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Interface sites on vanadia-based catalysts are highly active for No_(x) removal under realistic conditions

Journal of Environmental Sciences 2024年第2期136卷 523-536页

作者： Zhihui Lv Guangzhi He Wenshuo Zhang Jingjing Liu Zhihua Lian Yang Yang Zidi Yan Guangyan Xu Wenpo Shan Yunbo Yu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China Center for Excellence in Regional Atmospheric Environment and Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China Ningbo Research Center for Urban Environment Chinese Academy of SciencesNingbo 315800China

tio_(2)-supported v_(2)o_(5)catalysts are commonly used in No_(x)reduction with ammonia due to their robust catalytic performance.over these catalysts,it is generally considered that the active species are mainly derived from the vanadia species rather than the intrinsic structure of v-o-ti entities,namely the interface sites.To reveal the role of v-o-ti entities in NH_(3)-SCR,herein,we prepared tio_(2)/v_(2)o_(5)catalysts and demonstrated that v-o-ti entities were more active for No_(x)reduction under wet conditions than the v sites(v=o)working alone.on the v-o-ti entities,kinetic measurements and first principles calculations revealed that NH_(3)activation exhibited a much lower energy barrier than that on v=o sites.Under wet conditions,the v-o-ti interface significantly inhibited the transformation of v=o to v-oH sites thus benefiting NH_(3)activation.Under wet conditions,meanwhile,the migration of NH_(4)^(+)from ti site neighboring the v-o-ti interface to ti site of the v-o-ti interface was exothermic;thus,v-o-ti entities together with neighboring ti sites could serve as channels linking NH_(3)pool and active centers for activation of NH_(4)^(+).This finding reveals that the v-o-ti interface sites on v-based catalysts play a crucial role in No_(x)removal under realistic conditions,providing a new perspective on NH_(3)-SCR mechanism.

关键词： No_(x)removal vanadia-based catalysts v-o-ti entities Interface sites Reaction mechanism

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