Pd-Cu/C催化二氧化碳加氢合成甲酸
发布时间：2023-04-17 04:29
大量温室气体二氧化碳(CO2)排放到大气中,引起全球变暖。因此捕集CO2并将其转化为各种燃料和化学物质成为了迫切需要。其中,二氧化碳加氢制甲酸备受关注,因为甲酸广泛应用于橡胶、食品、皮革、化肥、农业、制药和纺织工业等商业领域。同时,甲酸具有良好储氢能力。采用等体积浸渍法,以Cu为助剂,将Pd纳米颗粒负载在碳材料上。制备了不同金属比例(1:0,1:2,1:1,2:1,3:1,0:1)的Pd-Cu/C催化剂,并应用于CO2加氢催化甲酸。催化剂的形貌、晶粒尺寸、金属分散程度、晶体结构、还原性质、元素价态及含量等通过XRD、TEM、HAADF-STEM、EDS、TPR、XPS以及ICP等进行表征。Cu的加入形成了Pd-Cu合金,平均粒径仅为1.7 nm。通过Cu向Pd的电子转移提高了Pd的亲核性以及促进了氢气的解离和吸附能力,进而提高了CO2加氢合成甲酸的活性。对反应条件进行了优化,包括温度、压力以及反应溶剂。在一系列催化剂中,Pd2Cu1/C对CO2<...
【文章页数】：83 页
【学位级别】：硕士
【文章目录】：
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
本文编号：3792570
【文章页数】：83 页
【学位级别】：硕士
【文章目录】：
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
2.3.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
本文编号：3792570
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