Perovskite solar cells passivated by distorted two-dimensional structure

Fu Peng-Fei; Yu Dan-Ni; Peng Zi-Jian; Gong Jin-Kang; Ning Zhi-Jun

doi:10.7498/aps.68.20190306

Abstract

Hybrid perovskites are a series of solution-processable materials for photovoltaic devices. To achieve better performance and stability, interface passivation is an effective method. So far, the most commonly used passivators are organic amines, which can tailor perovskite into a lower-dimensional structure (Ruddlesden-Popper perovskite). Here, we select a biimizole (BIM) molecule as a new passivator for perovskite. The BIM based single layer perovskite has a more rigid structure. And multi-layered structure cannot be formed due to large lattice mismatching and structural rigidity. By inducing the excess MAI (methanaminium iodide) into the lattice, the layered structure is maintained, and half of the BIM molecules are replaced by MA (methylamine). The mixed layered structure is distorted, because of the difference in size between two kinds of cations. We then investigate passivation effect of BIM on perovskite solar cells. By carefully controlling the feed ratio in precursor solutions, we fabricate solar cells with different passivation structures. We find that the introduction of BIM can cause V_oc to increase generally, indicating that MAPbI₃ is well passivated. The peak at 7.5° and 15° in X-ray diffraction pattern are corresponding to a two-dimensional (2D) phase with a shorter layer distance. There are no peaks at lower degrees, so that no multi-layered structure is formed in the film either. We suppose that a dual-phase 2D-3D (where 3D represents three-dimensional) structure is formed in the perovskite film. To explain the passivation effect of the two 2D structures, we investigate their lattice matching towards MAPbI₃. The distorted 2D structure is well matched with (110) face of o-MAPbI₃, and the mismatching rate is lower 1% in the two directions. On the other hand, the BIM based 2D structure cannot well match with (–110) face of o-MAPbI₃, nor with (001) face of c-MAPbI₃. We also consider that the less rigidity of distorted structure contributes to better passivation. As a result, we achieve a BIM passivated perovskite solar cell with a power conversion efficiency up to 14%. This work paves a new way to the interface engineering of perovskite solar cells.

Keywords:

Authors and contacts

1.
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
2.
Shanghai Institute of Ceramics, Shanghai 200050, China
3.
University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Ning Zhi-Jun, ningzhj@shanghaitech.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 21571129, 51572128).

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References

[1]	Luo W, Wu C, Wang D, Zhang Y, Zhang Z, Qi X, Zhu N, Guo X, Qu B, Xiao L, Chen Z 2019 ACS Appl. Mater. Interfaces 11 9149 Google Scholar
[2]	Shang Y, Li G, Liu W, Ning Z 2018 Adv. Funct. Mater. 28 1801193 Google Scholar
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[13]	Zheng H, Liu G, Zhu L, Ye J, Zhang X, Alsaedi A, Hayat T, Pan X, Dai S 2018 Adv. Energy Mater. 8 1800051
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[28]	Li Y, Milić J V, Ummadisingu A, Seo J Y, Im J H, Kim H S, Liu Y, Dar M I, Zakeeruddin S M, Wang P, Hagfeldt A, Grätzel M 2019 Nano Lett. 19 150
[29]	Cohen B E, Li Y, Meng Q, Etgar L 2019 Nano Lett. 19 2588

Cited By

图 1 二维钙钛矿的结构　(a) BA₂PbI₄; (b) BA₂MAPb₂I₇; (c) BIMPbI₄; (d) MA₂BIMPb₂I₈

Figure 1. Structure of two-dimensional perovskite: (a) BA₂PbI₄; (b) BA₂MAPb₂I₇; (c) BIMPbI₄; (d) MA₂BIMPb₂I₈.

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图 2 钙钛矿薄膜表征　(a)二维-三维(2D-3D)混合薄膜X射线衍射图; (b)薄膜吸收光谱及荧光光谱

Figure 2. Characterization of perovskite films: (a) X-ray diffraction of 2D-3D perovskite film; (b) Abs and PL of perovskite films.

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图 A1 钙钛矿薄膜X射线衍射小角度放大图

Figure A1. Magnification of low angle X-ray diffraction patterns of perovskite films

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图 3 不同组成对应器件性能比较　(a) 开路电压; (b) 短路电流; (c) 光电转换效率; (d) 电流-电压曲线

Figure 3. Device performance with different composition: (a) Open-circuit voltage; (b) short-circuit current; (c) power conversion efficiency; (d) plot of J-V curves.

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图 4 晶界的钝化模型　(a) MA₂BIMPb₂I₈ (002)面与MAPbI₃ (110)面晶格匹配; (b) BIMPbI₄ (002)面与MAPbI₃ (–110)面晶格匹配; (c) 晶面透视图及两个方向上的晶格参数; (d)钙钛矿钝化模型

Figure 4. Passivation model of interfaces: (a) Lattice matching of MA₂BIMPb₂I₈ (002) and MAPbI₃ (110); (b) lattice matching of BIMPbI₄ (002) and MAPbI₃ (–110); (c) perspective of layered crystal and lattice parameter of two directions; (d) passivation of perovskite.

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图 A2 最佳性能电池器件的回滞曲线

Figure A2. Hysteresis curves of the best device

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表 A2 器件制备前驱液配方

Table A2. Composition of perovskite precursor solutions

组成	投料摩尔比(BIMI₂:MAI:PbI₂)
BIM_0.2MA_0.8PbI_3.2 (BIMPbI₄:MAPbI₃ = 0.2 : 0.8)	0.2 : 0.8 : 1
BIM_0.1MA_0.9PbI_3.1 (BIMPbI₄:MAPbI₃ = 0.1 : 0.9)	0.1 : 0.9 : 1
BIM_0.2MAPbI_3.4 (MA₂BIMPb₂I₈:MAPbI₃ = 0.1 : 0.8)	0.2 : 1 : 1
BIM_0.1MAPbI_3.2 (MA₂BIMPb₂I₈:MAPbI₃ = 0.05 : 0.9)	0.1 : 1 : 1

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表 A3 器件基本参数

Table A3. Parameters of solar cell devices

组成	开路电压Voc/V	短路电流Jsc/ mA·cm^–2	填充因子FF/%	转换效率η/%
BIM_0.2MA_0.8PbI_3.2	1.08	8.90	45.8	4.41
BIM_0.1MA_0.9PbI_3.1	1.01	15.90	67.6	10.89
BIM_0.2MAPbI_3.4	1.07	14.72	66.1	10.46
BIM_0.1MAPbI_3.2	1.08	17.25	75.12	14.06

DownLoad: CSV

表 A4 钝化模型参数总结

Table A4. Summary of parameters in the passivation model

二维晶面	晶格间距/Å (横向, 纵向)	钝化晶面	晶格间距/Å (横向, 纵向)	失配率 (横向, 纵向)
MA₂BIMPb₂I₈ (002)	6.25, 6.38	正交MAPbI₃ (110)	6.26, 6.32	0.16%, 0.95%
BIMPbI₄ (002)	6.45, 6.45	正交MAPbI₃ (–110)	6.32, 6.26	2.06%, 3.04%
BIMPbI₄ (002)	6.45, 6.45	立方MAPbI₃ (001)	6.31, 6.31	2.22%, 2.22%

DownLoad: CSV

表 A1 MA₂BIMPb₂I₈ 单晶数据报告

Table A1. Crystallographic parameter of MA₂BIMPb₂I₈

参数	取值
Compound	MA₂BIMPb₂I₈
Formula weight	1628.6
Temperature/K	249.99
Crystal system	orthorhombic
Space group	Pmna
a/Å	12.5016(7)
b/Å	6.3876(4)
c/Å	18.8380(12)
α/(°)	90.00
β/(°)	90.00
γ/(°)	90.00
Volume/Å³	1504.31(16)
Z	4
ρ_calc/g·cm^–3	5.581
μ/mm^–1	46.218
F(000)	2086.0
Radiation	Mo K_α (λ = 0.71073)
2θ range for data collection/(°)	6.38 to 52.72
Index ranges	–15 ≤ h ≤ 15, –7 ≤ k ≤ 7, –23 ≤ l ≤ 23
Reflections collected	12046
Independent reflections	1608 [Rint = 0.0780, Rsigma = 0.0442]
Data/restraints/parameters	1608/0/64
Goodness-of-fit on F²	1.039
Final R indexes [I ≥ 2σ(I)]	R1 = 0.0485, wR2 = 0.1043
Final R indexes [all data]	R1 = 0.0767, wR2 = 0.1171
Largest diff. peak/hole/e·Å^–3	3.45/–2.09

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表 A5 近期二维钙钛矿太阳能电池进展

Table A5. Recent advances of 2D perovskite solar cells

组成	类型/层数	V_oc/V	J_sc /mA·cm^-2	FF/%	η/%
(PEA)₂(MA)₃Pb₄I₁₃	RP (4)	1.16	14.7	77	12.1^[22]
(BA)₂MA₃Pb₄I₁₃	RP (4)	0.99	18.43	75.2	13.8^[16]
(BEA)₂MA₃Pb₄I₁₃	RP (4)	1.01	20.63	78.0	16.1^[16]
(BYA)₂MA₃Pb₄I₁₃	RP (4)	1.01	19.53	76.4	15.1^[16]
(PEA)₂MA₃Pb₄I₁₃	RP (4)	1.14	18.78	62	13.41^[23]
BA₂MA₄Pb₅I₁₆	RP (5)	0.99	11.67	72.1	8.32^[24]
PA₂MA₄Pb₅I₁₆	RP (5)	1.13	18.89	49	10.41^[14]
(BA)₂(MA)₃Pb₄I₁₃	RP (4)	1.06	16.6	70.9	12.5^[25]
3AMP(MA)₃Pb₄I₁₃	DJ (4)	1.06	10.17	67.6	7.33^[26]
3AMP(MA_0.75FA_0.25)₃Pb₄I₁₃	DJ (4)	1.09	13.69	81.04	12.04^[27]
(PDMA)FA₂Pb₃I₁₀	DJ (3)	0.84	11.48	72.1	7.11^[28]
BzDA(Cs_0.05MA_0.15FA_0.8)₉Pb₁₀(I_0.93Br_0.07)₃₁	DJ (10)	1.02	21.5	71	15.6^[29]
BIM_0.2MAPbI_3.4	4	1.07	14.72	66.1	10.46
BIM_0.1MAPbI_3.2	9	1.08	17.25	75.1	14.06

DownLoad: CSV

[1]	Luo W, Wu C, Wang D, Zhang Y, Zhang Z, Qi X, Zhu N, Guo X, Qu B, Xiao L, Chen Z 2019 ACS Appl. Mater. Interfaces 11 9149 Google Scholar
[2]	Shang Y, Li G, Liu W, Ning Z 2018 Adv. Funct. Mater. 28 1801193 Google Scholar
[3]	Yang R, Li R, Cao Y, Wei Y, Miao Y, Tan W L, Jiao X, Chen H, Zhang L, Chen Q, Zhang H, Zou W, Wang Y, Yang M, Yi C, Wang N, Gao F, McNeill C R, Qin T, Wang J, Huang W 2018 Adv. Mater. 30 e1804771 Google Scholar
[4]	Si J, Liu Y, He Z, Du H, Du K, Chen D, Li J, Xu M, Tian H, He H, Di D, Lin C, Cheng Y, Wang J, Jin Y 2017 ACS Nano 11 11100 Google Scholar
[5]	Raghavan C M, Chen T P, Li S S, Chen W L, Lo C Y, Liao Y M, Haider G, Lin C C, Chen C C, Sankar R, Chang Y M, Chou F C, Chen C W 2018 Nano Lett. 18 3221 Google Scholar
[6]	Stoumpos C C, Cao D H, Clark D J, Young J, Rondinelli J M, Jang J I, Hupp J T, Kanatzidis M G 2016 Chem. Mater. 28 2852 Google Scholar
[7]	Tsai H, Nie W, Blancon J C, Stoumpos C C, Asadpour R, Harutyunyan B, Neukirch A J, Verduzco R, Crochet J J, Tretiak S, Pedesseau L, Even J, Alam M A, Gupta G, Lou J, Ajayan P M, Bedzyk M J, Kanatzidis M G 2016 Nature 536 312 Google Scholar
[8]	Wang K, Wu C, Yang D, Jiang Y, Priya S 2018 ACS Nano 12 4919 Google Scholar
[9]	Liao Y, Liu H, Zhou W, Yang D, Shang Y, Shi Z, Li B, Jiang X, Zhang L, Quan L N, Quintero-Bermudez R, Sutherland B R, Mi Q, Sargent E H, Ning Z 2017 J. Am. Chem. Soc. 139 6693 Google Scholar
[10]	Quintero-Bermudez R, Gold-Parker A, Proppe A H, Munir R, Yang Z, Kelley S O, Amassian A, Toney M F, Sargent E H 2018 Nat. Mater. 17 900 Google Scholar
[11]	Qiu J, Zheng Y, Xia Y, Chao L, Chen Y, Huang W 2018 Adv. Funct. Mater. DOI: 10.1002/adfm.201806831
[12]	Lai H, Kan B, Liu T, Zheng N, Xie Z, Zhou T, Wan X, Zhang X, Liu Y, Chen Y 2018 J. Am. Chem. Soc. 140 11639 Google Scholar
[13]	Zheng H, Liu G, Zhu L, Ye J, Zhang X, Alsaedi A, Hayat T, Pan X, Dai S 2018 Adv. Energy Mater. 8 1800051
[14]	Cheng P, Xu Z, Li J, Liu Y, Fan Y, Yu L, Smilgies D M, Müller C, Zhao K, Liu S F 2018 ACS Energy Lett. 3 1975 Google Scholar
[15]	Zhang T, Cao Z, Shang Y, Cui C, Fu P, Jiang X, Wang F, Xu K, Yin D, Qu D, Ning Z 2018 J. Photochem. Photobiol. A: Chem. 355 42 Google Scholar
[16]	Chao L, Niu T, Xia Y, Ran X, Chen Y, Huang W 2019 J. Phys. Chem. Lett. 10 1173
[17]	Liu D, Zhou W, Tang H, Fu P, Ning Z 2018 Sci. China: Chem. 61 1278 Google Scholar
[18]	You J, Meng L, Song T B, Guo T F, Yang Y M, Chang W H, Hong Z, Chen H, Zhou H, Chen Q, Liu Y, de Marco N, Yang Y 2016 Nat. Nanotech. 11 75 Google Scholar
[19]	Billing D G, Lemmerer A 2007 Acta Crystallogr. B 63 735 Google Scholar
[20]	Tang Z, Guan J, Guloy A M 2001 J. Mater. Chem. 11 479 Google Scholar
[21]	Niu G, Li W, Li J, Wang L 2016 Sci. Chi. Mater. 59 728 Google Scholar
[22]	Qing J, Liu X K, Li M, Liu F, Yuan Z, Tiukalova E, Yan Z, Duchamp M, Chen S, Wang Y, Bai S, Liu J M, Snaith H J, Lee C S, Sum T C, Gao F 2018 Adv. Energy Mater. 8 1800185
[23]	Yu S, Yan Y, Chen Y, Chábera P, Zheng K, Liang Z 2019 J. Mater. Chem. A 7 2015 Google Scholar
[24]	Stoumpos C C, Soe C M M, Tsai H, Nie W, Blancon J C, Cao D H, Liu F, Traoré B, Katan C, Even J, Mohite A D, Kanatzidis M G 2017 Chem 2 427 Google Scholar
[25]	Zuo C, Scully A D, Vak D, Tan W, Jiao X, McNeill C R, Angmo D, Ding L, Gao M 2019 Adv. Energy Mater. 9 1803258 Google Scholar
[26]	Mao L, Ke W, Pedesseau L, Wu Y, Katan C, Even J, Wasielewski M R, Stoumpos C C, Kanatzidis M G 2018 J. Am. Chem. Soc. 140 3775 Google Scholar
[27]	Ke W, Mao L, Stoumpos C C, Hoffman J, Spanopoulos I, Mohite A D, Kanatzidis M G 2019 Adv. Energy Mater. 9 1803384 Google Scholar
[28]	Li Y, Milić J V, Ummadisingu A, Seo J Y, Im J H, Kim H S, Liu Y, Dar M I, Zakeeruddin S M, Wang P, Hagfeldt A, Grätzel M 2019 Nano Lett. 19 150
[29]	Cohen B E, Li Y, Meng Q, Etgar L 2019 Nano Lett. 19 2588

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Vol. 68, Issue 15 - 2019-08-05

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