磷鉬酸-有機金屬骨架-RGO衍生之氧化銅氧化鉬複合材作為鋰(鈉)離子電池負極材料之應用

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题名:	磷鉬酸-有機金屬骨架-RGO衍生之氧化銅氧化鉬複合材作為鋰(鈉)離子電池負極材料之應用
作者:	吳佳儒;Wu, Chia-Ju
贡献者:	化學學系
关键词:	鋰電池;有機金屬骨架材料;還原氧化石墨烯;li-ion battery;Metal organic framework;Reduced graphene oxide
日期:	2025-07-28
上传时间:	2025-10-17 11:23:48 (UTC+8)
出版者:	國立中央大學
摘要:	本論文旨在開發具高電容量及優異穩定性之金屬氧化物-碳複合材料，應用於鋰離子與鈉離子電池負極材料。實驗以醋酸銅與磷鉬酸作為金屬離子前驅物，1,3,5-苯三甲酸（BTC）作為有機配體，並添加L-麩氨酸限制晶體成長，合成多酸-有機金屬骨架前驅物POM@Cu-BTC。此前驅物經於600 °C、氮氣環境下煅燒後，轉化為含銅及二氧化鉬的碳基複合材料Cu@MoO2-C。進一步透過熱氧化處理調控材料中銅的氧化態，並獲得CuO@MoO2-C-X系列材料。研究結果顯示，在250 °C條件下進行氧化處理可避免材料形成新的副產物且具有最佳的CuO、MoO2、碳材共存比例，進而提升其在電池測試中的比電容量表現。為進一步改善材料導電性與結構穩定性，本研究於合成POM@Cu-BTC過程中引入不同添加比例的親水性處理還原氧化石墨烯(HRGO)，製備CuO@MoO₂-HRGO(Y)複合材料。在鋰離子半電池測試中，CuO@MoO₂-HRGO(5)於0.1 A g-1電流密度下循環70圈後，仍可維持769.1 mAh g-1的高比電容量。在鈉離子全電池測試中，該材料於0.05 A g-1下展現124.9 mAh g-1的容量表現；與磷酸鋰鐵正極組成的全電池於17 mA g-1條件下測得154.9 mAh g-1的放電容量與84.11%的庫倫效率，展現其於新興能源儲存裝置中的應用潛力。;This study aims to develop metal oxide–carbon composite materials with high specific capacity and excellent stability. Copper acetate and phosphomolybdic acid were used as metal ion precursors, while 1,3,5-benzenetricarboxylic acid serve as an organic ligand. L-glutamic acid was introduced as an additive material while synthesizing the polyoxometalate–metal–organic framework precursor, POM@Cu-BTC. Upon calcination at 600 °C under a nitrogen atmosphere, this precursor was transformed into a material containing copper, molybdenum dioxide and carbon (Cu@MoO2-C). Subsequent thermal oxidation treatment was employed to modulate the oxidation state of copper, resulting in a series of CuO@MoO2-C-X materials. Among them, the sample oxidized at 250 °C exhibited the optimal phase composition of CuO, MoO2 and carbon without the formation of undesirable byproducts, thereby delivering the best electrochemical performance. To further enhance the conductivity and structural stability of the material, reduced graphene oxide with hydrophilic treated (HRGO) was introduced in varying amounts during the synthesis of POM@Cu-BTC, yielding CuO@MoO₂-HRGO(Y) composites. In lithium-ion half-cell test, CuO@MoO2-HRGO(5) demonstrated a high specific capacity of 769.1 mAh g-1 after 70 cycles at a current density of 0.1 A g-1. In sodium-ion half-cell test, the material achieved 124.9 mAh g-1 at 0.05 A g-1. When combined with an LiFePO4 cathode in a full-cell configuration, the device delivered a discharge capacity of 154.9 mAh g-1 and a Coulombic efficiency of 84.11% at a current density of 17 mA g-1. These results underscore the promising potential of the synthesized materials for energy storage applications.
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