新型铈钨钛复合氧化物催化还原脱硝机理

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摘要利用水热共沉淀法制备了铈钨钛复合氧化物催化剂，考察了H₂O₂络合修饰对其催化脱硝转化频率（TOF）的影响；并借助傅里叶原位红外光谱仪研究了H₂O₂络合修饰后铈钨钛复合氧化物的催化脱硝机理.结果表明：H₂O₂络合修饰可增强铈钨钛复合氧化物表面Brønsted酸位强度，提高其表面NH₃低温吸附和中低温NH₃-SCR脱硝性能，400℃时其NO_x催化脱除频率TOF高达0.658s^-1；NH₃和NO_x在H₂O₂络合修饰后铈钨钛复合氧化物表面存在竞争吸附，其表面催化脱硝反应主要为吸附态NH₃、NH₂和NH₄⁺与气态NO+O₂的反应，其低温NH₃-SCR反应机理遵循Eley-Rideal（E-R）机理.

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	刘晶
	熊志波
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	张磊

关键词 ：选择性催化还原脱硝, 铈钨钛复合氧化物, H₂O₂络合修饰, 转化频率, 脱硝机理

Abstract：Influence of H₂O₂ complex modification on the NH₃-SCR Turnover Frequency (TOF) of cerium-tungsten-titanium mixed oxide catalyst prepared through the hydrothermal co-precipitation method was investigated. And the NH₃-SCR mechanism for the catalyst modified by H₂O₂ complex was also studied by Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). The results indicated that the intensity of Brønsted acid for mixed oxide was improved by H₂O₂ complex modification. Its low-temperature NH₃ adsorption ability and low-medium temperature NH₃-SCR activity were enhanced. The TOF value of NO_x reduction at 400℃ was 0.658s^-1 for the catalyst modified by H₂O₂ complex. There existed the competitive adsorption of NH₃ and NO_x on its surface. The NH₃-SCR reaction was mainly the reaction between the adsorption of NH₃ group (NH₃, NH₂ and NH₄⁺) and the gaseous NO_x on the surface of cerium-tungsten-titanium mixed oxide catalyst modified by H₂O₂ complex, and its low-temperature NH₃-SCR mechanism obeys the Eley-Rideal mechanism.

Key words： selective catalytic reduction of NO_x with NH₃ cerium-tungsten-titanium mixed oxide H₂O₂ complex modification turnover frequency mechanism

收稿日期: 2017-09-27

X51

基金资助:国家自然科学基金资助项目（51406118）；上海市青年东方学者岗位计划资助项目（QD2015017）；上海理工大学流动控制与仿真重点实验室资助项目（D15013）

通讯作者: 熊志波,副教授,xzb328@163.com E-mail: xzb328@163.com

作者简介: 刘晶(1993-),女,山东泰安人,上海理工大学硕士研究生,主要从事燃煤电厂氮氧化物催化脱除方向研究.发表论文1篇.

引用本文:

刘晶, 熊志波, 周飞, 金晶, 陆威, 张磊. 新型铈钨钛复合氧化物催化还原脱硝机理[J]. 中国环境科学, 2018, 38(5): 1670-1676. LIU Jing, XIONG Zhi-bo, ZHOU Fei, JIN Jing, LU Wei, ZHANG Lei. The NH₃-SCR mechanism of a novel cerium-tungsten-titanium mixed oxide catalyst prepared through the hydrothermal co-precipitation method modified by H₂O₂ complex. CHINA ENVIRONMENTAL SCIENCECE, 2018, 38(5): 1670-1676.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2018/V38/I5/1670

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