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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 鄧茂華 | zh_TW |
| dc.contributor.advisor | Mao-Hua Teng | en |
| dc.contributor.author | 楊智淵 | zh_TW |
| dc.contributor.author | Chih Yuan Yang | en |
| dc.date.accessioned | 2024-06-17T16:07:04Z | - |
| dc.date.available | 2024-06-18 | - |
| dc.date.copyright | 2024-06-17 | - |
| dc.date.issued | 2024 | - |
| dc.date.submitted | 2024-03-30 | - |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/92729 | - |
| dc.description.abstract | 石墨包裹矽奈米顆粒(Graphite Encapsulated Silicon nanoparticles, GES)是一種內核為矽或碳化矽晶粒、外殼為非晶質碳或是石墨層之奈米複合材料。GES具有作為鋰離子電池陽極的潛力，內核矽或碳化矽之儲電量約為常見石墨電極的3至10倍，但電池充放電過程中，鋰離子會與矽結成Li15Si4合金，造成體積膨脹3至4倍，而石墨外殼具有良好導電性與延展性，在增加導電度的同時，也能有效限縮矽材料因充放電所造成的體積膨脹，延長電池使用壽命。
本團隊於2020年成功以改良式鎢電弧法合成GES，然而產物中碳化矽比例過高，由於碳化矽之儲電量僅為矽的三分之一倍，會造成GES的儲電量下降；另外，過去製程產量過低，導致難以進行後續量化分析與實務應用之研究。因此，本研究目的在於減少GES產物中的碳化矽比例與試圖提高產量。 從碳-矽二元相圖與文獻回顧發現，控制系統碳含量能有效限制碳化矽的生成，透過比較反應式的自由能高低發現，若系統中含有氧則能降低碳之比例，因此加入一定比例的石英粉末於經過改良之坩堝配置中，於電弧中心提供氧原子，以限制碳化矽的生成反應，並且也能作為矽的來源。根據實驗產物之XRD分析結果，產物中的碳化矽繞射峰強度有明顯下降，顯示石英粉末能有效限制碳化矽生成；透過HRTEM影像分析得知GES的核心為矽單晶或單晶碳化矽，並統計影像中矽核心GES與碳化矽核心GES之數量比為2:1，相對於前人研究之1:9，石英粉末能大幅減少產物中碳化矽比例。此外，透過本研究之製程改良能有效提升GES產量約10倍以上，解決前人產量不足的問題。最後綜合實驗結果提出GES的生成機制模型，說明系統在不同碳含量下，GES可能的生成路徑與結構，且能針對前人研究無法解釋的部分給予合理的解釋。 | zh_TW |
| dc.description.abstract | Graphite Encapsulated Silicon nanoparticles (GES) are core-shell nanocomposite materials with a silicon (Si) or silicon carbide (SiC) core and an outer shell of amorphous carbon or graphite. GES has the potential to be used as the anode material for lithium-ion batteries. The electrical capacity of the Si or SiC core in GES is approximately 3 to 10 times higher than that of conventional graphite electrodes. However, during the charging/discharging process, lithium ions react with silicon to form Li15Si4 alloy, resulting in a 3 to 4 times volume expansion. The graphite shell exhibits excellent electrical conductivity and ductility, which not only increases the electrode’s conductivity but also effectively restricts the volume expansion of the Si core during charging/discharging, thereby extending the battery’s lifespan.
In 2020, our group successfully synthesized GES by modified tungsten arc- discharge method. Nevertheless, the product contained a high proportion of SiC, which caused a decreased electrical capacity since the electrical capacity of SiC is only one-third of the electrical capacity compared to Si. Additionally, the low production rate in the past made it difficult to do subsequent quantitative analysis and research on practical applications. Therefore, the purpose of this study is to reduce the proportion of SiC in the GES product and attempt to increase the production rate. Based on the carbon-silicon binary phase diagram and literature reviews, it was found that controlling the carbon content in the system can effectively limit the formation of SiC. By comparing with the Gibbs free energy of the reactions, it was observed that the presence of oxygen in the system can decrease the proportion of carbon. Consequently, by adding a certain proportion of quartz powder to the improved crucible setup, which provides oxygen atoms at the center of the arc limits the formation of SiC and also serves as a silicon source. XRD analysis of the experimental products showed a significant decrease in the intensity of the SiC diffraction peak, indicating that the quartz powder can effectively limit the formation of SiC. HRTEM images revealed that the core of GES consists of single crystal Si or single crystal SiC. Quantitative analysis of the TEM images showed a ratio of 2:1 between GES with Si core and GES with SiC core, which is in comparison to the 1:9 in the previous study. It indicated that quartz powder can significantly reduce the proportion of SiC in the product. In addition, the process improvement in this study increased the production rate of GES by more than about 10-fold, which resolved the problem of low production rate in previous study. Finally, based on the experimental results, we proposed a model to explain the formation mechanism of GES. This model describes the possible formation pathways and structures of GES, providing reasonable explanations for some aspects that couldn’t be explained in previous study. | en |
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| dc.description.provenance | Made available in DSpace on 2024-06-17T16:07:04Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 致謝 i
中文摘要 ii Abstract iii 目次 v 圖目次 viii 表目次 xii 第一章 緒論 1 1.1 研究動機與目的 1 1.2 研究方法 3 1.3 章節內容 3 第二章 文獻回顧 5 2.1 奈米材料 5 2.1.1 奈米材料之特殊效應 6 2.1.2 奈米材料的合成 9 2.2 石墨包裹金屬奈米晶粒(GEM) 12 2.2.1 石墨包裹奈米顆粒之發展史 13 2.2.2 改良式鎢電弧法(Modified Tungsten Arc-Discharge Method) 15 2.2.3 石墨包裹奈米顆粒之合成機制 17 2.3 本團隊在石墨包裹金屬奈米晶粒之研究發展 21 2.3.1 機械設計 22 2.3.2 產物後處理 23 2.3.3 產物熱處理 23 2.3.4 坩堝設計改良 24 2.3.5 碳源選擇 25 2.4 石墨包裹矽奈米晶粒(GES) 26 2.4.1 其他學者對於石墨包裹矽奈米晶粒之研究 26 2.4.2 本團隊於石墨包裹矽奈米晶粒之研究發展 29 2.4.3 碳熱還原法(Carbonthermic Reduction Method) 32 第三章 實驗方法與流程 33 3.1 實驗相關設備 33 3.1.1 真空電弧蒸發裝置 33 3.1.2 電弧系統 34 3.1.3 冷卻系統 35 3.1.4 電源供應系統 36 3.2 實驗流程 37 3.2.1 實驗原料來源 37 3.2.2 實驗配置 38 3.2.3 產物的收集與分散 40 3.3 分析儀器 40 3.3.1 X光粉末繞射儀(X-ray powder diffractometer, XRD) 41 3.3.2 高分辨解析率穿透式電子顯微鏡(High resolution transmission electron microscopy, HRTEM) 43 3.3.3 掃描式電子顯微鏡(Scanning electron microscope, SEM) 44 3.3.4 熱重分析儀(Thermogravimetric analysis, TGA) 46 第四章 結果與討論 47 4.1 抑制碳化矽的生成 47 4.1.1 系統中的碳含量 48 4.1.2 碳熱還原法(Carbonthermic reduction method)的啟發 49 4.1.3 自由能數據與石英粉末假說 49 4.2 實驗設計改良與初步結果討論 52 4.2.1 碳源選擇與固態原料晶相分析 53 4.2.2 坩堝內配置與初步結果 56 4.3 儀器分析結果 75 4.3.1 XRD晶相分析 75 4.3.2 電子顯微鏡影像分析 77 4.3.3 GES的熱重分析(Thermogravimetric analysis, TGA) 92 4.4 GES的機制模型 97 4.4.1 GES可能的生成路徑 97 4.4.2 GES生成路徑模型與前人研究之探討 99 第五章 結論與未來建議 101 5.1 結論 101 5.2 未來建議 102 參考文獻 103 附錄A 110 | - |
| dc.language.iso | zh_TW | - |
| dc.title | 以石英粉末輔助合成石墨包裹矽奈米顆粒之初步研究 | zh_TW |
| dc.title | Preliminary Study on the Synthesis of Graphite Encapsulated Silicon Nanoparticles with Quartz Powder | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 112-2 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 謝文斌;李尚實;陳卉君 | zh_TW |
| dc.contributor.oralexamcommittee | Wen-Pin Hsieh;Shang-Shih Li ;Hui-Chun Chen | en |
| dc.subject.keyword | 核-殼結構,碳化矽,石英粉末,物理氣相沉積,鋰離子電池, | zh_TW |
| dc.subject.keyword | core-shell structure,silicon carbide,quartz powder,PVD,lithium-ion battery, | en |
| dc.relation.page | 111 | - |
| dc.identifier.doi | 10.6342/NTU202304216 | - |
| dc.rights.note | 同意授權(全球公開) | - |
| dc.date.accepted | 2024-03-30 | - |
| dc.contributor.author-college | 理學院 | - |
| dc.contributor.author-dept | 地質科學系 | - |
| 顯示於系所單位： | 地質科學系 | |
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