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研究生： 阮停遵
Nguyen, Dinh-Tuan
論文名稱： 具可擴展性的2D材料合成法
Scalable Synthesis of 2D Materials
指導教授： 蘇彥勳
Su, Yen-Hsun
共同指導教授: 謝馬利歐
Mario, Hofmann
學位類別： 博士
Doctor
系所名稱： 工學院 - 材料科學及工程學系
Department of Materials Science and Engineering
論文出版年： 2021
畢業學年度： 109
語文別： 英文
論文頁數： 104
中文關鍵詞： graphene 、2D materials synthesis 、transition metal dichalcogenide 、CVD 、liquid-liquid interface
外文關鍵詞： graphene, 2D materials synthesis, transition metal dichalcogenide, CVD, liquid-liquid interface
相關次數： 點閱：60  下載：0 
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    • 2D materials have been at the forefront of the materials science in the last two decades, exhibiting extraordinary properties that can be game-changing in various areas of application. However, their adoption by industrial players have been slow, due to the lack of suitable synthesis techniques that can produce these materials in large quantity and high quality at competitive costs. This thesis describes efforts to improve several aspects of 2D materials synthesis with novel technical setups. For chemical vapor deposition – the leading method of 2D film fabrication, a solid diffusion-based pretreatment method is found to efficiently remove substrate impurities, leading to improved graphene film quality. Meanwhile, the introduction of additives into the process of high shear exfoliation substantially increases the yield of nanoflake production for non-graphene 2D materials. Finally, a new assembly technique involving dynamic liquid-liquid interface is invented to produce extremely strong membranes of 2D nanoflakes. Together, these studies represent a significant step towards mass production of 2D materials and unlocking their potentials.

    Abstract I Acknowledgements II Table of Contents III List of Tables VII List of Figures VIII Chapter 1: Introduction to Synthesis of 2D Materials 1 1.1 A brief history of 2D materials 1 1.2 Synthesis routes for 2D materials 3 1.2.1 Top-down synthesis 4 1.2.2 Bottom-up synthesis 7 1.3 Motivation and structure of this thesis 8 Chapter 2: Improving CVD Quality by Diffusion-induced Removal of Substrate Impurities 10 2.1 Background 10 2.2 Experimental methods 12 2.2.1 Materials and pretreatments 12 2.2.2 Annealing experiments 12 2.2.3 CVD growth and transfer 12 2.2.4 Characterization techniques 13 2.3 Results and Discussions 15 2.3.1 Limitations of conventional annealing 15 2.3.2 Capped annealing setup 16 2.3.3 Mechanism 17 2.3.4 Effect of the choice of cap material 20 2.3.5 Effect of capped annealing on graphene quality 21 Chapter 3: Additives-assisted Shear Exfoliation of 2D Materials 24 3.1 Background 24 3.2 Experimental Methods 27 3.2.1 Materials 27 3.2.2 Exfoliation 28 3.2.3 Centrifugation 28 3.2.4 Assembly and characterization techniques 29 3.3 Results and Discussions 31 3.3.1 Pilot tests 31 3.3.2 Characterization and quantifying the efficiency enhancement of AAE 34 3.3.3 Mechanism of AAE 41 3.3.4 Post-exfoliation removal of additive 43 3.3.5 On versatility of AAE 45 Chapter 4: Nanotetris: A Novel Way of Assembling 2D Materials in Edge-To-Edge Manner 49 4.1 Background 49 4.1.1 Mechanochemistry: Action under high pressure 49 4.1.2 Confinement and compression in interface assembly 50 4.1.3 Nanotetris: Dynamic compression and 2D confinement in tandem 51 4.2 Experimental Methods 52 4.2.1 X-ray photoelectron spectroscopy 53 4.2.2 Scanning Electron Microscopy and Transmission Electron Microscopy 53 4.2.3 Scanning Tunnel Microscopy and Scanning Tunnel Spectroscopy 54 4.2.4 White light interferometry 55 4.2.5 Dynamic light scattering 56 4.2.6 MD simulations 56 4.2.7 Force-displacement measurement 58 4.3 Results and Discussions 58 4.3.1 Edge-to-edge bonding under lateral pressure 58 4.3.2 Observation of membrane formation 59 4.3.3 Morphology and thickness 61 4.3.4 Evidence of bond formation 65 4.3.5 Extending nanotetris to other 2D materials and role of flake size 70 4.3.6 Mechanical, optical and electrical properties 72 4.3.7 Upscaling 76 4.3.8 Heterostructures 77 Chapter 5 Outlook 80 Appendixes 83 Appendix A: On universality of Nanotetris method 83 A.1 Choice of solvents 83 A.2 Choice of substrate materials and substrate treatment 85 Appendix B: On effects of experimental conditions and the question of upscaling 87 B.1 Inclined angle 87 B.2 Prewetting and adding tertiary liquid 87 B.3 Effects of temperature and ions and radicals 88 Appendix C: NMP draining and dry transfer 89 References 92

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