Operando拉曼光谱技术在铁基费托合成和二氧化碳加氢反应中的应用
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摘要
催化剂是多相催化反应的核心,由于催化反应的复杂性,人类对于催化剂活性相的认知十分有限。反应过程中催化剂构-效关系的构建对于理解催化反应过程和改进催化剂至关重要,动态现场原位(Operando)技术能实时监测催化剂结构演变并在线检测反应产物,促进工业催化剂的理性设计。本文首先介绍了催化反应和动态现场原位表征技术的发展历史,并结合近期的研究进展,描述了Operando拉曼技术在铁基费托合成(Fischer-Tropsch synthesis(FTS))和二氧化碳加氢两种典型催化反应中的应用,展示了不同预处理和前驱体条件下,催化剂的结构演变过程及构-效关系。然而,目前Operando技术的时间分辨率和空间分辨率仍需进一步提升,此外,Operando技术在固液,气液催化反应中仍具有巨大的开发潜力。
Catalysts are the core of heterogeneous catalytic reactions.Due to the complexity of catalytic reactions,humans have very limited knowledge of the active phases of the catalysts.The structure-performance relationship of the catalyst during the reaction is important for understanding the catalytic reaction process and improving the catalyst.The Operandotechnique can monitor the evolution of the catalyst structure in real time,detect the reaction products online and promote the rational design of industrial catalysts.Firstly,this paper introduces the development history of catalytic reaction and dynamic in-site characterization technique,and then describes theOperando Raman technique in Fischer-Tropsch synthesis(FTS)and CO2 hydrogenation combining with recent research progress.The application of typical catalytic reactions demonstrate the structural evolution process and structure-performance relationship of the catalyst under different pretreatment and precursor conditions.However,the temporal resolution and spatial resolution of the current Operandtechnique still need to be further improved.In addition,the Operando technique still has vast development potential in solid-liquid and gas-liquid catalytic reactions.
Catalysts are the core of heterogeneous catalytic reactions.Due to the complexity of catalytic reactions,humans have very limited knowledge of the active phases of the catalysts.The structure-performance relationship of the catalyst during the reaction is important for understanding the catalytic reaction process and improving the catalyst.The Operandotechnique can monitor the evolution of the catalyst structure in real time,detect the reaction products online and promote the rational design of industrial catalysts.Firstly,this paper introduces the development history of catalytic reaction and dynamic in-site characterization technique,and then describes theOperando Raman technique in Fischer-Tropsch synthesis(FTS)and CO2 hydrogenation combining with recent research progress.The application of typical catalytic reactions demonstrate the structural evolution process and structure-performance relationship of the catalyst under different pretreatment and precursor conditions.However,the temporal resolution and spatial resolution of the current Operandtechnique still need to be further improved.In addition,the Operando technique still has vast development potential in solid-liquid and gas-liquid catalytic reactions.
引文
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[14]ZHANG Y,FU D,LIU X,et al.Operando spectroscopic study of dynamic structure of iron oxide catalysts during CO2 hydrogenation[J].ChemCatChem,2018,10(6):1272-1276.
[15]张玉龙,邵光印,张征湃,等.活化气氛对CO2加氢制取低碳烯烃Fe-K催化剂构-效关系[J].化工学报,2018,69(2):690-698.
[2]ROBERTS M W.Birth of the catalytic concept(1800-1900)[J].Catalysis Letters,2000,67(1):1-4.
[3]TOPS E H.Developments in operando studies and in situ characterization of heterogeneous catalysts[J].Journal of Catalysis,2003,216(1/2):155-164.
[4]BANARES M A.Operando methodology:combination of in situ spectroscopy and simultaneous activity measurements under catalytic reaction conditions[J].Catalysis today,2005,100(1/2):71-77.
[5]HAW J F,JENTOFT F.In-situ spectroscopy in heterogeneous catalysis[J].Angewandte Chemie,2003,115(3):266-267.
[6]WECKHUYSEN B M.Determining the active site in a catalytic process:Operando spectroscopy is more than a buzzword[J].Physical Chemistry Chemical Physics,2003,5(20):4351-4360.
[7]SCHLOGL R.Heterogeneous catalysis[J].Angewandte Chemie International Edition,2015,54(11):3465-3520.
[8]OKAWA T,ONISHI T,TAMARU K.Infrared and kinetic study of ammonia decomposition on supported iron catalysts:infrared observation of molecularly adsorbed N2in ammonia decomposition[J].Zeitschrift für Physikalische Chemie,1977,107(2):239-243.
[9]WECKHUYSEN B M.Snapshots of a working catalyst:possibilities and limitations of in situ spectroscopy in the field of heterogeneous catalysis[J].Chemical Communications,2002(2):97-110.
[10]FU D,DAI W,XU X,et al.Probing the structure evolution of iron-based Fischer-Tropsch to produce olefins by Operando Raman spectroscopy[J].ChemCatChem,2015,7(5):752-756.
[11]林冰婕,黄雨婷.中俄印温室气体排放的指标分解和电力需求展望[J].可持续发展,2017,7(1):59-69.
[12]PRIETO G.Carbon dioxide hydrogenation into higher hydrocarbons and oxygenates:thermodynamic and kinetic bounds and progress with heterogeneous and homogeneous catalysis[J].ChemSusChem,2017,10(6):1056-1070.
[13]MA H,YING W,FANG D.Study on methanol synthesis from coal-based syngas[J].Journal of Coal Science and Engineering(China),2009,15(1):98-103.
[14]ZHANG Y,FU D,LIU X,et al.Operando spectroscopic study of dynamic structure of iron oxide catalysts during CO2 hydrogenation[J].ChemCatChem,2018,10(6):1272-1276.
[15]张玉龙,邵光印,张征湃,等.活化气氛对CO2加氢制取低碳烯烃Fe-K催化剂构-效关系[J].化工学报,2018,69(2):690-698.
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