| 摘要: | 鈣鈦礦太陽能電池由多層光電材料組成，其中電洞傳輸層協助電子與電洞拆解並擔任電洞傳遞的角色，在元件中佔有舉足輕重的地位。如何開發出價格低廉，電洞遷移率高的新型電洞傳輸材料(hole-transporting material, HTM)，一直是許多研究團隊努力的目標。
縱觀電洞傳輸材料的製備方法，歷來皆以傳統人名反應為主要合成途徑，往往有合成步驟多、純化困難、需要使用高毒性有機金屬試劑等缺點。因此在本次研究中，我們提出以鈀金屬催化劑進行的直接碳氫鍵芳香環化反應，並以此種合成途徑製備一系列以并三噻吩(dithieno[3,2-b:2’,3’-d]thiophene, DTT)為核心結構的線型電洞傳輸材料。
首先我們藉由更換不同種類的配位基、反應溶劑，對直接碳氫鍵芳香環化反應進行合成條件最佳化的篩選，並以最佳化條件製備TTh101和CHC03-07。在分子設計上，我們改變電洞傳輸材料的末端基團並引入3,4-乙烯二氧噻吩(3,4-ethylenedioxythiophene, EDOT)於共軛體系中，系統性的探討分子結構與光電化學性質間的關係，以及實際應用在鈣鈦礦太陽能電池上的表現。
;Among the composition of the perovskite solar cells (PSCs) device, hole transporting layer plays a significant role in exciton dissociation and hole migration. How to design a novel hole-transporting material (HTM) with high hole mobility and competitiveness in price has been the main issue that many research groups concerned.
Recently, various novel HTMs have been prepared by Stille and Suzuki–Miyaura cross-coupling reactions. However, these traditional synthesis routes have some common disadvantages, such as tedious synthetic steps, purification difficulties, and use of toxic organometallic reagents. Herein, a step-economical strategy for palladium-catalyzed direct C-H arylation of two arenes has been provided. Meanwhile, a series of dithienothiophene-incorporated linear HTMs, consisting of a dithieno[3,2-b:2’,3’-d]thiophene (DTT)-core and arylamine moieties has been synthesized via one-step direct C-H arylation and practically applied to the PSCs device.
In this research, we screened the different kinds of ligands and reaction solvents to optimize the reaction conditions of the direct C-H arylation, then to synthesize TTh101 and CHC03-07 by the optimized conditions. Based on the concept of the molecular design, we systematically investigated the relationship between the molecular structure and the photovoltaic characteristics by changing the functional groups and introducing 3,4-ethylenedioxythiophene (EDOT) moiety to the conjugated backbone of the HTMs. |
