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研究生:紀彥丞
研究生(外文):Ji, Yan-Cheng
論文名稱:研究錫摻雜對 CsPbI3鈣鈦礦量子點性能的影響
論文名稱(外文):Investigations of Sn-doped effects on the properties of CsPbI3 perovskite nanocrystals
指導教授:楊斯博
指導教授(外文):Yang, Zu-Po
口試委員:連峻儀蘇海清
口試委員(外文):Lien, Jiun-YiSu, Hai-Ching
口試日期:2023-06-17
學位類別:碩士
校院名稱:國立陽明交通大學
系所名稱:照明與能源光電研究所
學門:工程學門
學類:綜合工程學類
論文種類:學術論文
論文出版年:2023
畢業學年度:111
語文別:中文
論文頁數:78
中文關鍵詞:錫摻雜CsPbI3結構穩定性異價離子二維結構合金結構
外文關鍵詞:Tin dopingCsPbI3Structural stabilityHeterovalent ionsTwo-dimensional structureAlloy structure
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錫摻雜於CsPbI3已被許多研究實現,由於錫(Sn2+)的離子半徑小於鉛(Pb2+)的離子半徑,因此可以透過Sn2+來替換Pb2+使CsPbI3的晶格收縮,以提升其結構穩定性。就我們所知,至今還沒有研究使用SnI4作為摻雜劑提供Sn4+作為摻雜,由於Sn4+相比於Sn2+多了2個正電荷,此外Sn4+相對Sn2+更穩定,因此摻雜Sn4+可能對CsPbI3產生不同的影響。
本研究以熱注入合成法合成CsPbI3,並且在合成的過程中加入SnI2和SnI4作為摻雜劑,分別提供Sn2+與Sn4+對CsPbI3進行摻雜,探討Sn2+與Sn4+的摻雜分別會對CsPbI3造成甚麼影響。(1)當合成環境當中的碘為不守恆時,摻雜微量的Sn2+並不會使CsPbI3產生的結構變化,當摻雜Sn2+的比例持續提高時,CsPbI3會轉變為CsPb2I5之二維結構。除此之外,Sn4+與Sn2+具有相似的效果,只是Sn4+在相對Sn2+一半比例時就能使CsPbI3轉變為CsPb2I5之二維結構,這是因為電荷不平衡的關係使Sn4+比Sn2+能更有效的產生結構上的轉變。(2)當合成環境當中的碘為守恆時,與碘不守恆時的狀況不同,碘守恆的情況之下無法使CsPbI3轉變為二維結構,而是使CsPbI3轉變為CsSn1-xPbXI3之合金結構。
Tin (Sn2+) has been successfully doped into CsPbI3 reported in many studies. Due to the its smaller ionic radius than that of Pb2+, replacing Pb2+ with Sn2+ can cause lattice contraction and then enhance the structural stability of CsPbI3. To the best of our knowledge, there is no investigation about Sn4+-doped CsPbI3 by using SnI4 yet. Besides Sn4+-doped CsPbI3 may be more stable than Sn2+-doped CsPbI3, Sn4+-dopant might affect CsPbI3 differently from Sn2+-dopant because of heterovalent doping effect.
In this study, CsPbI3 nanocrystals were synthesized by hot-injection method. For the synthesis of Sn2+- and Sn4+-doped CsPbI3, the Sn2+ and Sn4+ dopant were provided by introducing the SnI2 and SnI4 during the synthesis process, respectively. The effects of Sn2+ and Sn4+ doping on CsPbI3 were investigated. (1) For the iodine non-conservation, doping small amounts of Sn2+ does not induce CsPbI3 structure changes. However, as the Sn2+ doping is over certain amount, CsPbI3 starts to transform into a two-dimensional (2D) CsPb2I5 structure. Sn4+ exhibits similar effects as Sn2+, but only the half amount of Sn2+ is required to trigger the 2D CsPb2I5 formation. This is attributed to the charge imbalance, which makes Sn4+ more effectively induce structure transformation than Sn2+. (2) For iodine conservation, unlike the non-conservative situation, there is no observation of 2D CsPb2I5 structures. Instead, an alloy CsSn1-xPbXI3 structure is obtained.
摘要 i
Abstract ii
目錄 iv
圖目錄 vi
表目錄 ix
第一章 緒論 1
1-1 鹵化物鈣鈦礦的歷史 1
1-2 鈣鈦礦量子點的簡介及應用 3
1-3 研究動機與目的 4
第二章 基本原理及文獻回顧 5
2-1 鈣鈦礦量子點的晶體結構 5
2-2 熱注入合成法 8
2-3 CsPbI3不穩定性的原因 10
2-3-1 結構的不穩定性 10
2-3-2 外部環境的影響 12
2-3-3 配體的動態結合 13
2-4 解決CsPbI3不穩定性的方法 14
2-4-1 離子摻雜 14
2-4-1-1 離子摻雜帶來的影響 14
2-4-1-1-1 提升結構的穩定性 14
2-4-1-1-2 降低鉛的含量 15
2-4-1-1-3 改變光電特性 15
2-4-1-2 不同金屬離子的摻雜 17
2-4-1-2-1 同價摻雜 17
2-4-1-2-2 異價摻雜 17
2-4-2 降低維度 18
2-4-3 外層保護 19
2-4-4 配體改良 20
第三章 實驗製程與設備 21
3-1 實驗材料 21
3-2 實驗設備 23
3-3 實驗製程 26
3-3-1 Cs-oleate前體溶液的合成 26
3-3-2 CsPbI3與錫摻雜的CsPbI3的合成 27
3-4 量測設備 31
第四章 結果與討論 36
4-1 錫濃度對於CsPbI3的影響 36
4-1-1 Sn2+摻雜CsPbI3 36
4-1-2 Sn4+摻雜CsPbI3 46
4-2 比較Sn2+與Sn4+摻雜對CsPbI3的影響 55
4-3 碘對於CsPbI3的影響 60
第五章 結論與未來展望 66
參考文獻 67
附錄一 XPS的原始數據與擬合數據 72
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