本文選題：鈣鈦礦太陽(yáng)能電池 + 薄膜��； 參考：《華僑大學(xué)》2017年博士論文

【摘要】：自2009年CH_3NH_3PbI_3作為太陽(yáng)能電池吸光材料被報(bào)道以來(lái),鈣鈦礦太陽(yáng)能電池已經(jīng)取得了飛快的進(jìn)步,理論探索和工藝制備獲得了長(zhǎng)足的發(fā)展。如何實(shí)現(xiàn)進(jìn)一步的跨越,加快鈣鈦礦太陽(yáng)能電池的產(chǎn)業(yè)化進(jìn)程,還有很多科學(xué)問(wèn)題需要解決,其中高質(zhì)量鈣鈦礦薄膜的制備工藝顯得尤為重要。針對(duì)目前存在的問(wèn)題,本論文開展鈣鈦礦薄膜晶體生長(zhǎng)、材料能級(jí)調(diào)控、薄膜結(jié)構(gòu)設(shè)計(jì)以及大面積器件開發(fā)等科學(xué)問(wèn)題的研究,通過(guò)材料制備、性能結(jié)構(gòu)表征、器件設(shè)計(jì)組裝、效能評(píng)價(jià)測(cè)試,研究薄膜制備優(yōu)化條件對(duì)器件光伏性能的影響,進(jìn)一步研究鈣鈦礦薄膜電子傳輸動(dòng)力學(xué)、界面匹配、能級(jí)匹配和結(jié)構(gòu)匹配等科學(xué)規(guī)律,獲得較好的進(jìn)展,主要研究?jī)?nèi)容和結(jié)果如下:(1)開發(fā)三步旋涂法制備優(yōu)質(zhì)鈣鈦礦薄膜。采用異丙醇溶劑處理PbI2液膜而非傳統(tǒng)的加熱退火處理,獲得了具有可控形貌和結(jié)晶度的巨石陣結(jié)構(gòu)PbI2薄膜,為CH_3NH_3I的滲透提供了足夠的通道和空間,保證了PbI2向鈣鈦礦的完全轉(zhuǎn)化,最高獲得了17.84%的光電轉(zhuǎn)換效率。(2)提出使用環(huán)境友好型醇類溶劑浴法制備高質(zhì)量鈣鈦礦薄膜,解決使用不良溶劑(乙醚、氯苯、甲苯等)帶來(lái)的毒性問(wèn)題。探索了不同類型溶劑浴中鈣鈦礦薄膜的生長(zhǎng)機(jī)理,研究溶劑浴成膜方式對(duì)器件光伏性能的影響,以及電子傳輸動(dòng)力學(xué)的作用機(jī)制。(3)通過(guò)控制鈣鈦礦前驅(qū)液中強(qiáng)配位劑二亞甲砜(DMSO)的含量,研究一步旋涂滴加反溶劑法制備鈣鈦礦薄膜的成膜機(jī)理,研究了中間配合物對(duì)于薄膜結(jié)晶及器件重現(xiàn)性的影響。調(diào)控二亞甲砜(DMSO)含量,拓寬滴加乙醚的工作窗口時(shí)間,獲得高質(zhì)量的鈣鈦礦薄膜。(4)研究雜化鈣鈦礦(CH_3NH_3PbI3-xBrx)薄膜的生長(zhǎng)機(jī)理,通過(guò)控制I-Br的摻雜比例,研究溴化甲胺(CH_3NH_3Br)對(duì)雜化鈣鈦礦薄膜晶體形貌的影響,研究了鈣鈦礦材料的能級(jí)結(jié)構(gòu)以及太陽(yáng)能電池中電子傳輸動(dòng)力學(xué)的微觀機(jī)理。由于Br的引入,拓寬了鈣鈦礦材料的能級(jí),提升了器件的開路電壓,提高TiO_2/鈣鈦礦層界面的電子提取能力。(5)基于功能梯度結(jié)構(gòu)設(shè)計(jì),將Spiro-OMeTAD空穴傳輸材料以梯度變化的形式分散于鈣鈦礦薄膜中。通過(guò)能量色散X射線光譜儀(EDX)和二次離子質(zhì)譜(SIMS)證實(shí)了梯度結(jié)構(gòu)的存在,研究載流子傳輸及復(fù)合動(dòng)力學(xué),分析梯度結(jié)構(gòu)的作用機(jī)理,最終獲得18.84%的光電轉(zhuǎn)換效率。(6)通過(guò)一步旋涂滴加反溶液法和正丁醇溶劑浴法制備大面積鈣鈦礦太陽(yáng)能電池,比較多種大面積鈣鈦礦太陽(yáng)能電池的光電性能,研究?jī)煞N制備方法在不同尺寸下的適用性。一步旋涂滴加反溶液法僅適用于制備小面積高效鈣鈦礦太陽(yáng)能電池;正丁醇溶劑浴法可以制備大面積高質(zhì)量鈣鈦礦薄膜,制備的10×10 cm2鈣鈦礦薄膜具有良好的“鏡面”效果。
[Abstract]:Since the report of Ch _ 3NH _ 3PbI _ 3 as solar cell absorbent material in 2009, the perovskite solar cell has made rapid progress, theoretical exploration and process preparation have made great progress. There are still many scientific problems to be solved in order to realize further leap and accelerate the industrialization of perovskite solar cells, among which the preparation process of high quality perovskite thin films is particularly important. In order to solve the existing problems, the research of perovskite thin film crystal growth, material energy level control, thin film structure design and large area device development has been carried out in this paper, through material preparation, performance structure characterization, device design and assembly, etc. The effects of the optimal preparation conditions on the photovoltaic properties of perovskite thin films are studied, and the scientific laws of electron transport dynamics, interface matching, energy level matching and structure matching of perovskite films are further studied. The main contents and results are as follows: (1) three-step spin coating method was developed to prepare high-quality perovskite films. PbI2 films with controllable morphology and crystallinity were obtained by using isopropanol solvent to treat PBI2 liquid film instead of traditional heating annealing treatment, which provided sufficient channel and space for CH3NHS3i permeation. The conversion of PBI2 to perovskite is guaranteed, and the highest photoelectricity conversion efficiency of 17.84% is obtained. (2) it is proposed to prepare high quality perovskite films by using environment-friendly alcohols solvent bath method to solve the problem of using bad solvents (ether, chlorobenzene, chlorobenzene). The toxicity of toluene etc. The growth mechanism of perovskite films in different kinds of solvent bath was studied. (3) by controlling the content of DMSO in perovskite precursor, the film-forming mechanism of perovskite thin films prepared by one-step spin coating and anti-solvent method was studied. The effects of the intermediate complexes on the crystallization of the films and the reproducibility of the devices were investigated. The high quality perovskite thin films were obtained by adjusting the content of DMSO and widening the working window time of dimethyl ether. (4) the growth mechanism of hybrid perovskite films was studied. By controlling the doping ratio of I-Br, the growth mechanism of hybrid perovskite films was studied. The effect of Ch _ 3CH _ 3BR on the crystal morphology of hybrid perovskite films was studied. The energy level structure of perovskite and the microscopic mechanism of electron transport kinetics in solar cells were studied. Because of the introduction of Br, the energy level of perovskite material is widened, the open circuit voltage of the device is raised, and the electronic extraction ability of TiO-2 / perovskite interface is improved. (5) based on the design of functionally gradient structure, Spiro-OMeTAD hole-transport materials were dispersed in perovskite films in the form of gradient changes. The existence of gradient structure was confirmed by energy dispersive X-ray spectrometer (edX) and secondary ion mass spectrometry (Sims). The carrier transport and recombination kinetics were studied, and the mechanism of gradient structure was analyzed. Finally, 18.84% photovoltaic conversion efficiency was obtained. (6) large area perovskite solar cells were prepared by one-step spin-drop adding inverse solution method and n-butanol solvent bath method, and the optoelectronic properties of many kinds of large area perovskite solar cells were compared. The applicability of the two preparation methods in different sizes was studied. The one-step spin-coating dripping and reverse solution method is only suitable for the preparation of small area high efficiency perovskite solar cells, and n-butanol solvent bath method can be used to prepare large area and high quality perovskite films, and the 10 脳 10 cm2 perovskite thin films have good "mirror" effect.
【學(xué)位授予單位】：華僑大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2017
【分類號(hào)】：TM914.4

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