多酸促進(jìn)無機(jī)—有機(jī)雜化鈣鈦礦光電轉(zhuǎn)換性能及光伏器件
發(fā)布時(shí)間：2019-02-25 13:17
【摘要】：近期,以新一代光敏材料——鈣鈦礦型無機(jī)有機(jī)雜化鉛鹵化物為代表的一系列光電轉(zhuǎn)換材料引起科研工作者們的廣泛關(guān)注。提高鈣鈦礦材料以及基于鈣鈦礦材料的光電器件光伏性能是一個(gè)重要的研究課題。多金屬氧酸鹽(多酸),擁有許多優(yōu)異的理化性質(zhì),最重要的是多酸是一類優(yōu)秀的電子接收材料,令其能夠加速光生電子-空穴的分離,提高光電轉(zhuǎn)換效率。本文將多酸引入至鈣鈦礦材料以及鈣鈦礦光伏器件體系中,旨在提高它們的光電性能,具體工作如下:1.我們將多酸引入到鈣鈦礦材料前驅(qū)體溶液中,在室溫及常規(guī)條件下,利用經(jīng)典的“一步成膜法”制備成平面型光電導(dǎo)和光檢測器件。光電導(dǎo)測試結(jié)果表明,多酸/鈣鈦礦復(fù)合物的光電流是單純鈣鈦礦的三倍。單色光檢測結(jié)果表明,由于多酸的引入使得鈣鈦礦對365 nm單色光的靈敏度由0.646A·W-1提高到1.175 A·W-1,對420 nm單色光的靈敏度由0.224 A·W-1提高到0.621 A·W-1。光電導(dǎo)性能和光檢測性的提高表明,在鈣鈦礦內(nèi)部光生載流子的分離-復(fù)合競爭過程中,多酸的引入促進(jìn)了載流子的分離并加快其遷移,因而充分地削弱了光生電子-空穴的再結(jié)合現(xiàn)象。2.基于全印刷無空穴傳輸層鈣鈦礦太陽能電池模型,我們將多酸(PW12)引入到(5-AVA)x(MA)1-xPbI3鈣鈦礦材料中來提高太陽能電池的光伏性能。經(jīng)過多酸分子摻雜,鈣鈦礦電池的平均效率從9.17%提升至11.35%,提高程度為24%。在考察鈣鈦礦成核生長過程中,我們發(fā)現(xiàn)了多酸可以誘導(dǎo)奧斯瓦爾德熟化作用的發(fā)生——鈣鈦礦小晶粒相互融合生長成大尺寸的鈣鈦礦多晶膜,晶粒尺寸由5μm生長至30μm。生長后的大尺寸晶粒薄膜的缺陷態(tài)密度大幅度減小,促進(jìn)了載流子的傳輸。正因?yàn)檫@種顯著的形貌調(diào)控機(jī)制,使這類全印刷鈣鈦礦太陽能電池器件的光電性能顯著改善。3.我們制備了以多酸/TiO_2為致密層的全印刷無空穴傳輸層鈣鈦礦太陽能電池。利用多酸可以捕捉光生電子、抑制載流子復(fù)合并促進(jìn)其遷移的能力有效地提高了電池的光電轉(zhuǎn)換效率,由9.42%提升至10.65%,提高幅度約為13%。另外,通過電化學(xué)阻抗分析,我們認(rèn)為適量的多酸可以有效地促進(jìn)電子轉(zhuǎn)移,形成電子淺陷阱,而過量的多酸反而會促進(jìn)電子-空穴的復(fù)合,形成電子深陷阱。4.我們利用靜電吸附原理巧妙地使呈負(fù)電性的多酸和表面呈正電性的氧化亞銅納米晶復(fù)合。光電測試結(jié)果表明,與單純Cu2O相比,PW10Mo2/Cu2O復(fù)合物膜電極的光電流響應(yīng)提高了179%,另外,復(fù)合物膜電極的光電轉(zhuǎn)換效率提高了125%。提高的原因是多酸在復(fù)合物中起到了電子淺陷阱的作用,抑制光激發(fā)的電子-空穴再結(jié)合,加速了電子的遷移。
[Abstract]:Recently, a series of photoelectric conversion materials, represented by perovskite-type inorganic organic hybrid lead halide, have attracted wide attention of researchers. It is an important research topic to improve the photovoltaic performance of perovskite materials and photovoltaic devices based on perovskite materials. Polyoxometalates (polyoxometalates) have many excellent physical and chemical properties. The most important is that polyacids are a kind of excellent electron receiving materials, which can accelerate the separation of photogenerated electrons and holes and improve the efficiency of photoelectric conversion. In this paper, polyacids are introduced into perovskite materials and perovskite photovoltaic device systems in order to improve their photoelectric properties. The specific work is as follows: 1. In this paper, we introduce polyacid into perovskite precursor solution. At room temperature and under conventional conditions, a planar photoconductive and optical detector is prepared by the classical "one-step film forming method". The photoconductivity test results show that the photocurrent of polyacid / perovskite composite is three times higher than that of perovskite alone. The results of monochromatic light detection showed that the sensitivity of perovskite to the 1.175 nm monochromatic light was increased from 0.646 A W-1 to 1.175 AW-1 due to the introduction of polyacid. Sensitivity to 420 nm monochromatic light increased from 0.224 A W / 1 to 0.621 A W / 1. The improvement of photoconductivity and photodetection shows that the introduction of polyacids promotes the separation and migration of carriers in perovskite during the process of separation and composite competition of photogenerated carriers. Therefore, the recombination of photogenerated electrons and holes is fully weakened. 2. Based on the all-print hole-free transport layer perovskite solar cell model, we introduce polyacid (PW12) into (5-AVA) x (MA) 1-xPbI3) perovskite material to improve the photovoltaic performance of solar cells. The average efficiency of perovskite battery was increased from 9.17% to 11.35%, and the increase was 24%. During the investigation of perovskite nucleation and growth, we found that polyacid can induce Oswald ripening, in which perovskite grains fuse and grow into large perovskite polycrystalline films, and the grain size increases from 5 渭 m to 30 渭 m. The density of defect states of the grown large-size grain films decreases greatly, which promotes carrier transport. The photoelectric properties of these all-printed perovskite solar cell devices have been greatly improved because of this remarkable morphology regulation mechanism. We prepared fully printed hole-free perovskite solar cells with polyacid / TiO_2 as dense layer. Using polyacid can capture photogenerated electrons, inhibit carrier recombination and promote its migration. The photoelectric conversion efficiency of the battery is improved from 9.42% to 10.65%, and the increase is about 13%. In addition, by electrochemical impedance analysis, we think that proper amount of polyacid can effectively promote electron transfer and form electron shallow trap, while excessive polyacid can promote electron hole recombination and form electron deep trap. 4. We use the principle of electrostatic adsorption to skillfully combine the negatively charged polyacids and the surface positively charged cuprous oxide nanocrystals. The photocurrent response of PW10Mo2/Cu2O composite membrane electrode was increased by 179% compared with that of pure Cu2O, and the photoelectric conversion efficiency of the composite membrane electrode was increased by 125%. The reason for the increase is that polyacids act as electron shallow traps in the complex, inhibit photoinduced electron-hole rebinding, and accelerate electron migration.
【學(xué)位授予單位】：東北師范大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2017
【分類號】：TB34
本文編號：2430216
[Abstract]:Recently, a series of photoelectric conversion materials, represented by perovskite-type inorganic organic hybrid lead halide, have attracted wide attention of researchers. It is an important research topic to improve the photovoltaic performance of perovskite materials and photovoltaic devices based on perovskite materials. Polyoxometalates (polyoxometalates) have many excellent physical and chemical properties. The most important is that polyacids are a kind of excellent electron receiving materials, which can accelerate the separation of photogenerated electrons and holes and improve the efficiency of photoelectric conversion. In this paper, polyacids are introduced into perovskite materials and perovskite photovoltaic device systems in order to improve their photoelectric properties. The specific work is as follows: 1. In this paper, we introduce polyacid into perovskite precursor solution. At room temperature and under conventional conditions, a planar photoconductive and optical detector is prepared by the classical "one-step film forming method". The photoconductivity test results show that the photocurrent of polyacid / perovskite composite is three times higher than that of perovskite alone. The results of monochromatic light detection showed that the sensitivity of perovskite to the 1.175 nm monochromatic light was increased from 0.646 A W-1 to 1.175 AW-1 due to the introduction of polyacid. Sensitivity to 420 nm monochromatic light increased from 0.224 A W / 1 to 0.621 A W / 1. The improvement of photoconductivity and photodetection shows that the introduction of polyacids promotes the separation and migration of carriers in perovskite during the process of separation and composite competition of photogenerated carriers. Therefore, the recombination of photogenerated electrons and holes is fully weakened. 2. Based on the all-print hole-free transport layer perovskite solar cell model, we introduce polyacid (PW12) into (5-AVA) x (MA) 1-xPbI3) perovskite material to improve the photovoltaic performance of solar cells. The average efficiency of perovskite battery was increased from 9.17% to 11.35%, and the increase was 24%. During the investigation of perovskite nucleation and growth, we found that polyacid can induce Oswald ripening, in which perovskite grains fuse and grow into large perovskite polycrystalline films, and the grain size increases from 5 渭 m to 30 渭 m. The density of defect states of the grown large-size grain films decreases greatly, which promotes carrier transport. The photoelectric properties of these all-printed perovskite solar cell devices have been greatly improved because of this remarkable morphology regulation mechanism. We prepared fully printed hole-free perovskite solar cells with polyacid / TiO_2 as dense layer. Using polyacid can capture photogenerated electrons, inhibit carrier recombination and promote its migration. The photoelectric conversion efficiency of the battery is improved from 9.42% to 10.65%, and the increase is about 13%. In addition, by electrochemical impedance analysis, we think that proper amount of polyacid can effectively promote electron transfer and form electron shallow trap, while excessive polyacid can promote electron hole recombination and form electron deep trap. 4. We use the principle of electrostatic adsorption to skillfully combine the negatively charged polyacids and the surface positively charged cuprous oxide nanocrystals. The photocurrent response of PW10Mo2/Cu2O composite membrane electrode was increased by 179% compared with that of pure Cu2O, and the photoelectric conversion efficiency of the composite membrane electrode was increased by 125%. The reason for the increase is that polyacids act as electron shallow traps in the complex, inhibit photoinduced electron-hole rebinding, and accelerate electron migration.
【學(xué)位授予單位】：東北師范大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2017
【分類號】：TB34
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