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无机钙钛矿CsPbI3由于好的热稳定性和合适的光学带隙具有很好的发展前景, 作为太阳电池的吸收层, CsPbI3必须形成黑色相(α-CsPbI3). 为了低温制备出空气中稳定的优质α-CsPbI3, 本文在前驱液中同时添加碱金属碘化物(NaI, KI)和氢碘酸(HI). 研究发现: 与仅有HI添加剂相比, 添加碱金属碘化物后低温制备的α-CsPbI3薄膜的质量和稳定性均有提高, 即薄膜致密度提高、晶粒增大、内部缺陷减少、光吸收增强. 因此, 碱金属碘化物和HI共添加是进一步提高CsPbI3无机钙钛矿太阳电池效率和稳定性的有效方法.Inorganic cesium lead triiodide (CsPbI3) perovskite films show great prospect due to their high thermal stability and ideal band gap energy. To be used as a photovoltaic absorber, the CsPbI3 must form the black phase (α-CsPbI3). To prepare high-quality CsPbI3 films with phase stability in air at low temperatures, alkali metal iodides and hydroiodic acid (HI) additives are added into precursor solution. The results show that the quality and the phase stability of CsPbI3 with alkali metal iodides and HI additives are obviously improved compared with those with only HI additive. The SEM images show that the CsPbI3 film with 2.5% KI additive becomes more compact than that without KI additive and has no visible pinholes. As the KI additive increases, pinholes start to appear. From the XRD, it can be seen that the crystallinity of perovskite is improved when KI additive increases to 5.0%, while it starts to decrease with KI additive further increasing. The PL intensity of the CsPbI3 film with 2.5% KI additive is higher than the others’, implying a relatively low non-radiative recombination loss and low defect state in that film. And the CsPbI3 film with 2.5% KI additive exhibits increased absorption in the visible region, which is beneficial to enhancing the efficiency of perovskite solar cells. Considering the SEM images, crystallinity, PL intensity and light absorption of perovskite, the optimized KI additive is 2.5% in our work. For the CsPbI3 film with NaI additive, the SEM images show that the films become more compact and have no visible pinholes when NaI additive is 5%. As the NaI additive increases, pinholes appear. The crystallinity of perovskite increases with NaI additive increasing. The PL intensity of the CsPbI3 film with 5% NaI additive is higher than the others’, implying lower defect states in films. And the CsPbI3 film with 5% NaI additive exhibits the improved absorption in the visible region. Considering the SEM images, crystallinity, PL intensity and light absorption of perovskite, the optimized NaI additive is 5%. Therefore, adding alkali metal iodides and HI is an effective method to further improve the stability and efficiency of CsPbI3 perovskite solar cells.
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Keywords:
- CsPbI3 film /
- alkali metal iodide /
- HI /
- stability
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图 1 不同KI掺杂浓度CsPbI3薄膜的SEM图像 (a) x = 0%; (b) x = 2.5%; (c) x = 5.0%; (d) x = 7.5%; (e) x = 10.0%
Fig. 1. SEM surface images of CsPbI3 perovskite films doped with different KI content: (a) x = 0%; (b) x = 2.5%; (c) x = 5.0%; (d) x = 7.5%; (e) x = 10.0%.
图 2 不同KI掺杂浓度CsPbI3薄膜的 (a) XRD图谱与(b)(100)衍射峰半高宽
Fig. 2. (a) (XRD) patterns of CsPbI3 perovskite films doped with different KI content and (b) full width of half maximum at (100) peak
图 3 不同KI掺杂浓度CsPbI3薄膜的(a) PL谱和(b)吸收谱
Fig. 3. (a) PL spectra and (b) UV-vis absorption spectra of CsPbI3 films doped with different KI content.
图 4 不同NaI掺杂浓度CsPbI3薄膜的SEM图像 (a) x = 0%; (b) x = 2.5%; (c) x = 5.0%; (d) x = 7.5%; (e) x = 10.0%
Fig. 4. SEM surface images of CsPbI3 perovskite films doped with different NaI content: (a) x = 0%; (b) x = 2.5%; (c) x = 5.0%; (d) x = 7.5%; (e) x = 10.0%.
图 5 不同NaI掺杂浓度CsPbI3薄膜的XRD图谱
Fig. 5. XRD patterns of CsPbI3 films with different NaI content.
图 6 不同NaI掺杂浓度CsPbI3薄膜的(a) PL谱和(b)吸收谱
Fig. 6. (a) PL spectra, (b) UV-vis absorption spectra of CsPbI3 films doped with different NaI content.
图 7 未掺杂(0%)、2.5% KI和5.0% NaI掺杂CsPbI3薄膜 (a)在空气中放置24 h后的XRD图谱和(b)新鲜制备及空气中放置24 h后的PL图谱
Fig. 7. (a) XRD patterns of undoped, 2.5% KI and 5.0% NaI doped CsPbI3 films exposed for 24 h in ambient air, and (b) PL patterns of the above as-deposited films and films exposed for 24 h in ambient air.
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[1] Yang S, Fu W, Zhang Z, Chen H, Li C Z 2017 J. Mater. Chem. A 5 11462
Google Scholar
[2] 陈永亮, 唐亚文, 陈沛润, 张力, 刘琪, 赵颖, 黄茜, 张晓丹 2020 69 138401
Google Scholar
Chen Y L, Tang Y W, Chen P R, Zhang L, Liu Q, Zhao Y, Huang Q, Zhang X D 2020 Acta Phys. Sin. 69 138401
Google Scholar
[3] Wang Z, Zeng L X, Zhang C L, Lu Y L, Qiu S D, Wang C, Liu C, Pan L J, Wu S H, Hu J L, Liang G X, Fan P, Egelhaaf H J, Brabec C J, Guo F, Mai Y H 2020 Adv. Funct. Mater. 30 2001240
Google Scholar
[4] 李少华, 李海涛, 江亚晓, 涂丽敏, 李文标, 潘玲, 杨仕娥, 陈永生 2018 67 158801
Google Scholar
Li S H, Li H T, Jiang Y X, Tu L M, Li W B, Pan L, Yang S E, Chen Y S 2018 Acta Phys. Sin. 67 158801
Google Scholar
[5] Chang R G, Yan Y T, Zhang J Y, Zhu Z L, Gu J H 2020 Thin Solid Films 712 138279
Google Scholar
[6] Kojima A, Teshima K, Shirai Y, Miyasaka T 2009 J. Am. Chem. Soc. 131 6050
Google Scholar
[7] Best research-cell efficiencies https://www.nrel.gov/pv/cell-efficiency.html [2020-11-1]
[8] Wang F, Geng W, Zhou Y, Fang H H, Tong C J, Antonietta L M, Liu L M, Zhao N 2016 Adv. Mater. 28 9986
Google Scholar
[9] Jiang J X, Wang Q, Jin Z W, Zhang X S, Lei J B, Hai J, Zhang Z G, Li Y f, L iu, S Z 2018 Adv. Energy Mater. 8 1701757
Google Scholar
[10] Huang H, Yuan H F, Jansse K P F, Solís-Fernández G, Wang Y, Tan C Y X, Jonckheere D, Debroye E, Long J L, Hendrix J, Hofkens J, Steele J A, Roeffaers M B J 2018 ACS Energy Lett. 3 755
Google Scholar
[11] Li Z Z, Zhou F G, Wang Q, Ding L M, Jin Z W 2020 Nano Energy 71 104634
Google Scholar
[12] Brennan M C, Draguta S, Kamat P V, Kuno M 2017 ACS Energy Lett. 3 204
[13] Eperon G E, Paterno'Giuseppe M, Sutton R J, Zampetti A, Haghighirad A, Cacialli F, Snaith H 2015 J. Mater. Chem. A 3 19688
Google Scholar
[14] Luo P, Xia W, Zhou S W, Sun L, Cheng J G, Xu C X, Lu Y W, 2016 J. Phys. Chem. Lett. 7 3603
Google Scholar
[15] Ripolles T S, Nishinaka K, Ogomi Y, Miyata Y, Hayase S 2016 Sol. Energy Mater. Sol. Cells 144 532
Google Scholar
[16] Sutton R J, Eperon G E, Miranda L, Parrott E S, Patel J B, Hörantner M T, Johnston M B, Haghighirad A A, Moore D T, Snaith H J 2016 Adv. Energy Mater. 6 1502458
Google Scholar
[17] Haque F, Wright M, Mahmud M A, Yi H M, Wang D, Duan L P, Xu C, Upama M B, Uddin A 2018 ACS Omega. 3 11937
Google Scholar
[18] Zhou Y Y, Game O S, Pang S P, Padture N P J 2015 Phys. Chem. Lett. 6 4827
Google Scholar
[19] Liu F, Zhang Y, Ding C 2017 ACS Nano 11 10373
Google Scholar
[20] Straus D B, Kagan C R 2018 Phys. Chem. Lett. 9 1434
Google Scholar
[21] Miyata K, Atallah T L, Zhu X Y 2017 Sci. Adv. 3 e1701469
Google Scholar
[22] Li B, Zhang Y, Fu L, Yu T, Zhou S, Zhang L, Yin L 2018 Nat.Commun. 9 1076
Google Scholar
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