Ni-Ce复合协同促进CO同步催化去除NO的性能和机理  

Performance and mechanism of Ni-Ce composite synergistically promoting CO-selective catalytic reduction of NO

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作  者:马倩 王赫[1,2] 屈嘉鑫 吉硕 王薇 黄宇 党小庆[1] MA Qian;WANG He;QU Jia-xin;JI Shuo;WANG Wei;HUANG Yu;DANG Xiao-qing(School of Environment&Municipal Engineering,Xi’an University of Architecture&Technology,Xi’an 710055,China;Key Laboratory of Northwest Water Resource,Environment,and Ecology,Ministry of Education,Key Laboratory of Environmental Engineering of Shaanxi Province,Xi’an 710055,China;Xi’an Institute for Innovative Earth Environment Research,Xi’an 710061,China;State Key Laboratory of Loess and Quaternary Geology,Key Laboratory of Aerosol Chemistry and Physics,Institute of Earth Environment,Chinese Academy of Sciences,Xi’an 710061,China)

机构地区:[1]西安建筑科技大学环境与市政工程学院,陕西西安710055 [2]陕西省环境工程重点实验室,西北水资源与环境生态教育部重点实验室,陕西西安710055 [3]西安地球环境创新研究所,陕西西安710061 [4]中国科学院地球环境研究所,气溶胶化学与物理重点实验室,黄土与第四纪地质国家重点实验室,陕西西安710061

出  处:《中国环境科学》2025年第2期671-681,共11页China Environmental Science

基  金:陕西省重点研发计划项目(2024SF-ZDCYL-05-06,2024SFYBXM-569)。

摘  要:采用水热法制备了双金属NiCe-x(x=1:3、2:2、3:1、0:1、1:0)催化剂,并应用于CO选择性催化还原NO(CO-SCR)反应.结果显示,与NiO和CeO_(2)催化剂相比,NiCe复合催化剂展现出了优良的低温CO同步催化去除NO的性能,其中NiCe比例为3:1的催化剂在200~450℃的宽温域达到90%以上的NO转化率,并且表现出对H_(2)O和SO_(2)的良好耐受性.利用表征手段对样品的结构和性能进行了探究,发现NiCe双金属催化剂的比表面积较单一金属氧化物均提高,NiCe复合催化剂中Ce^(4+)和Ce^(3+)之间的电子转移增加了催化剂表面的氧空位,Ni和Ce离子共存促使氧化还原循环(Ce^(3+)+Ni^(3+)↔Ce^(4+)+Ni^(2+))增强,进而提高了催化剂脱硝活性.最后,基于原位DRIFTS结果,发现吸附的NCO是NiCe-3:1在CO同步催化去除NO过程中的重要中间物种.The bimetallic NiCe-x(x=1:3,2:2,3:1,0:1,1:0)catalysts were successfully synthesized using the hydrothermal method and subsequently evaluated for their efficacy in the selective catalytic reduction of NO by CO(CO-SCR).The results indicated that compared to NiO and CeO_(2)catalysts,the NiCe composite catalyst exhibited superior performance in simultaneously removing low-temperature CO and NO.Superior performance was demonstrated by the NiCe composite catalyst with a 3:1 ratio,which achieved over 90%NO conversion over an extensive temperature range of 200~450℃and exhibited strong resistance to SO_(2)and H_(2)O.Characterization indicated that the existence of Ni and Ce ions led to an increased specific surface area and accelerated redox cycling(Ce^(3+)+Ni^(3+)↔Ce^(4+)+Ni^(2+)),which improved denitrification activity.In-situ DRIFTS findings confirmed that adsorbed NCO played a crucial role as an intermediate in the CO-SCR process employing NiCe-3:1.

关 键 词:NiCe复合 CO-SCR 氧空位 反应机理 

分 类 号:X701[环境科学与工程—环境工程]

 

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