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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 陳嘉晉 | zh_TW |
dc.contributor.advisor | Chia-Chin Chen | en |
dc.contributor.author | 呂明彥 | zh_TW |
dc.contributor.author | Ming-Yen Lu | en |
dc.date.accessioned | 2024-02-26T16:28:21Z | - |
dc.date.available | 2024-02-27 | - |
dc.date.copyright | 2024-02-26 | - |
dc.date.issued | 2022 | - |
dc.date.submitted | 2002-01-01 | - |
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Solid State Ionics, 1999. 122(1): p. 41-49. 29. Kuhn, M., et al., Oxygen Nonstoichiometry and Defect Chemistry of Perovskite-Structured BaxSr1–xTi1–yFeyO3–y/2+δ Solid Solutions. Chemistry of Materials, 2013. 25(15): p. 2970-2975. 30. Yan, D., et al., NiCo2O4 with oxygen vacancies as better performance electrode material for supercapacitor. Chemical Engineering Journal, 2018. 334: p. 864-872. 31. Fleischmann, S., et al., Pseudocapacitance: From Fundamental Understanding to High Power Energy Storage Materials. Chemical Reviews, 2020. 120(14): p. 6738-6782. 32. Andreas, H.A., Self-Discharge in Electrochemical Capacitors: A Perspective Article. Journal of The Electrochemical Society, 2015. 162(5): p. A5047-A5053. 33. Isaacs, M.A., et al., Advanced XPS characterization: XPS-based multi-technique analyses for comprehensive understanding of functional materials. Materials Chemistry Frontiers, 2021. 5(22): p. 7931-7963. 34. 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Le, T.H., et al., In-situ growth of MnO 2 crystals under nanopore-constraint in carbon nanofibers and their electrochemical performance OPEN. Scientific Reports, 2016. 6. 39. Yang, Z., et al., Vertically-aligned Mn(OH)2 nanosheet films for flexible all-solid-state electrochemical supercapacitors. Journal of Materials Science: Materials in Electronics, 2017. 28(23): p. 17533-17540. 40. Sun, H., et al., Progress on X-ray Absorption Spectroscopy for the Characterization of Perovskite-Type Oxide Electrocatalysts. Energy & Fuels, 2021. 35(7): p. 5716-5737. 41. Gilbert, P., et al., Multiple Scattering Calculations of Bonding and X-ray Absorption Spectroscopy of Manganese Oxides. J. Phys. Chem. A, 2010. 107. 42. Tomar, A.K., et al., Zero-Dimensional Ordered Sr2CoMoO6-δ Double Perovskite as High-Rate Anion Intercalation Pseudocapacitance. ACS Applied Materials & Interfaces, 2020. 12(13): p. 15128-15137. 43. van der Haar, L.M., et al., Chemical Diffusion and Oxygen Surface Transfer of La[sub 1−x]Sr[sub x]CoO[sub 3−δ] Studied with Electrical Conductivity Relaxation. Journal of The Electrochemical Society, 2002. 149(3): p. J41. 44. Shu, Q., et al., Solid-state Reaction for Preparation of Lanthanum Manganite. High Temperature Materials and Processes, 2005. 24. 45. Wei, H. Conductivity behavior of LaNiO3- and LaMnO3- based thin film superlattices. 2016. 46. Cortés-Gil, R., et al., Evolution of magnetic behaviour in oxygen deficient LaMnO3−δ. Journal of Physics and Chemistry of Solids, 2006. 67(1): p. 579-582. 47. Shafi, P.M., et al., Enhanced electrochemical performances of agglomeration-free LaMnO3 perovskite nanoparticles and achieving high energy and power densities with symmetric supercapacitor design. Chemical Engineering Journal, 2018. 338: p. 147-156. 48. Yufeng, C., et al., Magnetic characteristics of LaMnO 3+δ thin films deposited by RF magnetron sputtering in an O 2 /Ar mixture gas. Materials Research Express, 2021. 8. 49. Kumar, V., et al., Electronic structure and electrical transport properties of LaCo1−xNixO3 (0 ≤ x ≤0.5). Journal of Applied Physics, 2013. 114(7): p. 073704. 50. Wang, J., et al., Realizing semiconductivity by a large bandgap tuning in Bi4Ti3O12 via inserting La1-xSrxMnO3 perovskite layers. Applied Physics Letters, 2017. 110(21): p. 212102. 51. Suntivich, J., et al., Estimating Hybridization of Transition Metal and Oxygen States in Perovskites from O K-edge X-ray Absorption Spectroscopy. The Journal of Physical Chemistry C, 2014. 118(4): p. 1856-1863. 52. Lim, D.K., et al., Electrochemical properties of LaMO3 (M=Co or Fe) as the negative electrode in a hydrogen battery. Journal of Physics and Chemistry of Solids, 2013. 74(1): p. 115-120. 53. 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Schober, T., et al., Effective hydrogen diffusivity in SrCe0.95Yb0.05O3 − α and SrZr0.95Yb0.05O3 − α. Solid State Ionics, 1995. 77: p. 175-179. 59. Skipworth, E., et al., Role of graphite in self-discharge of nickel(III) oxyhydroxide. Journal of Power Sources, 2007. 174(1): p. 186-190. 60. Conway, B. E. Electrochemical supercapacitors, 1999. | - |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/91923 | - |
dc.description.abstract | 鈣鈦礦氧化物為常見的擬電容材料(pseudocapacitor),在室溫下可展現高電容量,在充放電過程中,電極發生氧化還原反應,透過改變材料金屬價態儲存電荷。然而其儲存之電荷量遠超過材料表面可儲存之最大電容量,表明其電荷儲存不僅來自表面金屬價態改變,還需要涉及體相(bulk)金屬價態改變,即充放電過成中存在電荷嵌入機制(intercalation)。傳統上認為鈣鈦礦氧化物將氧離子作為電荷載子(charge carrier) [1],氧離子嵌入並透過晶格中的氧空缺位(oxygen vacancy)儲存電荷,因此提升電容的策略大多集中於提高氧空缺濃度。然而,理論上氧化物中的氧離子在室溫下不具備移動能力,因此嵌入機制可能是由其他電荷載子主導。 本研究旨在探討嵌入機制的電荷載子,以及缺陷濃度對電容的影響。以微米級LaMnO3作為研究模型,探討鈣鈦礦氧化物作為擬電容的儲能機制。微米級粉末有助於區別材料的表面以及體相區域的訊號差異,並且微米級粉末的低表面積有助於探討體相儲能的現象。電化學實驗結果顯示,電容值隨著充放電次數增加而增強,並且超越表面儲存量一個數量級,由縱深分析(depth profile)發現隨著充放電次數增加電荷有嵌入的現象,因其涉及體相的金屬價態改變,如此便說明了該類材料的高電容來源。X光光電子能譜(X-ray photoelectron spectroscopy, XPS)結果顯示充放電過程中表面生成氫氧鍵(M-OH),且X光吸收光譜(X-ray absorption spectroscopy, XAS)的結果說明氫氧鍵的生成伴隨錳價態的降低(Mn3+Mn2+)。綜觀以上結果,電荷載子並非如同文獻提及的氧離子,而是將氫離子作為電荷載子,在充放電過程中利用氫化反應與材料氧形成金屬-氫氧鍵儲存電荷。 不同於文獻中透過提高氧空缺濃度提升電容量,本研究發現Mn-OH濃度才是顯著影響電容表現的關鍵因素,對提升儲能能力提供一個新的方向。希望可以透過缺陷影響鈣鈦礦氧化物的儲電能力,獲得製備高性能材料的策略。 | zh_TW |
dc.description.abstract | Perovskite oxides exhibit high capacitance as pseudocapacitors at room temperature. During charging and discharging, redox reactions occur at the electrodes, and charges are stored by changing the metal valence state of the material. However, the amount of stored charge exceeds the capacitance of the material surface, indicating that its charge storage not only comes from the change of the valence state of the surface metal, but also needs to involve the change of the valence state of the bulk metal., that is, there is a charge intercalation mechanism in the charge-discharge process. Perovskite oxides have traditionally been thought to use oxygen ions as charge carriers [1] , which intercalate and store charges through oxygen vacancy in the lattice, so most strategies to improve capacitance focus on increasing the oxygen vacancy concentration. Theoretically, oxygen atoms in oxides are not mobile at room temperature, as the result, the intercalation mechanism may be dominated by other charge carriers. This study aims to investigate the charge intercalation mechanism, and the effect of defect concentration on capacitance. Using micron-sized LaMnO3 as model material to explore the energy storage mechanism of perovskite oxides as pseudocapacitors. The micron-sized powder helps to distinguish the signal difference between the surface of the material and the bulk region, and the low surface base of the micron-sized powder helps to explore the phenomenon of energy storage in the bulk. Electrochemical experimental results show that the capacitance value increases with the number of charge and discharge, and exceeds the surface storage by an order of magnitude. From the depth profile, it was found that with the increase of the number of charge and discharge, there is a phenomenon of charge intercalation, because it involves the change of the metal valence state of the bulk, which explains the high capacitance of this type of material. The results of X-ray photoelectron spectroscopy (XPS) show that the hydrogen-oxygen bond (M-OH) is generated on the surface during the charging and discharging process, and X-ray absorption spectroscopy (XAS) indicates that the formation of hydrogen-oxygen bond is accompanied by the decrease of manganese valence (Mn3+Mn2+). Looking at the above results, the charge carriers are not oxygen as mentioned in the literature, but hydrogen ions are used as charge carriers, and the hydrogenation reaction is used to form a metal-hydrogen bond with the material during the charge and discharge process to store the charge. Unlike the literature in which the capacitance is improved by increasing the oxygen vacancy concentration, this study found that the Mn-OH concentration is the key factor that significantly affects the capacitance performance, providing a new direction for improving the energy storage capacity. It is hoped to adjust defects concentration to improve storage capacity of perovskite oxides, and obtained a strategy for preparing high-performance materials. | en |
dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2024-02-26T16:28:21Z No. of bitstreams: 0 | en |
dc.description.provenance | Made available in DSpace on 2024-02-26T16:28:21Z (GMT). No. of bitstreams: 0 | en |
dc.description.tableofcontents | 中文摘要 II Abstract III 目錄 V 圖目錄 VII 第一章 序論 1 1.1 鈣鈦礦氧化物 1 1.2 電容 2 1.2 擬電容 3 1.3 缺陷化學 6 1.4 電化學量測方法 8 1.4.1 二極式與三極式電解槽 8 1.4.2 電化學電容量測 9 1.6 XPS技術應用 13 1.7 XAS技術應用 15 1.8 實驗動機與目的 18 第二章 實驗儀器與步驟 19 2.1 LaMnO3粉末合成 19 2.2 粉末鑑定 19 2.3 電極製備 19 2.4 電化學測試 20 2.5 X光光電子能譜分析 20 2.6 X光吸收光譜分析 20 第三章 結果與討論 21 3.1 LaMnO3粉末鑑定 21 3.2 LaMnO3擬電容 23 3.3 表面分析 25 3.4 縱深分析 35 3.5 自放電現象 43 3.6 電位影響 44 3.7 儲能機制探討 48 第四章 結論與建議 52 4.1 結論 52 參考文獻 53 附錄一 58 | - |
dc.language.iso | zh_TW | - |
dc.title | LaMnO3作為擬電容應用之電荷存儲特性 | zh_TW |
dc.title | Charge storage in LaMnO3 for pseudocapacitor applications | en |
dc.type | Thesis | - |
dc.date.schoolyear | 110-2 | - |
dc.description.degree | 碩士 | - |
dc.contributor.oralexamcommittee | 吳乃立;方冠榮;周宏隆 | zh_TW |
dc.contributor.oralexamcommittee | Nae-Lih Wu;Kuan-Zong Fung;Hung-Lung Chou | en |
dc.subject.keyword | 鈣鈦礦氧化物,擬電容,電荷載子,嵌入機制, | zh_TW |
dc.subject.keyword | perovskite oxides,pseudocapacitor,charge carrier,intercalation mechanism, | en |
dc.relation.page | 61 | - |
dc.identifier.doi | 10.6342/NTU202204130 | - |
dc.rights.note | 同意授權(限校園內公開) | - |
dc.date.accepted | 2022-09-28 | - |
dc.contributor.author-college | 工學院 | - |
dc.contributor.author-dept | 化學工程學系 | - |
顯示於系所單位: | 化學工程學系 |
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