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Title: | 廢棄稻殼合成鋰離子電池矽-碳複合負極材料 SiOx/C Composite from Rice Husk and Its Application in Lithium-ion Batteries |
Authors: | Sheng-Siang Huang 黃聖翔 |
Advisor: | 吳乃立 |
Keyword: | 鋰離子電池,鋰硫電池,矽負極,稻殼,循環經濟, Lithium-ion batteries,Lithium-sulfur batteries,Silicon-based anodes,Rice husk,Recycling, |
Publication Year : | 2018 |
Degree: | 碩士 |
Abstract: | 現今工業發展的核心策略之一,即為回收廢棄物料再利用,創造高附加價值產物的製程開發。隨著人口成長以及經濟快速發展,未來數十年內,稻米的需求量勢必日益上揚。其中稻殼為稻穀收穫後所產生的廢棄副產物,然而回收稻殼的後續利用卻僅限於一些附加價值低的產業,像是灌溉用肥料、燃料及鋪路填充材料。近來,許多研究開發了以稻殼為原料的鋰離子電池負極材料,例如碳、奈米矽和碳-氧化矽複合材料。
根據食品與農業組織的報告,2017年越南的稻穀預估可收穫4330萬噸,而其稻殼產量估計為870萬噸,是相當豐裕的可再生能源。在此研究中,我們透過和越南的國合計畫,運用當地的稻殼資源,以相當簡易的程序製備出稻殼衍生複合材料。特別的是,由於其自然形成的奈米氧化矽結構和微孔碳基質,此複合材料在鋰離子電池電極的應用上,表現出穩定的充放電循環性能。 藉由煅燒參數的最佳化,在3%氫氣和氮氣的混合氣氛下,經過1000 °C,4小時還原煅燒而得的稻殼衍生氧化矽-碳複合物,是初步製程分析中具有相對優勢電化學性能的材料,在1010次充放電後,能保有87.9%的電容量維持率,並提供476.5 mAh g-1的可逆電容量。藉由導入外部矽源提升稻殼衍生複合物的矽含量,其電極之可逆電容量獲得了更進一步的改善,在720次充放電後,能夠保有568 mAh g-1之電容量以及75.7%電容量維持率。此外,我們更探索了此稻殼衍生複合電極的過鋰化能力,以及在不含LiNO3添加劑的醚基電解質中之穩定性。 再者,我們以電化學性能較佳的電極作為負極,應用於鋰硫電池,並進行分析。第一種類型的組件使用硫-碳正極和預鋰化的稻殼衍生複合負極,然而由於顯著的極化現象,與電池內部的交互作用,即便通過不同條件的測試,其電性表現始終不如預期。有趣的是,以預鋰化的稻殼衍生複合負極搭配硫-聚丙烯腈正極作為鋰硫電池,其能展現較佳的電化學性能。 總結而言,我們成功的轉化了越南碾米產業的廢料:稻殼,將其作為鋰離子電池負極材料,用於高附加價值之應用。稻殼衍生複合電極不僅具有穩定的可循環性,並且也在鋰硫電池的應用上展現出一定的潛力。 The important strategy for industrial processes is converting the recycled waste into high-value products. Despite the fact that rice demand is expected to remain strong in next few decades, the utilization of rice-generated waste by-products: rice husk (RH) has been limited to those with low added value, such as fertilizer additives, fuels, and paving materials. Studies have explored lithium-ion battery anode materials such as carbon, nanostructured Si and carbon/silicon oxide composites with RH as raw materials. In Vietnam, the rice paddy production is predicted to gather 43.3 million tons in 2017 according to a report by the Food and Agricultural Organization. The estimated RH production was about 8.7 million tons, which is an abundant renewable source. In this study, a facile method was developed to prepare RH-derived composite materials by using rice husk in Vietnam. Owing to their naturally formed silicon oxide nanoparticles and microporous carbon matrix, the RH-derived composite exhibited stable cycle performances as lithium-ion battery (LIB) anodes. With the optimization of calcination parameters, RH-derived material, RH_H2_4h, prepared by calcination of RH at 1000 °C for 4 h under 3%H2/N2, was found to exhibit the most promising electrochemical behavior. It offered a reversible capacity of 476.5 mAh g-1 after 1010 cycles with a retention of 87.9%. Reversible capacity was further improved by introducing Si-containing polymers. One of the modified electrodes delivered a corrected delithiation capacity of 568 mAh g-1 with a capacity retention of 75.7% after 720 cycles of full lithiation and delithiation. Interestingly, RH_H2_4h electrodes was discovered to obtain the ability to be overlithiated, and the stability in ether-based electrolyte without the LiNO3 additive. Further applications for Li-S batteries were characterized. The electrochemical performance of cells for the first kind of assembly including S/C cathodes and prelithiated RH_H2_4h anodes was analyzed under various conditions. However, due to large polarization and other interactions in the cell system, the capacity decay was obvious and reversible capacity was not high. Interestingly, as the second kind of assembly for Li-S cells, SPAN cathodes matched with prelithiated RH_H2_4h anodes could show an even better cycle performance. Our approach makes use of waste by-product from rice milling industry, rice husk, especially in Vietnam, by converting it into lithium-ion battery anode materials for high value-added applications. These anodes are demonstrated to have not only stable cyclability but also the potential for Li-S batteries after suitable adjustments. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/79077 |
DOI: | 10.6342/NTU201801395 |
Fulltext Rights: | 有償授權 |
metadata.dc.date.embargo-lift: | 2023-08-23 |
Appears in Collections: | 化學工程學系 |
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ntu-107-R05524023-1.pdf Restricted Access | 7.78 MB | Adobe PDF |
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