Improving crystallization and photoelectric performance of CsPbI<sub>2</sub>Br perovskite under ambient air via dynamic hot-air assisted recrystallization strategy

Zhang Zi-Fa; Yuan Xiang; Lu Ying-Shen; He Dan-Min; Yan Quan-He; Cao Hao-Yu; Hong Feng; Jiang Zui-Min; Xu Run; Ma Zhong-Quan; Song Hong-Wei; Xu Fei

doi:10.7498/aps.73.20240153

Abstract

CsPbI₂Br thin films prepared in ambient air are susceptible to humidity, resulting in low coverage, poor crystallization quality, numerous pinholes, and easy transformation into non perovskite phases. To overcome the troubles of pervoksite fabrication in ambient air, a feasible way is to reduce the moisture around the films as much as possible according to dynamic hot-air assisted strategy. However, the hot air accelerates the evaporation rate of solvent, resulting in the decrease of grain size. In order to improve the crystal growth and long-term stability in dynamic hot-air assisted strategy, in this work, we present a dynamic hot-air assisted recrystallization (DHR) strategy to prepare high-quality CsPbI₂Br thin films in ambient air (i.e. the CsPbI₂Br thin films prepared via dynamic hot-air strategy are recrystallized by using a green solvent (methylamine acetate) with high viscosity coefficient). Under ambient air with high humidity (RH＞60%), the CsPbI₂Br thin film with high coverage, (100) preferred orientation, large average grain size, and stable structure is prepared via DHR strategy. The dynamic hot-air process can effectively reduce the moisture around the film and increase the nucleation sites in the precursor solution, thereby improving the coverage of the film. However, this process inevitably results in the significant decrease of grain size (R_ave= 0.32 μm) (i.e. more grain boundaries), exacerbating non-radiative recombination of carriers associated with trap states at these boundaries. The high coverage increases the grain-to-grain contact area, facilitating complete recrystallization. Thus, the recrystallization process can significantly increase the grain size (R_ave = 2.63 μm) and obtain a (100) preferred orientation (I₍₁₁₀₎/I₍₂₀₀₎ = 0.006), resulting in high photoluminescence intensity and long fluorescence lifetime (118 ns). The unencapsulated CsPbI₂Br perovskite solar cell (PSC) optimized via DHR strategy with low hysterescence factor (2.34%) and high repeatability exhibits a high power conversion efficiency (PCE = 17.55%), which is higher than those of most CsPbI₂Br PSCs prepared in ambient air and gloveboxes previously reported. Moreover, the unencapsulated CsPbI₂Br PSC possesses an excellent storage stability under ambient air with high humidity (RH > 60%), remaining 96% of the original PCE after aging 40 days. This provides a promising approach for achieving high-performance and long-term stable CsPbI₂Br films under ambient air with high humidity, which is expected to promote the commercialization process of perovskite/silicon tandem cells and semi-transparent devices.

Keywords:

CsPbI₂Br /
dynamic hot-air assisted recrystallization /
ambient air /
photoelectric performance

Authors and contacts

1.
Shanghai Key Laboratory of High Temperature Superconductors, College of Sciences, Shanghai University, Shanghai 200444, China
2.
State Key Laboratory of Surface Physics, Department of Physics, Fudan University, Shanghai 200433, China
3.
Department of Electronic Information Materials, Shanghai University, Shanghai 200444, China

Corresponding author: Xu Fei, feixu@shu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 62350054, 12175131, 12374379).

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References

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Cited By

图 1 对照组和优化组薄膜的(a) OM表面形貌图、(b) AFM表面形貌图、(c)晶粒尺寸统计图、(d) XRD图谱和(e)示意图

Figure 1. The (a) OM images, (b) AFM images, (c) grain size statistics, (d) XRD patterns, and (e) schematic of the control group and optimized group thin films.

DownLoad: Full-Size Img PowerPoint

图 2 CsPbI₂Br单胞的(a)晶体结构和(b)能带结构; 对照组和优化组薄膜的(c)紫外-可见吸收光谱及PL光谱(实线表示玻璃基底上PVSK的PL光谱; 方块表示SnO₂上PVSK的PL光谱)

Figure 2. (a) Crystal structure and (b) band structure of CsPbI₂Br unit cell; (c) UV-vis absorption spectra and PL spectra of the control group and optimized group thin films (the solid line represents the PL spectra of PVSK on glass; the square dots represent the PL spectra of PVSK on SnO₂).

DownLoad: Full-Size Img PowerPoint

图 3 对照组和优化组薄膜的(a)吸收系数的对数形式与光子能量的曲线图, (b)透射光谱, (c) TRPL光谱, 以及(d)—(g)老化图像及其紫外-可见吸收光谱

Figure 3. The (a) ln(α) versus energy, (b) transmission spectra, (c) TRPL spectra, and (d)–(g) photos and UV-vis absorption spectra with aging time of the control group and optimized group thin films.

DownLoad: Full-Size Img PowerPoint

图 4 对照组和优化组钙钛矿太阳能电池的(a)光电流密度-电压曲线, (b)光电流密度-电压正反扫曲线, (c)外量子效率, (d)转换效率统计分布图, (e)短路电流统计分布图, (f)开路电压统计分布图, (g)填充因子统计分布图, (h)开路电压随光照强度变化, (i)电流-电压曲线, (j)储存稳定性

Figure 4. The (a) J-V curves, (b) hysteresis curves, (c) EQE spectra, (d) PCE statistics, (e) J_SC statistics, (f) V_OC statistics, (g) FF statistics, (h) light intensity-dependent V_OC variation, (i) current-voltage curves, and (j) storage stability of the control group and optimized group perovskite solar cells.

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表 1 对照组与优化组CsPbI₂Br薄膜TRPL光谱的拟合参数

Table 1. Fitting parameters of TRPL spectra for the control group and optimized group CsPbI₂Br thin films.

Sample	A₁	τ₁ /ns	A₂	τ₂ /ns	τ_ave/ns
Control	0.92	6.45	0.08	118	75
REC	0.91	7.35	0.09	160	112
DHA	0.71	2.77	0.29	105	99
DHR	0.69	9.36	0.31	135	118

DownLoad: CSV

表 2 采用动态热风辅助再结晶策略的CsPbI₂Br太阳能电池与其他CsPbI₂Br太阳能电池的性能比较

Table 2. Performance comparison of CsPbI₂Br solar cells via dynamic hot-air assisted recrystallization strategy with other reports.

年份	制备环境	策略	效率/%	稳定性	文献
2022	N₂	Doping	16.20	88.6%, 42 d (air, 30% RH)	[35]
2023	N₂	Interface engineering	17.33	88.7%, 42 d (air, 10% RH)	[36]
2023	N₂	Doping	17.70	97%, 42 d (air, 10% RH)	[37]
2019	Air, 25%—35% RH	DHA	14.85	90%, 17 d (air, 85 ℃)	[18]
2020	Air, 30% RH	Precursor engineering	16.14	93%, 35 d (air, 30% RH)	[17]
2021	Air, 35% RH	DHA+Doping	17.46	80%, 17 d (air, 30% RH)	[38]
2023	Air, —	DHA+Doping	16.74	90%, 17 d (air, 25% RH)	[39]
2023	Air, 20% RH	DHA+Doping	17.39	84%, 9 d (N₂, 85 ℃)	[19]
2023	Air, —	Doping	17.38	90%, 42 d (air, 25% RH)	[40]
2023	Air, —	DHA+Doping	17.40	87.25%, 30 d (air, 14% RH)	[41]
2024	Air, ＞60% RH	DHR	17.55	96%, 40 d (air, ＞60% RH)	This work

DownLoad: CSV

[1]	Zhang H, Pfeifer L, Zakeeruddin S M, Chu J H, Grätzel M 2023 Nat. Rev. Chem. 7 632 Google Scholar
[2]	Zhang S, Ye F Y, Wang X Y, Chen R, Zhang H D, Zhan L Q, Jiang X Y, Li Y W, Ji X Y, Liu S J, Yu M J, Yu F R, Zhang Y L, Wu R H, Liu Z H, Ning Z J, Neher D, Han L Y, Lin Y Z, Tian H, Chen W, Stolterfoht M, Zhang L J, Zhu W H, Wu Y Z 2023 Science 380 404 Google Scholar
[3]	Park J, Kim J, Yun H S, Paik M J, Noh E, Mun H J, Kim M G, Shin T J, Seok S I 2023 Nature 616 724 Google Scholar
[4]	Ahn N, Kwak K, Jang M S, Yoon H, Lee B Y, Lee J K, Pikhitsa P V, Byun J, Choi M 2016 Nat. Commun. 7 13422 Google Scholar
[5]	Xu D F, Wang J A, Duan Y W, Yang S M, Zou H, Yang L, Zhang N, Zhou H, Lei X R, Wu M Z, Liu S Z, Liu Z K 2023 Adv. Funct. Mater. 33 2304237 Google Scholar
[6]	Wang J A, Che Y H, Duan Y W, Liu Z K, Yang S M, Xu D F, Fang Z M, Lei X R, Li Y, Liu S Z 2023 Adv. Mater. 35 2210223 Google Scholar
[7]	Li Y R, Zhang Y, Zhu P D, Li J B, Wu J W, Zhang J Y, Zhou X Y, Jiang Z Y, Wang X Z, Xu B M 2023 Adv. Funct. Mater. 33 2309010 Google Scholar
[8]	Zeng Q S, Zhang X Y, Feng X L, Lu S Y, Chen Z L, Yong X, Redfern S A T, Wei H T, Wang H Y, Shen H Z, Zhang W, Zheng W T, Zhang H, Tse J S, Yang B 2018 Adv. Mater. 30 1705393 Google Scholar
[9]	Guo Y X, Yin X T, Liu J, Wen S, Wu Y T, Que W X 2019 Sol. RRL 3 1900135 Google Scholar
[10]	Long Y, Liu K, Zhang Y L, Li W Z 2021 Molecules 26 3398 Google Scholar
[11]	Sun S Q, Xu X W, Sun Q, Yao Q, Cai Y T, Li X Y, Xu Y L, He W, Zhu M, Lv X, Lin F C R, Jen A K Y, Shi T T, Yip H L, Fung M K, Xie Y M 2023 Adv. Energy Mater. 13 2204347 Google Scholar
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[13]	Liu X Y, Lian H J, Zhou Z R, Zou C, Xie J, Zhang F, Yuan H Y, Yang S, Hou Y, Yang H G 2022 Adv. Energy Mater. 12 2103933 Google Scholar
[14]	Wang Y, Mahmoudi T, Rho W Y, Hahn Y B 2019 Nano Energy 64 103964 Google Scholar
[15]	Cheng Y H, Xu X W, Xie Y M, Li H W, Qing J, Ma C Q, Lee C S, So F, Tsang S W 2017 Sol. RRL 1 1700097 Google Scholar
[16]	Gao H, Ban C X, Li F M, Yu T, Yang J, Zhu W D, Zhou X X, Fu G, Zou Z G 2015 ACS Appl. Mater. Interfaces 7 9110 Google Scholar
[17]	Duan C Y, Cui J, Zhang M M, Han Y, Yang S M, Zhao H, Bian H T, Yao J X, Zhao K, Liu Z K, Liu S Z 2020 Adv. Energy Mater. 10 2000691 Google Scholar
[18]	Mali S S, Patil J V, Hong C K 2019 Nano Lett. 19 6213 Google Scholar
[19]	Xiao H R, Zuo C T, Zhang L X, Zhang W H, Hao F, Yi C Y, Liu F Y, Jin H L, Ding L M 2023 Nano Energy 106 108061 Google Scholar
[20]	Blochl P E 1994 Phys. Rev. B 50 17953 Google Scholar
[21]	Yin G N, Zhao H, Jiang H, Yuan S H, Niu T Q, Zhao K, Liu Z K, Liu S Z 2018 Adv. Funct. Mater. 28 1803269 Google Scholar
[22]	Wang J X, Liu Y B, Xiao X D, Bi Z N, Lu Y, Sheng G Z, Cai X S, Zhu Y Q, Xu X Q, Xu G 2021 Sol. Energy 216 7 Google Scholar
[23]	Yu F Y, Han Q J, Wang L, Yang S Z, Cai X Y, Zhang C, Ma T L 2021 Sol. RRL 5 2100404 Google Scholar
[24]	Cao R N, Xu F, Zhu J B, Ge S, Wang W Z, Xu H T, Xu R, Wu Y L, Ma Z Q, Hong F, Jiang Z M 2016 Adv. Energy Mater. 6 1600814 Google Scholar
[25]	曹汝楠, 徐飞, 朱佳斌, 葛升, 王文贞, 徐海涛, 徐闰, 吴杨琳, 马忠权, 洪峰, 蒋最敏 2016 物理学报 65 188801 Google Scholar Cao R N, Xu F, Zhu J B, Ge S, Wang W Z, Xu H T, Xu R, Wu Y L, Ma Z Q, Hong F, Jiang Z M 2016 Acta Phys. Sin. 65 188801 Google Scholar
[26]	Wang X J, Ran X Q, Liu X T, Gu H, Zuo S W, Hui W, Lu H, Sun B, Gao X Y, Zhang J, Xia Y D, Chen Y H, Huang W 2020 Angew. Chem. Int. Edit. 59 13354 Google Scholar
[27]	Hong F, Li Y, Xiang W, Liu X, Jiang Z M, Ma Z Q, Xu F 2021 Chem. Lett. 50 1500 Google Scholar
[28]	Chao L F, Xia Y D, Li B X, Xing G C, Chen Y H, Huang W 2019 Chem 5 995 Google Scholar
[29]	Haque M A, Troughton J, Baran D 2020 Adv. Energy Mater. 10 1902762 Google Scholar
[30]	Xu F, Wang X, Li Y, Jiang B, Dong Z R, Yang Z C, Kang J X, Shu X, Jiang Z M, Hong F, Xu R, Ma Z Q, Chen T, Xu Z, Xu H T 2022 Adv. Opt. Mater. 10 2200930 Google Scholar
[31]	Xue Q F, Bai Y, Liu M Y, Xia R X, Hu Z C, Chen Z M, Jiang X F, Huang F, Yang S H, Matsuo Y, Yip H L, Cao Y 2017 Adv. Energy Mater. 7 1602333 Google Scholar
[32]	Gau D L, Galain I, Aguiar I, Marotti R E 2023 J. Lumines. 257 119765 Google Scholar
[33]	Yang B, Dyck O, Poplawsky J, Keum J, Puretzky A, Das S, Ivanov I, Rouleau C, Duscher G, Geohegan D, Xiao K 2015 J. Am. Chem. Soc. 137 9210 Google Scholar
[34]	Zhu Z K, Shang J T, Tang G Q, Wang Z, Cui X X, Jin J J, Zhou Y, Zhang X, Zhang D, Liu X W, Tai Q D 2023 Chem. Eng. J. 454 140163 Google Scholar
[35]	Wang A L, Wang J W, Niu X B, Zuo C T, Hao F, Ding L M 2022 InfoMat 4 e12263 Google Scholar
[36]	Guo Q, Dai Z, Dong C Q, Ding Y J, Jiang N Z, Wang Z B, Gao L, Duan C, Guo Q, Zhou E R 2023 Chem. Eng. J. 461 142025 Google Scholar
[37]	Jeong M J, Jeon S W, Kim S Y, Noh J H 2023 Adv. Energy Mater. 13 2300698 Google Scholar
[38]	Mali S S, Patil J V, Shinde P S, de Miguel G, Hong C K 2021 Matter 4 635 Google Scholar
[39]	Patil J V, Mali S S, Sadale S B, Hong C K 2023 Inorg. Chem. Front. 10 3213 Google Scholar
[40]	Hu Y Q, Cai L J, Xu Z, Wang Z, Zhou Y F, Sun G P, Sun T M, Qi Y B, Zhang S F, Tang Y F 2023 Inorg. Chem. 62 5408 Google Scholar
[41]	Bahadur J, Ryu J, Pandey P, Cho S W, Cho J S, Kang D W 2023 Nanoscale 15 3850 Google Scholar

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Vol. 73, Issue 9 - 2024-05-05

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Improving crystallization and photoelectric performance of CsPbI₂Br perovskite under ambient air via dynamic hot-air assisted recrystallization strategy

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Corresponding author: Xu Fei, feixu@shu.edu.cn

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Improving crystallization and photoelectric performance of CsPbI2Br perovskite under ambient air via dynamic hot-air assisted recrystallization strategy

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Corresponding author: Xu Fei, feixu@shu.edu.cn

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Improving crystallization and photoelectric performance of CsPbI₂Br perovskite under ambient air via dynamic hot-air assisted recrystallization strategy