原NOx(NH3-SCR)的性能.结果表明MnO2纳米棒的比表面积不是影响活性的主要因素,催化剂的晶相结构和表面性质对催化活性有很大影响,隧道状α-MnO2纳米棒的低温NH3-SCR活性明显高于层状δ-MnO2纳米棒.结构分析和NH3程序升温脱附(NH3-TPD)实验表明,α-MnO2纳米棒的暴露晶面(110)面存在大量的配位不饱和Mn离子,形成较多的Lewis酸性位点,而且α-MnO2较弱的Mn-O键和隧道结构都有利于NH3的吸附;而δ-MnO2纳米棒的暴露晶面(001)面上的Mn离子已达到配位饱和,所以其表面Lewis酸性位点较少.X射线光电子能谱(XPS)和热重(TG)分析表明α-MnO2纳米棒的表面更有利于NH3和NOx的活化.具有有利于吸附NH3和活化NH3和NOx的表面性质和晶型结构,是α-MnO2纳米棒活性高的主要原因. |
| Abstract_FL | Two manganese oxides with the same nanorod-shaped morphology but different crystal structures,tunnel and layer structures,were synthesized and investigated for selective catalytic reduction of NOx with NH3 (NH3-SCR) at low temperature.Tunneled α-MnO2 had much higher catalytic activity than layered δ-MnO2 under the same reaction conditions.Experiment results revealed that the surface area was not the main factor to affect the NH3-SCR activities over the MnO2 nanorods and that the activities were structure sensitive.Structure analysis and temperature-programmed desorption experiments of NH3 (NH3-TPD) suggested that the exposed (110) plane of α-MnO2 had many Mn cations in coordinatively unsaturated environment,while all of the Mn cations on the exposed (001) plane of δ-MnO2 were in coordinatively saturated environment.Thus,α-MnO2 possessed many more Lewis acid sites.Furthermore,α-MnO2 has weaker Mn - O bonds and an efficient tunnel structure,which are favorable characteristics for NH3 adsorption.Moreover,X-ray photoelectron spectroscopy (XPS) and thermal gravimetric (TG) analysis indicated that α-MnO2 obtained a higher capability for NH3 and NOx activation than δ-MnO2.The crystal structure and surface properties of α-MnO2 are more suitable to the adsorption of NH3 and activation of NH3and NOx,which accounts for the higher catalytic activity of the α-MnO2 nanorods. |
| Author | 戴韵 李俊华 彭悦 唐幸福 |
| AuthorAffiliation | 清华大学环境学院,环境模拟与污染控制国家重点联合实验室,北京100084 复旦大学环境科学与工程系,上海200433 |
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| Author_FL | DAI Yun LI Jun-Hua PENG Yue TANG Xing-Fu |
| Author_FL_xml | – sequence: 1 fullname: DAI Yun – sequence: 2 fullname: LI Jun-Hua – sequence: 3 fullname: PENG Yue – sequence: 4 fullname: TANG Xing-Fu |
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| Copyright | Copyright © Wanfang Data Co. Ltd. All Rights Reserved. |
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| DocumentTitleAlternate | Effects of MnO2 Crystal Structure and Surface Property on the NH3-SCR Reaction at Low Temperature |
| DocumentTitle_FL | Effects of MnO2 Crystal Structure and Surface Property on the NH3-SCR Reaction at Low Temperature |
| EndPage | 1776 |
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| Keywords | 低温 α-MnO2 晶相结构 NH3-选择性催化还原NOx Low-temperature Surface property Selective catalytic reduction of NOx with NH3 δ-MnO2 表面性质 Crystal structure |
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| Notes | 11-1892/06 DAI Yun, LI Jun-Hua, PENG Yue,TANG Xing-Fu （1.State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beo＇ing 100084, P. R. China; 2.Department of Environmental Science and Engineering, Fudan University, Shanghai 200433, P. R. China） Two manganese oxides with the same nanorod-shaped morphology but different crystal structures, tunnel and layer structures, were synthesized and investigated for selective catalytic reduction of NOx with NH3 （NH3-SCR） at low temperature. Tunneled e-MnO2 had much higher catalytic activity than layered δ-MnO2 under the same reaction conditions. Experiment results revealed that the surface area was not the main factor to affect the NH3-SCR activities over the MnO2 nanorods and that the activities were structure sensitive. Structure analysis and temperature-programmed desorption experiments of NH3 （NH~-TPD） suggested that the exposed （110） plane of e-MnO2 had many Mn cations in coordinatively unsaturated environ |
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| PublicationTitle | 物理化学学报 |
| PublicationTitleAlternate | Acta Physico-Chimica Sinica |
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| PublicationYear | 2012 |
| Publisher | 清华大学环境学院,环境模拟与污染控制国家重点联合实验室,北京100084%复旦大学环境科学与工程系,上海,200433 |
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| Snippet | 采用水热法合成了两种具有相同形貌但是不同物相结构的MnO2纳米棒，分别为隧道状和层状结构。考察其低温NH。选择性催化还原NOx（NH3-SCR）的性能．结果表明MnO2纳米棒的比表... O643; 采用水热法合成了两种具有相同形貌但是不同物相结构的MnO2纳米棒,分别为隧道状和层状结构,考察其低温NH3选择性催化还原NOx(NH3-SCR)的性能.结果表明MnO2纳米棒的比... |
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| SubjectTerms | a-MnO2 NH3-选择性催化还原NOx δ-MnO2 低温 晶相结构 表面性质 |
| Title | MnO2的晶相结构和表面性质对低温NH3-SCR反应的影响 |
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