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研究生:曾兆綦
研究生(外文):Tseng, Chao-Chi
論文名稱:以碳氫化合物熱裂解法製備碳包覆奈米高熵合金顆粒
論文名稱(外文):Carbon encapsulation of high-entropy alloy nanoparticles by catalytic pyrolysis of hydrocarbons
指導教授:徐文光徐文光引用關係
指導教授(外文):Hsu, Wen-Kuang
口試委員:連德軒薛森鴻呂昇益朱永祺
口試委員(外文):Lien, Der-HsienSyue, Sen-HongLu, Sheng-YiChu, Yung-Chi
口試日期:2021-12-10
學位類別:博士
校院名稱:國立清華大學
系所名稱:材料科學工程學系
學門:工程學門
學類:材料工程學類
論文種類:學術論文
論文出版年:2021
畢業學年度:110
語文別:英文
論文頁數:82
中文關鍵詞:奈米碳管高熵合金奈米顆粒碳氫化合物熱裂解法
外文關鍵詞:carbon nanotubeshigh-entropy alloy nanoparticlescatalytic pyrolysis
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由於具有獨特的性質和應用科技開發潛力,高熵合金已成為材料界極感興趣的研究目標。高熵合金是由四個以上的主要元素,以等莫爾比方式組成,因此本質上,它們的構型熵大於單一元素組成的合金。不過,在低維度時不僅表面能會增加,且會出現類似原子成簇的傾向,而使製造奈米顆粒變得極為困難。此論文中展示如何以簡單的製程於奈米碳管中合成出高熵合金奈米顆粒。電子顯微鏡和元素分析的結果皆證實被碳層所包覆的奈米顆粒為固溶相,且有些部分被碳化物環繞,組成成分元素為四元至五元的多域結構。多域結構和非磁性中心所產生的硬化現象,會顯著提高室溫下的矯頑磁場。較高的飽和磁場是源於合金化的過程會使電子重新分布到較高的能階。被碳層所包覆的高熵合金奈米顆粒其構型熵落在與塊材高熵合金相似的範圍中。

第一章 介紹奈米碳管和高熵合金的背景,包括碳管的結構、高熵合金的定義以及兩個主題分別的合成方法。

第二章 說明本論文使用的實驗設定和儀器介紹。

第三章 透過電子顯微鏡和成分分析證明本論文的方法可以製備出的高熵合金奈米顆粒,同時其磁性質和多域的現象也將在此章節中被討論。

第四章 總結以上實驗結果。
Owing to their unique properties and technological potential, high entropy alloys (HEAs) have become the subject of great interest in the materials science community. HEAs consist of more than four principle elements in equimolar ratio so their configurational entropy is intrinsically greater than one principle element based. The increasing surface energy and chemical tendency toward clustering of like atoms at low dimension, however, make production of HEA-nanoparticles (HEA-NPs) extremely difficult. A facile production of HEA-NPs inside carbon nanotubes and nanoparticles is demonstrated in this work. Electron microscopic and elemental analyses confirm encapsulated to be solution phase; some embrace carbides and form multidomains with chemical composition ranging from quaternary to quinary phase. Multidomains and nonmagnetic centers create hardening thus promoting coercivity significantly at room temperature. Alloying induces electron redistribution into high spin states, accounting for observed high saturation. Configurational entropy of encapsulated HEA-NPs lies on a range comparable with bulk.

Chapter 1 introduces the background of carbon nanotubes (CNTs) and HEAs, including the structure of CNTs, definition of HEAs and the synthetic method of both structures.

Chapter 2 describes the experimental setups and characterization techniques employed in this thesis.

Chapter 3 discusses results, including electron microscopic and elemental analyses. Analyses further reveal that encapsulated NPs consist of multidomains thus creating a significant coercivity (Hc) ever reached by existing soft magnetic materials at room temperature (T). A high saturation (Ms) due to alloying induced electron redistribution is also observed.

Chapter 4 concludes the experimental results.
Contents
Abstract I
摘要 III
致謝 IV
Contents V
Figure Captions VII
Tabel lists XII


Chapter 1 Introduction & Literature Review 1
1-1 Carbon nanotubes 1
1-1-1 Structure of carbon nanotubes 1
1-1-2 Synthesis of carbon nanotubes 4
1-1-3 Synthesis of Fe-filled carbon nanotubes 8
1-2 High entropy alloys (HEAs) 10
1-2-1 Definition of high-entropy alloy 11
1-2-2 Four Core Effects of HEAs 11
1-2-3 The fabrication processes of high-entropy alloys 20
1-2-4 The fabrication processes of HEA-NPs 26
1-3 Density Functional Theory and virtual-crystal approximation 33
Chapter 2 Experimental Section 35
2-1 Drugs and Kits 35
2-2 Characterization Instruments 36
Chapter 3. Carbon Encapsulation of High Entropy Alloy Nanoparticles with Extraordinary Coercivity and Saturation at Room Temperature 40
3-1 Introduction 40
3-2 Synthesis of HEA-NPs inside Graphitic Shells 40
3-3 Characteristic Analysis 41
3-4 Coexistence of multiple structure in individual NPs 51
3-5 Configurational entropy of encapsulated HEA-NPs 64
3-6 Magnetic property of encapsulated HEA-NPs 65
Chapter 4. Conclusions 70
References 71
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