摘要
采用等体积浸渍法、旋转真空浸渍法、机械化学法和机械化学/旋转真空浸渍法分别制备了IWIP、RVIP、MC和MC/RVIP四种Ni/ZSM-5催化剂.通过XRD、H_(2)-TPR、NH_(3)-TPD、N2吸附/脱附、SEM、EDX-mapping、TG-DTG和H_(2)-TPH等分析催化剂的晶相结构、还原性、酸碱性、织构性质、微观形貌和积炭含量.结果表明,IWIP催化剂的Ni颗粒尺寸较大,金属-载体相互作用较弱,主要是游离态α-NiO.RVIP催化剂的活性组分前驱体在真空状态下被充分浸入载体孔隙内部,较大的比表面积有助于提高RVIP催化剂活性金属的分散性.MC和MC/RVIP催化剂的Ni颗粒尺寸较小,且金属-载体相互作用显著增强.在温度为250~550℃、压力为0.1 MPa、CO_(2)流量为80 mL·min^(-1)、CO_(2)∶H_(2)体积比4∶1条件下反应10 h评价催化剂反应性能,MC/RVIP催化剂表现出最佳的反应活性,其CO_(2)转化率、CH4选择性分别为84.8%、94.1%.通过稳定性测试发现,MC/RVIP催化剂的稳定性效果较好,反应后催化剂的积炭量较少,活性较高,积炭类型主要是β型炭物种.
Four Ni/ZSM-5 catalysts of IWIP,RVIP,MC,and MC/RVIP were prepared by incipient-wetness impregnation method,rotary vacuum impregnation,mechanochemical method and mechanochemical/rotary vacuum impregnation,respectively.And the crystal structure,reducibility,acidity and alkalinity,texture properties,microstructure and carbon deposition of the catalyst were analyzed by XRD,H_(2)-TPR,NH_(3)-TPD,N2 adsorption/desorption,SEM,EDX mapping,TG-DTG,and H_(2)-TPH.The results show that IWIP catalyst shows large Ni particle size,with the weak metal-support interaction,and NiO species mainly exists in the form of α-NiO.RVIP catalyst can fully immerse the active component precursor into the pores of the support at vacuum conditions and presents a large specific surface area,which is beneficial for improving the dispersion of active components.MC catalyst and MC/RVIP catalyst show the smaller Ni particle size and stronger metal-support interaction.The catalytic performance was evaluated under the following conditions:temperature of 250 to 550℃,pressure of 0.1 MPa,CO_(2) flow rate of 80 mL·min^(-1),CO_(2):H_(2) volume ratio of 4:1,with the reaction conducted for 10 h.The MC/RVIP catalyst demonstrated the highest activity,with CO_(2) conversion of 84.8%,CH4 selectivity of 97.1%and CH4 yield of 79.8%,and this catalyst also shows well stability test.The carbon deposition of the catalyst after the stability test is low,and the carbon deposition type is mainly β-type carbon species.
作者
黄贤金
莫文龙
马童童
丛兴顺
卢立菊
马亚亚
王锋
杨晓勤
HUANG Xianjin;MO Wenlong;MA Tongtong;CONG Xingshun;LU Liju;MA Yaya;WANG Feng;YANG Xiaoqin(College of Chemical and Textile Engineering,Xinjiang College of Science&Technology,Korla,Xinjiang 841000,China;State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources and Key Laboratory of Coal Clean Conversion&Chemical Engineering Process(Xinjiang Uyghur Autonomous Region),College of Chemical Engineering,Xinjiang University,Urumqi,Xinjiang 830017,China;School of Chemistry,Chemical Engineering,and Materials Science,Zaozhuang University,Zaozhuang,Shandong 277160,China;Xinjiang Yihua Chemical Industry Co.,Ltd.,Changji,Xinjiang 831700,China)
出处
《分子催化(中英文)》
北大核心
2025年第5期405-414,I0001,I0002,共12页
Journal of Molecular Catalysis(China)
基金
中央引导地方科技发展专项(ZYYD2022C16)
新疆维吾尔自治区天山创新团队计划(2025D14013)
昌吉州科技支撑产业高质量发展专项(2022Z04)。
