铈钛混合氧化物负载磷钨酸吸附-分解NO<sub><i>x</i></sub>性能

引用本文: 程琳, 王睿. 铈钛混合氧化物负载磷钨酸吸附-分解NO_x性能[J]. 无机化学学报, 2013, 29(6): 1206-1214. doi: 10.3969/j.issn.1001-4861.2013.00.195 shu

Citation: CHENG Lin, WANG Rui. Ce-Ti Mixed Oxides Supported H₃PW₁₂O₄₀ for Effective Adsorption-Decomposition of NO_x[J]. Chinese Journal of Inorganic Chemistry, 2013, 29(6): 1206-1214. doi: 10.3969/j.issn.1001-4861.2013.00.195 shu

铈钛混合氧化物负载磷钨酸吸附-分解NO_x性能

程琳 ,
王睿

基金项目:
国家自然科学基金(No.20576064,20776080,20911120088) 、教育部“新世纪优秀人才”支持计划(No.NECT-05-0584) (No.20576064,20776080,20911120088) 、教育部“新世纪优秀人才”支持计划(No.NECT-05-0584)

教育部博士点基金 (No.20070422087) (No.20070422087)

山东省科技计划(No.2006BS08020,2008GG10006005)资助项目。 (No.2006BS08020,2008GG10006005)

摘要: 通过软化学途径合成了铈钛混合氧化物(CeO₂-TiO₂)载体材料,并分别通过等体积浸渍法和机械研磨法负载磷钨酸(H₃PW₁₂O₄₀)。采用FTIR、XRD、SEM和BET比表面积测定对CeO₂-TiO₂及负载型多酸催化剂进行了表征;考察了负载量、负载方法、吸附温度等因素对催化剂吸附NO_x效率的影响;选取吸附性能最佳的催化剂进行了NO_x催化分解实验,探讨了NO_x吸附-分解机理。结果表明:相对于等体积浸渍法,机械研磨法更适合此类载体负载H₃PW₁₂O₄₀,其NO_x吸附效率均高于H₃PW₁₂O₄₀及载体本身;在0～60%的负载量范围内,随着H₃PW₁₂O₄₀负载量的增加,负载型催化剂吸附NO_x的效率呈先升后降趋势,负载量为40%时NO_x吸附效率最佳,达90%;吸附过程中NO_x与催化剂活性组分H₃PW₁₂O₄₀发生作用,生成NOH⁺;H₃PW₁₂O₄₀二级结构中结晶水对催化剂吸附NO_x有重要作用;当温度从150 ℃升至 450 ℃时,被吸附的NO_x发生分解,分解产物的组成与N₂的收率均受升温速率的影响,升温速率越快,N₂收率越高。向吸附分解NO_x后的催化剂床层通入含有水蒸气的空气,可有效补充NO_x分解过程中H₃PW₁₂O₄₀失去的结晶水,从而恢复催化剂优良的NO_x吸附分解性能,实现催化剂的有效再生利用。

关键词:

铈钛混合氧化物;磷钨酸;NO_x;吸附-分解

English

Ce-Ti Mixed Oxides Supported H₃PW₁₂O₄₀ for Effective Adsorption-Decomposition of NO_x

CHENG Lin ,
WANG Rui

1.
School of Environmental Science & Engineering, Shandong University, Jinan 250100, China
Received Date: 11 October 2012
Fund Project:
国家自然科学基金(No.20576064,20776080,20911120088) 、教育部“新世纪优秀人才”支持计划(No.NECT-05-0584)

教育部博士点基金 (No.20070422087)

山东省科技计划(No.2006BS08020,2008GG10006005)资助项目。

Abstract: Ce-Ti mixed oxides (CeO₂-TiO₂) were prepared as the support for solid tungstophosphoric acid (H₃PW₁₂O₄₀). FTIR, XRD, BET surface area measurement, SEM and TPD-MS were employed for characterization and mechanism analysis. CeO₂-TiO₂ is an excellent support for H₃PW₁₂O₄₀. By loading on CeO₂-TiO₂, the NO_x adsorption efficiency of H₃PW₁₂O₄₀ increases, with a peak efficiency of 90%, which is much higher than that of H₃PW₁₂O₄₀ (60%). With the increase of H₃PW₁₂O₄₀ loading, the NO_x adsorption efficiency tends to reach a peak value before dropping down. The mechanical grinding method is superior to the incipient impregnation method for preparing H₃PW₁₂O₄₀/CeO₂-TiO₂. In NO_x adsorption process, NO_x reacts with H₃PW₁₂O₄₀ to produce NOH⁺. The crystal water in the secondary structure of H₃PW₁₂O₄₀ plays an important role in NO_x adsorption. The lost crystal water and oxygen vacancy can be effectively compensated by adding water vapor to regenerate the catalyst. Furthermore, the adsorbed NO_x is decomposed into N₂, O₂ and N₂O, and rapid heating contributes significantly to the decomposition of NO_x over the catalyst, where a yield of 30.5% is achieved for N₂ with the supported catalyst at a temperature ramp of 50 ℃·min^-1.

Key words:

Ce-Ti mixed oxides;H₃PW₁₂O₄₀;NO_x;adsorption-decomposition

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沈阳化工大学材料科学与工程学院沈阳 110142

铈钛混合氧化物负载磷钨酸吸附-分解NO_x性能

English

Ce-Ti Mixed Oxides Supported H₃PW₁₂O₄₀ for Effective Adsorption-Decomposition of NO_x

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铈钛混合氧化物负载磷钨酸吸附-分解NOx性能

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