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Catalytic ozonation of NOx into HNO3 with low concentration ozone over MnOx-CeO2/TiO2: Two-phase synergistic effect of TiO2
Molecular Catalysis ( IF 4.6 ) Pub Date : 2020-07-07 , DOI: 10.1016/j.mcat.2020.111095
Lina Guo , Fanyu Meng , Yiqing Zeng , Yong Jia , Fuping Qian , Shule Zhang , Qin Zhong

Anatase TiO2 (TiO2-A), TiO2-B, and TiO2-B/anatase mixed-phase TiO2 (TiO2-AB) are synthesized, and then utilized as supports for the preparation of Mn-Ce/TiO2-A, Mn-Ce/TiO2-B and Mn-Ce/TiO2-AB, respectively. These catalysts are investigated by various characterizations to understand different phase effect of TiO2 on physicochemical properties and catalytic activities for ozonation of NOx into HNO3, aiming to improve the total NOx removal efficiency during the subsequent wet absorption process. Characterizations reveal that the catalytic performances follow the order of Mn-Ce/TiO2-AB > Mn-Ce/TiO2-B > Mn-Ce/TiO2-A, which is relevant to the surface -OH content, oxygen vacancy amount, and reducibility property. The surface -OH groups participate in the transformation of O3 into reactive oxygen species (ROS), the oxygen vacancies increase the activity of surface -OH for ROS generation, and the superior reducibility property accelerates the cycling of Ce3+ → Ce4+ → Ce3+ reaction. Moreover, OH and HO2 radicals are identified as the main reactive species involved in the ozonation of NOx into HNO3. Especially, Mn-Ce/TiO2-AB presents the best catalytic performance mainly because of the optimal reducibility property.



中文翻译:

NO的催化臭氧X为HNO 3与低浓度的臭氧过的MnO X -CeO 2 /的TiO 2:二相协同的TiO效果2

合成了锐钛矿型TiO 2(TiO 2 -A),TiO 2 -B和TiO 2 -B /锐钛矿混合相TiO 2(TiO 2 -AB),然后用作制备Mn-Ce / TiO的载体2 -A,Mn-Ce / TiO 2 -B和Mn-Ce / TiO 2 -AB。通过各种表征对这些催化剂进行了研究,以了解TiO 2对NOx的物理化学性质和催化活性的不同相作用,以将NO x臭氧化为HNO 3,目的是改善总NO x在随后的湿吸收过程中的去除效率。表征表明,催化性能遵循Mn-Ce / TiO 2 -AB> Mn-Ce / TiO 2 -B> Mn-Ce / TiO 2 -A的顺序,这与表面-OH含量,氧空位量有关以及可还原性属性。表面-OH基团参与O 3向活性氧(ROS)的转化,氧空位增加了表面-OH生成ROS的活性,并且优异的还原性加速了Ce 3+ →Ce 4+的循环→Ce 3+反应。此外,OH和HO 2 自由基被确定为将NO x臭氧化为HNO 3的主要反应物种。尤其是,Mn-Ce / TiO 2 -AB表现出最佳的催化性能,这主要是由于其最佳的还原性。

更新日期:2020-07-07
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