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作 者:高飞 刘志松 潘珂珂 刘敏敏 代斌[1] 但建明[1] 于锋[1,2] GAO Fei;LIU Zhisong;PAN Keke;LIU Minmin;DAI Bin;DAN Jianming;YU Feng(Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan,School of Chemistry and Chemical Engineering,Shihezi University,Shihezi 832003,Xinjiang,China;Carbon Neutralization and Environmental Catalytic Technology Laboratory,Bingtuan Industrial Technology Research Institute,Shihezi University,Shihezi 832003,Xinjiang,China)
机构地区:[1]石河子大学化学化工学院化工绿色过程兵团重点实验室,新疆石河子832003 [2]石河子大学兵团工业技术研究院碳中和与环境催化技术研究室,新疆石河子832003
出 处:《化工进展》2024年第4期1851-1862,共12页Chemical Industry and Engineering Progress
基 金:兵团区域创新计划(2021BB005);兵团科技创新团队计划(2020CB006);兵团重大科技计划(2018AA002)。
摘 要:以CO为还原剂去除NO的选择性催化还原(CO-SCR)技术受到了广泛关注。本文以天然矿物蛭石为载体,采用共沉淀辅助浸渍法(CP-IM)制备了蛭石负载的铁铈双金属氧化物(FeCe/VMT)用于CO-SCR脱硝反应。表征结果显示,相比传统的浸渍法(IM),共沉淀辅助浸渍制备的FeCe/VMT催化剂具有更大的比表面积(106.9m^(2)/g)和更多氧空位,可以提供更多的活性位点。共沉淀过程形成更多Fe^(3+),并促进了FeCe间的协同作用,有利于提高CO-SCR的催化活性和稳定性。性能测试表明,在300℃和50000h^(−1)的空速下,NO转化率可达100%,48h后NO转化率几乎无衰减。当温度降至250℃时,NO的转化率依然可以达到97%。同时,利用原位红外光谱和密度泛函理论计算技术,揭示了相应的催化反应机理,为制备大比表面积的负载型催化剂提供了一种方法。NO removal by CO selective catalytic reduction(CO-SCR)has gained great attentions.In this paper,vermiculite-supported Fe-Ce bimetallic oxides(FeCe/VMT)for CO-SCR were prepared by coprecipitation-assisted impregnation(CP-IM)with the natural mineral vermiculite as the carrier.The characterization results showed that compared with the traditional impregnation method(IM),FeCe/VMT(CP-IM)prepared by coprecipitation-assisted impregnation had larger specific surface area(106.9m^(2)/g)and more oxygen vacancies due to more active sites available.The enhanced synergistic effect between FeCe was beneficial to the increase of both catalytic activity and stability in CO-SCR reaction.Performance tests showed that NO conversion reached 100%at 300℃with 50000h^(−1) gas hourly space velocity(GHSV),and the performance of the catalyst didn’t decrease within 48h.When the temperature dropped to 250℃,the conversion of NO could still reach 97%.At the same time,in situ infrared spectroscopy and density functional theory were used to reveal the corresponding catalytic mechanism.This research provided a promising method for preparing supported catalysts with large specific surface area.
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