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研究生： 鍾德華
Chung, De-Hua
論文名稱： 聲波振動對火焰合成奈米碳結構的影響
Acoustic Modulation on Flame Synthesis of Carbon Nano-Materials
指導教授： 林大惠
Lin, Ta-Hui
學位類別： 博士
Doctor
系所名稱： 工學院 - 機械工程學系
Department of Mechanical Engineering
論文出版年： 2012
畢業學年度： 100
語文別： 英文
論文頁數： 114
中文關鍵詞： 燃燒合成 、自然擺盪頻率 、聲波共振頻率 、乙烯噴流火焰 、奈米碳管 、奈米碳球
外文關鍵詞： Flame synthesis, Natural flickering frequency, Acoustically resonant frequency, Ethylene jet diffusion flame, Carbon nanotubes, Carbon nano-onions
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    • 本研究使用聲波振動乙烯噴流擴散火焰，進行燃燒合成奈米碳結構。並用冷流場模擬氣體濃度與軸向速度分佈，以探討適合奈米碳結構的可能原因。
    火焰型態方面，平均流速20 cm/s之乙烯噴流火焰，在振動功率P = 15 W，振動頻率f = 0 ~ 80 Hz的情況下，可以在f = 10 ~ 20 Hz及60 ~ 70 Hz的兩個區間內觀察到雙層火焰的結構。低頻振動(f = 10 ~ 20 Hz)之頻率接近自然擺盪頻率，浮力與流場耦合產生共振現象，火焰形成雙層結構。聲波共振(f = 60 ~ 70 Hz)則是在振動頻率66 Hz下，燃燒管(fuel line)中傳遞的聲波以燃燒管兩端為節點，產生半波共振模態，火焰亦為雙層的結構。然而雙層火焰結構在暫態影像拍攝的時候可發現，其為火焰徑向的直徑變化，經過視覺暫留的觀察所產生，火焰薄層仍然只有一層。
    暫態火焰的變化中，火焰型狀有梭型、錐形與蕈狀。高溫熱傳使折射率改變，可取得外部渦漩輪廓之Schlieren影像，並藉此判斷渦漩方向與冷流場模擬匹配。冷流場之模擬等值線的變化，與暫態火焰與Schiliren影像之趨勢接近，可觀察燃燒器出口處的流場變化。
    於z = 5與10 mm位置取樣，在f = 10 ~ 80 Hz中奈米碳結構皆為葡萄狀堆積的奈米碳球。其中f = 10 與66 Hz取樣之奈米碳球較f = 0 Hz數量皆高出數個量級，其他頻率的奈米碳球則比兩種共振頻率較少，但比f = 0 Hz的產量較多。若減少乙烯氣體之濃度，則奈米碳球之數量也隨之減少，甚至在乙烯濃度20%，f = 10 Hz的產物轉變為奈米碳管。

    Acoustically modulated ethylene jet diffusion flame was used in the synthesis of carbon nano-materials. The cold-flow axial velocity and gas concentration were simulated to search the suitable condition of synthesizing.
    The flame types were observed in an ethylene jet flow with mean velocity of 20 cm/s and acoustic frequency (f) of 0 ~ 80 Hz. Double-layer flame was formed at f = 10 ~ 20 Hz and 60 ~ 70 Hz because of resonance near the natural flickering frequency and acoustically resonant frequency, respectively. The former was caused by the flame/buoyancy coupling, while the latter was caused by the acoustics/fuel line coupling. However, the double–layer flame was only a single-layer flame, which was formed by the persistence of vision with quick change of flame diameter.
    There were shuttle-, cone- and mushroom-like flames observed in the instantaneous flames. The Schlieren images of vortices would be caught due to the change of refractive index, which was resulted in with heat transfer. The sequence of Schlieren images were determined by vortex growth in the cold flow simulation. The isopleths (cold flow simulation) of axial velocity and ethylene concentration matched respectively the vortical motions and Schiliren images in the flow field. It can help to analyze the suitable condition for flame synthesis.
    The carbon nano-onions (CNOs) were mainly deposited grape-likely on the Ni substrate. The amount of CNOs at f = 10 and 66 Hz were both formed much more those formed at f = 0 Hz (z = 5 and 10 mm). At the other frequency (f = 30 ~ 50 and 80 Hz), the amount of CNOs were less those at two resonant regions (f = 10 and 66 Hz), but more than those without acoustic modulation (f = 0 Hz). CNOs would be decreased with the decreasing of ethylene concentration, even carbon nanotubes (CNTs) would replace CNOs to be the main product at ethylene concentration 20% and f = 10 Hz.

    CONTENTS I LIST OF FIGURES V NOMENCLATURE IX 1. INTRODUCTION 1 1.1 Applications and Synthesis of Carbon Materials 1 1.2 Flame Synthesis of Carbon Nano-Materials 2 1.2.1 Fuel-Rich Premixed Flames 3 1.2.2 Diffusion Flames 5 1.2.3 Flame Synthesis of Metal Nano-Materials 9 1.2.4 Mechanisms of CNT and CNO Synthesis 9 1.3 Acoustic Modulation in Diffusion Flames 11 1.4 Objectives 12 2. EXPERIMENTS 14 2.1 Burner System 14 2.1.1 Gas Supply System 14 2.1.2 Acoustic Modulation System 14 2.1.3 Fuel Line 15 2.2 Measurement and Sampling Systems 15 2.2.1 Camera and Image Tools 15 2.2.2 Temperature Measurement System 16 2.2.3 Hot-Wire Anemometry 16 2.2.4 Sampling System 17 2.3 Nano-Analytic Instruments 17 2.3.1 Field Emission Scanning Electron Microscopy 18 2.3.2 Transmission Electron Microscopy 18 2.3.3 Raman Spectrophotometer 19 2.4 Experimental Methods and Steps 21 2.4.1 Flame Types and Stability 21 2.4.2 Gas Temperature Measurement 21 2.4.3 Axial Velocity of Cold Flow without Acoustic Modulation 22 2.4.4 Axial Velocity of Cold Flow with Acoustic Modulation 22 2.4.5 Carbon Nano-Material Sampling and Analyzing 22 3. SIMULATION METHODS AND MODELS 24 3.1 Physical Model and Assumptions 24 3.2 Governing Equations 24 3.3 Boundary Conditions 25 3.4 Mesh Creation and Simulation Solver 26 3.4.1 ANSYS Fluent 26 3.4.2 Discretization Methods 26 3.5 Simulation Tactics for Acoustic Modulation 27 3.5.1 Cold Flow without Acoustic Modulation 27 3.5.2 Cold Flow with Acoustic Modulation 27 4. VELOCITY FIELD OF FREE JET WITHOUT AND WITH ACOUSTIC MODULATION 29 4.1 Axial Velocity without Acoustic Modulation 29 4.2 Experimental Measurement of Axial Velocity at 66 Hz 30 4.3 Numerical Simulation of Axial Velocity at 10 and 66 Hz 31 5. ACOUSTIC MODULATION AND NITROGEN DILUTION EFFECT ON JET DIFFUSION FLAMES 34 5.1 Jet Diffusion Flames with Acoustic Modulation 34 5.1.1 Flame Types and Stability 34 5.1.2 Flame Height and Gas Temperature Measurements 36 5.2 Nitrogen Dilution Effect in Jet Diffusion Flames with Acoustic Modulation 37 5.2.1 Flame Types and Stability 38 5.2.2 Flame Height and Gas Temperature Measurements 43 6. FLAME STRUCTURES, SCHILIREN IMAGES AND COLD FLOW SIMULATIONS 45 6.1 Flame Structures and Schiliren Images 45 6.1.1 For 10 Hz 45 6.1.2 For 66 Hz 46 6.2 Cold Flow Simulations 47 6.2.1 For 10 Hz 47 6.2.2 For 66 Hz 49 7. ANALYSIS ON CARBON NANO-MATERIALS 52 7.1 Carbon Nano-Materials Synthesized by Jet Diffusion Flames with Acoustic Modulation 52 7.1.1 At z = 5 mm 52 7.1.2 At z = 10 mm 54 7.2 Carbon Nano-Materials Synthesized by N2-Diluted Jet Diffusion Flames with Acoustic Modulation 57 8. CONCLUSIONS 60 9. REFERENCES 63 10. FIGURES 74 11. PUBLICATION LIST 113

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