合成用於鈣鈦礦太陽能電池載子傳遞 及界面修飾材料的D-A type有機分子

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题名:	合成用於鈣鈦礦太陽能電池載子傳遞及界面修飾材料的D-A type有機分子
作者:	吳姿儀;Wu, Tzu-Yi
贡献者:	化學學系
关键词:	鈣鈦礦太陽能電池;載子傳遞材料;界面修飾材料;D-A type有機分子
日期:	2022-09-26
上传时间:	2022-10-04 11:01:31 (UTC+8)
出版者:	國立中央大學
摘要:	鈣鈦礦太陽能電池(Perovskite Solar Cells, PSCs)中，鈣鈦礦吸光層受光激發的激子要能夠順利被分開並各別傳遞至兩側電極才有機會流至外線路轉換成電能，因此載子傳輸材料與界面修飾材料在元件中扮演關鍵角色之一。近年來有機分子材料由於具有高的載子遷移率及可調整的前置軌域能階，極具運用在PSCs載子傳輸層及界面修飾層上的潛力。本研究以具有高平面性、高熱穩定性的IDT (indacenodithieno[3,2-b]-thiophene)骨架做為Donor單元，透過高平面性及剛性結構使分子間排列緊密，搭配帶有兩個強拉電子基的ITN-CN (benzo[c]thiophene-5,6-dicarbonitrile)做為Acceptor單元，一方面利用氰基的拉電子能力拉低化合物的前置軌域能階，另一方面透過路易斯鹼的氰基來修飾鈣鈦礦層缺陷，合成出小分子BT-IDT以及共聚物PBT-IDT。另外，在Donor單元的側鏈上引入電負度大的氟原子，降低共聚物前置軌域能階並增強分子間作用力，合成出共聚物PBT-F-IDT。小分子BT-IDT、共聚物PBT-IDT及共聚物PBT-F-IDT的熱裂解溫度分別為382℃、252℃及254℃，水接觸角皆大於90o；三個化合物的UV-Vis吸收光譜顯示小分子BT-IDT的邊界吸收(onset)落在約636 nm，而兩個共聚物PBT-IDT及PBT-F-IDT的onset延伸至835~855 nm。將小分子BT-IDT做為鈣鈦礦層/電洞傳遞層間的界面修飾層所組裝之一般式PSCs的光電轉換效率(Power conversion efficiency, PCE)可達22.10%(相對於無添加BT-IDT的20.50%)；將兩共聚物PBT-IDT與PBT-F-IDT做為電洞傳遞層(hole transport layer, HTL)組裝成一般式PSCs的PCE值分別為10.40%及5.16%；將兩共聚物做為電子傳遞層(electron transport layer, ETL)組裝成反式PSCs的PCE值分別是5.19%及2.74%，其中以PBT-IDT為ETL所組裝之元件的效率(5.19%)高於無ETL所組裝之元件的效率(3.33%)，表示PBT-IDT是有傳遞電子的能力。兩個共聚物中PBT-IDT做為HTL及ETL分別組裝之元件的效率皆優於PBT-F-IDT的原因之一為PBT-IDT的成膜性較佳，因此有較多的載子可以順利傳遞到電極。;In Perovskite Solar Cells (PSCs), the sunlight excited excitons must be successfully separated and transferred to the cathod and anode then to the external circuit to convert solar energy into electrity. Therefore, charge transport layers and interfacial layers play important roles in PSCs. Organic chemicals have great potential to be the PSC’s charge transport matreials due to their excellent carrier mobility and adjustable front orbital energy level. In this study, IDT (Indacenodithieno[3,2-b]-thiophene) derivatives with planarity and high thermal stability are used as donor units, and their planarity can stack tighly. ITN-CN (benzo[c]thio-phene-5,6-dicarbonitrile) is used as acceptor unit, two strong electron-withdrawing cyano groups on ITN-CN not only lower the front orbital energy level of the compound but also passivate perovskite layer by its Lewis basic nature. D-A small molecule as well as BT-IDT and PBT-IDT copolymers were designed and prepared in this study. Then insert fluorine atoms on the donor unit to lower the front orbital energy level and stronger the intermolecular interaction to form copolymer PBT-F-IDT. The decomposition temperatures of BT-IDT、PBT-IDT, and PBT-F-IDT are 382℃、252℃ ,and 254℃, respectively. UV-Vis absorption spectra show that the λonset of BT-IDT is about 636 nm and those of copolymer PBT-IDT and PBT-F-IDT extend to 835~855 nm. The power conversion efficiency (PCE) of regular PSCs based on BT-IDT as Perovskite/HTL interlayer is 22.10% (the PCE of PSC without BT-IDT layer is 20.50%). The PCE of regular PSCs devices based on PBT-IDT and PBT-F-IDT as HTLs are 10.40% and 5.16%, respectively. The PCE of inverted PSCs devices based on the two copolymers ETLs are 5.19% and 2.74%. Moreover the efficiency of inverted PSCs devices based on PBT-IDT as ETL is better than the deviced without ETL (3.33%). This means PBT-IDT has the ability to transport electrons.
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