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The electron transport layer is an important functional layer of perovskite solar cells, and its surface and internal defects are critical parts of limiting the performance improvement of perovskite solar cells. The double electron transport layer (double ETL) strategy can effectively passivate inherent defects in the electron transport layer (such as SnO2) and improve electron extraction and transport between the functional layers, providing an effective way for developing efficient and stable PSCs. However, due to the existence of independent interfaces in the dual ETL, the cell mismatch in different ETL materials also leads to additional carrier defects, hindering the continuous advancement of the dual ETL strategy. This work proposes a strategy for introducing di[2-((oxo)diphenylphosphino)phenyl]ether (DPEPO) into SnO2 ETL to design a hybrid electron transport layer strategy. Using the hole-blocking effect of DPEPO, which has a higher HOMO energy level and good ability to transfer electrons, the intrinsic defects in SnO2 are successfully passivated, while significantly improving the crystalline quality of the SnO2 film surface. So, avoiding the direct contact between the perovskite photoactive layer and the conductive substrate can effectively improve the extraction and transport of electrons. Due to the preparation of high-quality electron transport layer, the crystallization regulation of perovskite thin film is further achieved, thereby improving the performance of perovskite solar cells. Finally, 21.53% of the power conversion rate is obtained, the open-circuit voltage (VOC) reaches 1.220 V, the short-circuit current (JSC) is 23.19 mA/cm2, and the fill factor (FF) is 76.11%. This efficiency is 1.39% higher than that of the control one. It is shown that the hybrid electron transport layer strategy can not only optimize the carrier transport dynamics efficiently and reduce the device performance affected by the defects in the functional layer significantly, but also regulate the perovskite crystallization, which has the prospect for preparing high-performance solar cells.
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Keywords:
- perovskite /
- solar cell /
- electron transport layer /
- carrier composite /
- defect passivation
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图 1 本文采用的电池结构示意图
Figure 1. Schematic diagram of the solar cell structure used in this work.
图 2 (a)基于SnO2 ETL的SEM图像; (b)基于SnO2:DPEPO ETL的SEM图像; (c)经过以及未经过DPEPO处理的SnO2 ETL薄膜的XPS光谱, Sn-3d信号; (d)经过以及未经过DPEPO处理的SnO2 ETL薄膜的XPS光谱, O-1s信号; (e) SnO2和SnO2:DPEPO作为ETL的器件的电导率数据; (f) SnO2和SnO2:DPEPO ETL薄膜的紫外-可见光透过光谱
Figure 2. (a) SEM image of SnO2 electron transport layer; (b) SEM image of SnO2:DPEPO electron transport layer; (c) XPS spectra of SnO2 ETL films with and without DPEPO treatment, Sn-3d signal; (d) XPS spectra of SnO2 ETL films with and without DPEPO treatment, O-1s signal; (e) conductivity data for devices with SnO2 and SnO2:DPEPO as ETLS; (f) the ultraviolet-visible (UV-Vis) transmittance spectra of SnO2 and SnO2:DPEPO as ETLS.
图 3 (a)基于SnO2 ETL的CsFAMA钙钛矿SEM表面俯视图像; (b)基于在SnO2: DPEPO双ETL的CsFAMA钙钛矿SEM表面俯视图像; (c)基于SnO2和SnO2:DPEPO ETL的CsFAMA钙钛矿薄膜XRD图谱
Figure 3. (a) Top view SEM image of CsFAMA perovskite surface deposited on SnO2 ETL; (b) top view image SEM of CsFAMA perovskite surface deposited on SnO2:DPEPO ETL; (c) XRD images of CsFAMA perovskite films prepared on SnO2 and SnO2:DPEPO ETLs.
图 4 (a)纯钙钛矿薄膜以及基于SnO2/CsFAMA以及SnO2:DPEPO/CsFAMA的PL光谱; (b)基于SnO2以及SnO2:DPEPO ETL纯电子器件对数J-V特性曲线; (c)基于SnO2以及SnO2:DPEPO ETL结构器件暗J-V分析对数曲线; (d)基于SnO2以及SnO2:DPEPO ETL结构器件在1 kHz频率下的莫特-肖特基分析
Figure 4. (a) Steady-state PL measurements of pure perovskite thin films and SnO2/CsFAMA and SnO2:DPEPO/CsFAMA; (b) logarithmic J-V characteristic curves of SnO2 and SnO2:DPEPO purely electronic devices; (c) dark J-V analysis of SnO2 and SnO2:DPEPO ETL structured devices; (d) Mott-Schottky analysis of SnO2-based and SnO2:DPEPO ETL structured devices at 1 kHz frequency.
图 5 (a) 基于SnO2和SnO2:DPEPO作为ETL PSCs的J-V曲线; (b) 基于SnO2和SnO2:DPEPO作为ETL PSCs的IPCE曲线; (c) 基于SnO2和SnO2:DPEPO作为ETL PSCs的环境空气中稳定性测试
Figure 5. (a) J-V curves of PSCs based on SnO2 and SnO2:DPEPO as ETL; (b) IPCE curves based on SnO2 and SnO2:DPEPO as ETL; (c) stability test in ambient air based on SnO2 and SnO2:DPEPO as ETL PSCs.
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[1] Kojima A, Teshima K, Shirai Y, Miyasaka T 2009 J. Am. Chem. Soc 131 6050
Google Scholar
[2] Liang Z, Zhang Y, Xu H F, Chen W J, Liu B Y, Zhang J Y, Zhang H, Wang Z H, Kang D H, Zeng J R, Gao X Y, Wang Q S, Hu H J, Zhou H M, Cai X B, Tian X Y, Reiss P, Xu B M, Kirchartz T, Xiao Z G, Dai S Y, Park N G, Ye J J, Pan X 2023 Nature 624 557
Google Scholar
[3] Deng K M, Chen Q H, Li L 2020 Adv. Funct. Mater. 30 2004209
Google Scholar
[4] Lv J C, Li H X, Chen H Y, Ke L L, Du W J, Xiong J, Zhou C H, Liu G 2023 Appl. Phys. Lett. 122 233501
Google Scholar
[5] Dahal B, Guo R, Pathak R, Rezaee M D, Elam J W, Mane A U, Li W J 2023 J. Phys. Chem. Solids 181 111532
Google Scholar
[6] Bai C, Dong W, Cai H Y, Zu C P, Yue W, Li H X, Zhao J, Huang F Z, Cheng Y B, Zhong J 2023 Adv. Energy Mater. 13 2300491
Google Scholar
[7] Khan U, Iqbal T, Khan M, Wu R 2021 Sol. Energy 223 346
Google Scholar
[8] Gan Y J, Qiu G X, Qin B Y, Bi X G, Liu Y C, Nie G C, Ning W L, Yang R Z 2023 Nanomaterials 13 1313
Google Scholar
[9] Zhang Y H, Xu L, Sun J, Wu Y J, Kan Z T, Zhang H, Yang L, Liu B, Dong B, Bai X, Song H W 2022 Adv. Energy Mater. 12 2201269
Google Scholar
[10] Zhou Y, Ren X G, Yan Y Q, Ren H, Du H M, Cai X Y, Huang Z X 2022 Acta Phys. Sin. 71 208802 [周玚, 任信钢, 闫业强, 任昊, 杜红梅, 蔡雪原, 黄志祥 2022 物理学报 71 208802]
Google Scholar
Zhou Y, Ren X G, Yan Y Q, Ren H, Du H M, Cai X Y, Huang Z X 2022 Acta Phys. Sin. 71 208802
Google Scholar
[11] Jang H J, Lee J Y 2019 J. Phys. Chem. C 123 26856
Google Scholar
[12] Zhang J, Ding D X, Wei Y, Xu H 2016 Chem. Sci. 7 2870
Google Scholar
[13] Fan W L, Shen Y, Deng K M, Chen Q H, Bai Y, Li L 2022 Nano Energy 100 107518
Google Scholar
[14] Zhao L C, Tang P Y, Luo D Y, Dar M I, Eickemeyer F T, Arora N, Hu Q, Luo J S, Liu Y H, Zakeeruddin S M, Hagfeldt A, Arbiol J, Huang W, Gong Q H, Russell T P, Friend R H, Grätzel M, Zhu R 2022 Sci. Adv. 8 eabo3733
Google Scholar
[15] Hu P, Zhou W B, Chen J L, Xie X, Zhu J W, Zheng Y X, Li Y F, Li J M, Wei M D 2024 Chem. Eng. J. 480 148249
Google Scholar
[16] Wu J, Li M H, Fan J T, Li Z, Fan X H, Xue D J, Hu J S 2023 J. Am. Chem. Soc. 145 5872
Google Scholar
[17] Li X D, Zhang W X, Guo X M, Lu C Y, Wei J Y, Fang J F 2022 Science 375 434
Google Scholar
[18] Khan M T, Hemasiri N H, Kazim S, Ahmad S 2021 Sustain. Energ. Fuels 5 6352
Google Scholar
[19] Cha J, Kim M K, Lee W, Jin H, Na H, Cung Tien Nguyen D, Lee S, Lim J, Kim M 2023 Chem. Eng. J. 451 138920
Google Scholar
[20] Tan H R, Che F L, Wei M Y, Zhao Y C, Saidaminov M I, Todorović P, Broberg D, Walters G, Tan F R, Zhuang T T, Sun B, Liang Z Q, Yuan H F, Fron E, Kim J, Yang Z Y, Voznyy O, Asta M, Sargent E H 2018 Nat. Commun. 9 3100
Google Scholar
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