大量溫室氣體二氧化碳(CO₂)排放到大氣中,引起全球變暖。因此捕集CO₂并將其轉(zhuǎn)化為各種燃料和化學(xué)物質(zhì)成為了迫切需要。其中,二氧化碳加氫制甲酸備受關(guān)注,因?yàn)榧姿釓V泛應(yīng)用于橡膠、食品、皮革、化肥、農(nóng)業(yè)、制藥和紡織工業(yè)等商業(yè)領(lǐng)域。同時(shí),甲酸具有良好儲(chǔ)氫能力。采用等體積浸漬法,以Cu為助劑,將Pd納米顆粒負(fù)載在碳材料上。制備了不同金屬比例(1:0,1:2,1:1,2:1,3:1,0:1)的Pd-Cu/C催化劑,并應(yīng)用于CO₂加氫催化甲酸。催化劑的形貌、晶粒尺寸、金屬分散程度、晶體結(jié)構(gòu)、還原性質(zhì)、元素價(jià)態(tài)及含量等通過(guò)XRD、TEM、HAADF-STEM、EDS、TPR、XPS以及ICP等進(jìn)行表征。Cu的加入形成了Pd-Cu合金,平均粒徑僅為1.7 nm。通過(guò)Cu向Pd的電子轉(zhuǎn)移提高了Pd的親核性以及促進(jìn)了氫氣的解離和吸附能力,進(jìn)而提高了CO₂加氫合成甲酸的活性。對(duì)反應(yīng)條件進(jìn)行了優(yōu)化,包括溫度、壓力以及反應(yīng)溶劑。在一系列催化劑中,Pd₂Cu₁/C對(duì)CO_2<...

【文章頁(yè)數(shù)】：83 頁(yè)

【學(xué)位級(jí)別】：碩士

【文章目錄】：
摘要
abstract
Symbols and Acronyms
Chapter One Introduction
    1.1.Research Background
    1.2.Research Motivation
    1.3.Research Objectives and Aims
    1.4.Methodology
Chapter Two Literature Review
    2.1.Introduction
    2.2.Physical and Chemical Properties of CO2

        2.2.1.Molecular structure of CO₂

        2.2.2.Molecular orbital and CO₂ activation
    2.3.CO₂ Utilization and Conversion
    2.4.Introduction to Formic Acid,Importance,Properties and Applications
    2.5.CO₂Hydrogenation to Formic Acid
        2.5.1.Different catalytic systems for hydrogenation of CO₂to formic acid
        2.5.2.Homogeneous catalysts for CO₂ hydrogenation to formic acid
        2.5.3.Homogeneous catalysts for CO₂ hydrogenation to formic acid
    2.6.Pd-Based Supported Heterogeneous Catalysts
    2.7.Presentation of Research Work
Chapter Three Experimental Section
    3.1.Chemical Reagents,Sources and Specifications
    3.2.Experimental Steps and Equipments
    3.3.Preparation of Pd-Cu/C Catalyst
    3.4.Characterizations of Catalyst
        3.4.1.X-ray diffraction analysis(XRD)
        3.4.2.X-ray photoelectron spectroscopy(XPS)
        3.4.3.Inductively coupled plasma optic emission spectrometer(ICP-OES)
        3.4.4.Transmission electron microscope (TEM) and energy-dispersive X-ray spectroscopy (EDS)
        3.4.5 .Hydrogen-temperature programmed reduction(H₂-TPR)
        3.4.6.High angle annular dark field with scanning transmission electron microscopy (HAADF-STEM)
    3.5.Experimental Product Analysis
    3.6.Calculations of Experimental Results
Chapter Four Prepration and Characterization of Pd-Cu/C Catalysts
    4.1.Introduction
    4.2.Effect of Different Metal Precursors and Reduction Methods
    4.3.Support Material
    4.4.Impact of Cu on Pd Particle Size in Pd-Cu/C Catalyst
    4.5.Characterization of Pd-Cu/C Catalysts
        4.5.1.X-ray diffraction analysis(XRD)analysis
        4.5.2.Inductively coupled plasma optic emission spectrometer(ICP-OES)analysis
        4.5.3.Temperature programmed reduction(TPR)analysis
        4.5.4.Transmission electron microscope(TEM) and high angle annular dark field with STEM (HAADF-STEM) analysis
        4.5.5.X-ray photoelectron spectroscopy(XPS)analysis
Chapter Five Catalytic Hydrogenation of CO2 to Formic Acid over Pd-Cu/C
    5.1.Evaluation of Reaction Temperature And Pressure
        5.1.1.Effect of temperature on catalytic activity
        5.1.2.Effect of pressure on catalytic activity
    5.2.Effect of Different Composed Pd-Cu/C Catalysts on Catalytic Activity
    5.3.Effect of Different Solvents on Catalytic Activity
Chapter Six Conclusions and Prospects
    6.1.Conclusions
    6.2.Innovations
    6.3.Prospects
References
Published Papers
Acknowledgements
Dedication



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