普魯士藍類似物製備的二硒化鈷/二硒化鐵奈米顆粒異質結構對鉀離子電池負極之應用

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研究生：	麥守善 Mai, Shou-Shan
論文名稱：	普魯士藍類似物製備的二硒化鈷/二硒化鐵奈米顆粒異質結構對鉀離子電池負極之應用 CoSe2/FeSe2 nanoparticle heterostructure prepared by Prussian blue analogs as electrode materials for Potassium-ion Battery anode
指導教授：	段興宇 Tuan, Hsing-Yu
口試委員:	呂明諺 Lu, Ming-Yen 曾院介 Tseng, Yuan-Chieh
學位類別：	碩士 Master
系所名稱：	工學院 - 化學工程學系 Department of Chemical Engineering
論文出版年：	2023
畢業學年度：	112
語文別：	英文
論文頁數：	86
中文關鍵詞：	普魯士藍類似物、異質結構、鉀離子電池、錯配物、劍峰、pn結、肖特基結
外文關鍵詞：	Prussian blue analogs, Potassium-ion Battery, heterostructure, misfit layered compound, Janus, p-n junction, Schottky junction
相關次數：	點閱：45 下載：0
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轉換型金屬硒化物電極在鉀離子電池（PIB）中的實際應用遇到了許多挑戰，例如顆粒聚集、穿梭效應和循環過程中的粉化。因此，我們設計了一種具有CoSe2-FeSe2/石墨/N摻雜碳（CFS//g@NC）的Janus異質結構，透過雙異質結（p-n和肖特基結）產生協同效應，增強界面電荷儲存並改善電極結構。當Janus異質結構用作PIB陽極時，它表現出高達10 A g−1的高倍率性能並能提供200 mA h g−1的容量，而在0.5 A g−1下表現出超過2500次循環的優異循環穩定性。根據密度泛函理論（DFT）計算，K離子在CFS//g@NC上的擴散勢壘比CoSe2或FeSe2上的擴散勢壘低兩倍。 Janus 粒子中 n 型和 p 型半導體的分佈已透過暗場電子顯微鏡的定量評估得到證實。除了跨越兩個半導體界面的 p-n 結外，普魯士藍類似物 (PBA) 衍生的石墨層與半導體之間的肖特基結也會產生內置電場，從而增強離子/電子傳輸並增加鉀的擴散離子。這項工作為多層異質介面的架構策略提供了新的見解，並為 PIB 中的陽極設計提供了一條有前景的新途徑。

The practical application of conversion-type metal selenide electrodes in potassium-ion batteries (PIBs) poses several challenges. These challenges include issues like particle aggregation, the shuttle effect, and pulverization during cycling. To address these challenges, we have developed a novel Janus heterostructure, referred to as CoSe2-FeSe2/graphite/N-doped carbon (CFS//g@NC). This Janus heterostructure incorporates dual heterojunctions, namely a p-n junction and a Schottky junction. These dual junctions work synergistically to enhance interface charge storage and bolster the structural integrity of the electrode. When utilized as the anode in PIBs, this Janus heterostructure demonstrates exceptional high-rate performance, supporting current densities of up to 10 A g−1. It boasts a high capacity of 200 mA h g−1 and exhibits outstanding cycling stability, with over 2500 cycles at a current density of 0.5 A g−1. Density functional theory (DFT) calculations reveal that the diffusion barrier for potassium ions on CFS//g@NC is only half that of CoSe2 or FeSe2. Additionally, quantitative analysis through dark-field electron microscopy confirms the distribution of n-type and p-type semiconductors within the Janus particles. Besides the p-n junction that spans two semiconductor interfaces, the Schottky junction formed between the graphite layer, derived from Prussian blue analogues (PBA), and the semiconductor, creates an inherent electric field. This field enhances ion and electron transport and facilitates the diffusion of potassium ions. This research offers valuable insights into the architectural strategy of multi-layer heterointerfaces, presenting a promising new direction for anode design in PIBs.

Table of contents
中文摘要............................................................................................................................. 1
Abstract .............................................................................................................................. 2
Table of contents ................................................................................................................ 3
List of Figure....................................................................................................................... 4
List of Table ....................................................................................................................... 7
Chapter 1. Introduction ...................................................................................................... 8
1.1    Challenges and development of potassium-ion batteries ............................................. 8
1.2 Concepts of prussian blue analogs (PBA). .................................................................... 9
1.3 Bimetallic heterostructure materials for batteries. ..................................................... 12
1.4 Transition metal selenide for potassium-ion batteries. ............................................... 15
Chapter 2. Experimental Section ...................................................................................... 16
2.1 Materials ..................................................................................................................... 16
2.2 Synthesis of Co/Fe-Prussian blue analogues (PBA). ................................................. 16
2.3 Synthesis of Co/Fe−PBA@PDA. ............................................................................... 16
2.4 Synthesis of CFS//g@NC. .......................................................................................... 17
2.5 Material characterization. ........................................................................................... 17
2.6 Electrochemical measurements. ................................................................................. 18
2.7 Mott-Schottky test ...................................................................................................... 18
2.8 DFT Calculation ......................................................................................................... 19
Chapter 3. Results and discussion for CFS//g@NC ......................................................... 20
3.1 Structure characterization. .......................................................................................... 20
3.2 Electrochemical tests and analysis. ............................................................................ 36
3.3 Energy band diagram, KPFM analysis and DFT calculations ................................... 47
3.4 Discussion. ................................................................................................................. 51
Chapter 4. Conclusion ...................................................................................................... 54
Chapter 5. Experimental section of FL-(BiSe)1.10NbSe2 ................................................... 55
5.1 Materials ..................................................................................................................... 55
5.2 Material Characterization............................................................................................ 55
5.3 Synthesis of bulk NbSe2, BiSe, (BiSe)1.10NbSe2 ........................................................ 56
5.4 Synthesis of few-layered (BiSe)1.10NbSe2. ................................................................. 56
5.5 Electrochemical measurement .................................................................................... 56
5.6 Finite element analysis simulation ............................................................................. 57
Chapter 6. Result and discussion of FL-(BiSe)1.10NbSe2 ................................................. 58
Chapter 7. Conclusion ...................................................................................................... 79
Reference .......................................................................................................................... 80

                                

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