P-I-N型锡铅钙钛矿太阳电池性能的限制因素及解决策略

王俪璇; 李仁杰; 刘辉; 王鹏阳; 石标; 赵颖; 张晓丹

doi:10.7498/aps.70.20201678

摘要

锡铅钙钛矿太阳电池已被证明可以用于全钙钛矿叠层太阳电池中, 作为窄带隙底电池进一步提高器件光电转换效率. 目前, P-I-N型锡铅钙钛矿太阳电池的最高效率为21.7%, 明显低于铅基钙钛矿太阳电池. 本文分析了限制其性能提高的主要因素, 并针对性地总结了近几年研究工作者们提出的有效解决策略, 主要包括: 1)通过添加富锡化合物、强还原剂或含大的有机阳离子的化合物以抑制Sn²⁺氧化, 减少锡铅钙钛矿材料p型掺杂程度, 降低电池开路电压损耗; 2)通过调控组分、改变钙钛矿薄膜制备方法、溶剂工程或添加含功能性基团的化合物以延缓锡铅钙钛矿薄膜结晶生长速率, 提高薄膜质量; 3)通过选用合适的电子传输层或空穴传输层, 减少能级失配对载流子传输的影响或避免载流子传输层的本身不稳定性对器件的影响. 最后, 本文展望了锡铅钙钛矿太阳电池的未来发展, 认为其不仅有望实现高效稳定的单结太阳电池, 而且还可以应用于高效全钙钛矿叠层太阳电池.

关键词:

Abstract

In order to break through the limit of Shockley-Queisser (SQ) radiation and further improve the efficiency of perovskite solar cells, tin-lead perovskite solar cells have widely and successfully been used as narrow-bandgap bottom cells in all-perovskite tandem solar cells. The highest efficiency of tin-lead perovskite solar cells has recently reached 21.7%, which, however, is still lower than that of lead-based perovskite solar cells. This article analyzes the main factors that limit the further improving of their performances, and summarizes the effective solutions proposed by researchers in recent years. The main points are as follows: 1) by adding tin-rich additives, strong reducing agents or compounds containing large organic cations, Sn²⁺ oxidation is inhibited and the p-doped degree of tin-lead perovskite and the open-circuit voltage loss are reduced; 2) through regulating the composition, changing the method of preparing the perovskite film, adding functional groups or solvent engineering, the crystallization rate of tin-lead perovskite film is delayed and the crystallization quality of the film is improved; 3) by selecting an appropriate electron transport layer or hole transport layer the influence of energy level mismatch on carrier transport or the instability of carrier transport layer on devices can be avoided. Finally, the future development of Sn-Pb perovskite solar cells is prospected. It is believed that the tin-lead perovskite solar cells can realize not only the high efficiency and stable single-junction solar cells, but also high efficiency perovskite-perovskite tandem solar cells.

Keywords:

作者及机构信息

1.
南开大学, 光电子薄膜器件与技术研究所, 太阳能转换中心, 天津　300350

2.
天津市光电子薄膜器件与技术重点实验室, 天津　300350

3.
薄膜光电子技术教育部工程研究中心, 天津　300350

4.
化学科学与工程协同创新中心, 天津　300072

5.
南开大学可再生能源转换与储存中心, 天津　300072

通信作者: 张晓丹, xdzhang@nankai.edu.cn

基金项目: 国家重点研发计划(批准号: 2018YFB1500103)、国家自然科学基金(批准号: 61674084)、高等学校学科创新引智计划(111 计划)(批准号: B16027)、天津市军民融合科技重大专项(批准号: 18ZXJMTG00220)和中央高校基本科研业务费(批准号: 63201171, 63201173)资助的课题

Authors and contacts

1.
Solar Energy Conversion Center, Institute of Photoelectronic Thin Film Devices and Technology, Nankai University, Tianjin 300350, China

2.
Key Laboratory of Photoelectronic Thin Film Devices and Technology of Tianjin, Tianjin 300350, China

3.
Engineering Research Center of Thin Film Photoelectronic Technology of Ministry of Education, Tianjin 300350, China

4.
Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, China

5.
Renewable Energy Conversion and Storage Center, Nankai University, Tianjin 300072, China

Corresponding author: Zhang Xiao-Dan, xdzhang@nankai.edu.cn

Funds: Project supported by the National Research Program of China (Grant No. 2018YFB1500103), the National Natural Science Foundation of China (Grant No. 61674084), the 111 Project, China (Grant No. B16027), the Tianjin Civil Military Integration Project, China (Grant No. 18ZXJMTG00220), and the Fundamental Research Funds for the Central Universities, China (Grant Nos. 63201171, 63201173)

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施引文献

图 1 提高P-I-N型锡铅钙钛矿太阳电池性能的解决策略

Fig. 1. Solutions to improve the performance of P-I-N type tin lead perovskite solar cells.

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图 2 钙钛矿材料的能带结构随着金属比例的变化而调整　(a) Ogomi等^[5]表征CH₃NH₃Sn_1–xPb_xI₃能带结构随金属比例的变化; (b) Eperon等^[7]通过Tauc plot、PL及第一性原理计算FASn_xPb_1–xI₃带隙随金属比例的变化趋势; (c) Hao等^[8]通过紫外吸收光谱表征CH₃NH₃Sn_1–xPb_xI₃的带隙变化

Fig. 2. The energy band of Sn-Pb perovskite changed with the metal ratios: (a) Ogomi et al.^[5] characterized the CH₃NH₃Sn_1–xPb_xI₃ energy band structure changed with the metal ratio; (b) Eperon et al.^[7] used the Tauc plot, PL and first-principles calculations to obtain the variable trend of HC(NH₂)₂Sn_xPb_1–xI₃(FASn_xPb_1–xI₃) band gap with metal proportions; (c) Hao et al.^[8] characterized the band gap changes of CH₃NH₃Sn_1–xPb_xI₃ by electronic absorption spectra.

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图 3 不同结构的Sn-Pb钙钛矿太阳电池器件效率进展图, 包括N-I-P型(绿色)和P-I-N型(红色)结构

Fig. 3. The efficiency progress diagram of Sn-Pb perovskite solar cells in different structures, including N-I-P (green) and P-I-N (red) structures.

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图 4 (a)不同SnF₂添加量的钙钛矿薄膜扫描电子显微镜(scanning electron microscope, SEM)扫描图^[34]; (b) Zhu等^[39]利用伽伐尼置换反应(GDR)制备MAPb_xSn_1–xI₃钙钛矿溶液的照片和示意图以及薄膜老化过程机制示意图; (c)由于前驱体溶液中存在Sn⁴⁺而在Sn-Pb钙钛矿中形成锡空位的示意图^[18]; (d) Wei等^[42]利用PEAI实现Sn-Pb钙钛矿表面钝化或膜内钝化的处理方法示意图; (e) Ramirez等^[43]引入叔丁胺离子n = 4和n = 5的Sn-Pb钙钛矿晶格示意图; (f) Li等^[44]引入4-氟苯乙基碘化铵(FPEAI)使(MAPbI₃)_0.75(FASnI₃)_0.25晶粒高度垂直排列的示意图及未使用与使用(FPEAI)的器件J-V曲线

Fig. 4. (a) SEM images of perovskite films with different SnF₂ additions^[34]; (b) photos and schematic diagrams of preparing MAPb_xSn_1–xI₃ precursor solution using GDR and the schematic diagram of film aging process^[39]; (c) the schematic diagram of tin vacancies formation in Sn-Pb perovskite due to the presence of Sn⁴⁺ in the precursor solution^[18]; (d) Wei et al. ^[42]used PEAI to achieve surface passivation or in-film passivation of Sn-Pb perovskit; (e) the schematic diagram of Sn-Pb perovskite lattice with n = 4 and n = 5 introduced by Ramirez et al.^[43]; (f) Li et al.^[44]introduced FPEAI to vertically arrange the (MAPbI₃)_0.75(FASnI₃)_0.25 grain height and the J-V curve of unused and used FPEAI devices.

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图 5 (a) AMX₃型钙钛矿材料常用元素组分及不同组分的材料性质^[45]; (b) FA⁺掺入对MA_1–yFA_yPb_0.75Sn_0.25I₃钙钛矿器件稳定性的影响^[49]; (c)由计算和实验所得的MASn_1–xPb_xI₃带隙随x的变化^[6]; (d)不同Sn-Pb比例的FA_0.66MA_0.34Pb_1–xSn_xI₃钙钛矿的XRD图谱^[24]; (e) Br含量分别为0, 6%和16%的Sn-Pb钙钛矿太阳电池的暗态J-V曲线^[53]; (f)未掺入Cl和掺入2.5% Cl对钙钛矿薄膜的SEM扫描图^[30]; (g)掺入不同比例(0, 15%, 25%, 40%)MASCN对薄膜钙钛矿薄膜的SEM顶部扫描图及横截面扫描图^[54]

Fig. 5. (a) The commonly used element compositions and their properties of AMX₃^[45]; (b) FA⁺-doping effects to the stability of MA_1–yFA_yPb_0.75Sn_0.25I₃ perovskite devices^[49]; (c) the band gap variation with x changes of MASn_1–xPb_xI₃ obtained from calculations and experiments^[6]; (d) XRD patterns of FA_0.66MA_0.34Pb_1–xSn_xI₃ perovskites with different Sn-Pb ratios^[24]; (e) dark J-V curves of Sn-Pb perovskite solar cells with Br concentrations of 0, 6% and 16% respectively^[53]; (f) SEM images of perovskite films without Cl and with 2.5% Cl^[30]; (g) the top and cross-section SEM images of perovskite films mixed with 0, 15%, 25%, 40% of MASCN^[54].

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图 6 (a)两步顺序沉积结合DMSO溶剂蒸气处理的方式制备MASn_0.1Pb_0.9I₃的过程示意图^[59]; (b)两步顺序沉积FA_0.66MA_0.34Pb_0.5Sn_0.5I₃的过程示意及原位吸收光谱图^[24]

Fig. 6. (a) The schematic diagram of the two-step sequential depositions combined with DMSO solvent vapor treatment method to prepare MASn_0.1Pb_0.9I₃ perovskite films^[59]; (b) the schematic diagram of the two-step sequential deposition process of FA_0.66MA_0.34Pb_0.5Sn_0.5I₃ and in-situ absorption spectra^[24].

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图 7 (a)真空辅助热退火结合一步溶液法制备的器件结构及原理示意图^[60]; (b)使用/不使用真空辅助热退火所制备的薄膜形貌顶部SEM图^[60]; (c)真空辅助生长(VAGC)方法的原理示意图及横截面SEM图像^[61]; (d)双源共蒸法制备FA_1–xCs_xSn_1–yPb_yI₃钙钛矿薄膜过程示意图及晶体结构示意图^[62]

Fig. 7. (a) Device architecture and schematic diagram that combined the vacuum-assisted thermal annealing process and one-step solution method^[60]; (b) the top SEM images of the film prepared with/without vacuum-assisted thermal annealing^[60]; (c) the schematic diagram and cross-section SEM image of the film prepared by VAGC method^[61]; (d) the schematic diagram and crystal structure of FA_1–xCs_xSn_1–yPb_yI₃ perovskite films prepared by dual-source co-evaporation method^[62].

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图 8 (a)不同DMSO/DMF溶剂比的Sn-Pb钙钛矿反应机理示意图^[56]; (b) MAPb_1–xSn_xI₃(0 ≤ x ≤ 1)薄膜的形成机理以及相应的晶体结构示意图^[64]; (c)在不同偏置电压下未掺杂及掺杂C₆₀的MAPb_0.75Sn_0.25I₃钙钛矿器件的本体复合寿命和表面复合寿命^[65]

Fig. 8. (a) The mechanism diagram of Sn-Pb perovskite reactions with different DMSO/DMF solvent ratio^[56]; (b) the formation mechanisms of MAPb_1–xSn_xI₃ (0 ≤ x ≤ 1) film and corresponding crystal structures^[64]; (c) bulk recombination life and surface recombination life of MAPb_0.75Sn_0.25I₃ perovskite devices with or without C₆₀-doped under different amplitude voltages^[65].

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图 9 (a)含GABr的FA_0.7MA_0.3Pb_0.7Sn_0.3I₃表面的电荷密度分布图(等电势为0.03 eÅ^–3)以及未添加与添加12%的GABr的钙钛矿SEM扫描图^[66]; (b)添加CdI₂的1.22 eV窄带隙钙钛矿与1.80 eV宽带隙钙钛矿叠层太阳电池的结构示意图和SEM横截面扫描图^[68]; (c) (4AMP)²⁺, 哌嗪离子和PEA⁺阳离子的结构式及用(4AMP)I₂, 碘化哌嗪和PEAI表面处理的CsPb_0.6Sn_0.4I₃钙钛矿太阳电池的J-V曲线^[67]

Fig. 9. (a) The charge density distribution on the FA_0.7MA_0.3Pb_0.7Sn_0.3I₃ surface containing GABr (the isopotential is 0.03 eÅ^–3) and the SEM images of the perovskite without and with 12% GABr^[66]; (b) structure diagram and cross-section SEM inage of 1.22 eV narrow-bandgap perovskite with CdI₂ added and 1.80 eV wide-bandgap perovskite tandem solar cell^[68]; (c) structure of(4AMP)²⁺, piperazine ion and PEA⁺ and J-V curves of CsPb_0.6Sn_0.4I₃ perovskite solar cell that absorber film surface treated with (4AMP)I₂, piperazine iodide and PEAI, respectively^[67].

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图 10 (a) Kapil等^[69]对比传统无PCBM层和带PCBM层的电荷提取和复合过程示意图, τ_r表示从FAMA到C₆₀的载流子注入时间; (b)添加DF-C₆₀形成的梯度异质结(GHJ)结构示意图^[72]; (c)在NiO_x及PEDOT:PSS上沉积钙钛矿膜的SEM顶部扫描图及截面扫描图^[27]; (d)使用BHJ PBDB-T:ITIC中间层形成的逐步升高的HOMO能级结构示意图^[82]; (e) S-乙酰硫代胆碱氯化物分子锚定在缺陷部位的示意图, 其中红色、黄色和蓝色符号分别代表S-乙酰硫代胆碱氯化物分子中的O原子、S原子和N原子^[71]

Fig. 10. (a) The diagram of Kapil et al^[69]. compared the traditional charge extraction and recombination process without and with PCBM, τ_r represents the carrier injection time from FAMA to C₆₀; (b) the schematic diagram of the gradient heterojunction (GHJ) with DF-C₆₀^[72]; (c) the top and cross-section SEM images of the perovskite films deposited on NiO_x and PEDOT:PSS^[27]; (d) the schematic diagram of the gradually increasing HOMO energy level structure formed by BHJ PBDB-T:ITIC intermediate layer^[82]; (e) the schematic diagram of the S-acetylthiocholine chloride molecule anchored at the defect sites, where the red, yellow and blue symbols represent the O atom, S atom and N atom in the acetylthiocholine chloride molecule, respectively^[71].

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表 A1 P-I-N型Sn-Pb钙钛矿太阳电池性能统计

Table A1. Statistics of P-I-N type tin-lead perovskite solar cells performance

Year	Perovskite	Device structure	Eg/eV	V_OC/V	J_SC/(mA·cm^–2)	FF/%	PCE/(%)	Ref.
2016	MA_0.5FA_0.5Pb_0.75Sn_0.25I₃	ITO/PEDOT:PSS/PVK/PCBM/Bis-C₆₀/Ag	1.33	0.78	23.03	79	14.19	[49]
2016	(FASnI₃)_0.6(MAPbI₃)_0.4	ITO/PEDOT:PSS/PVK/C₆₀/BCP/Ag	1.25	0.795	26.86	70.6	15.08	[26]
2017	MA_0.5FA_0.5Pb_0.5Sn_0.5I₃	ITO/PEDOT:PSS/PVK/PCBM/Bis-C₆₀/Ag	1.2	0.78	25.69	70	14.01	[38]
2017	MAPb_0.5Sn_0.5I₃	ITO/PEDOT:PSS/PVK-DF-C₆₀/ICBA/Bis-C₆₀/Ag	1.22	0.87	26.1	69	15.61	[72]
2018	(t-BUA)₂(FA_0.85Cs_0.15)_n–1 Pb_0.6Sn_0.4)_nI_3n+1	ITO/PEDOT:PSS/2 D-PVK/PCBM/BCP/Ag	1.24	0.70	24.2	63	10.6	[43]
2018	FA_0.6MA_0.4Sn_0.6Pb_0.4I₃	ITO/PFI-(PEDOT:PSS)/PVK/PCBM/BCP/Ag	1.22	0.784	27.22	74.36	15.85	[81]
2018	(FAPbI₃)_0.7(CsSnI₃)_0.3	ITO/PEDOT:PSS/PVK/C₆₀/BCP/Al	1.3	0.74	25.89	81.4	15.6	[36]
2018	(FASnI₃)_0.6(MAPbI₃)_0.34(MAPbBr₃)_0.06	ITO/PEDOT:PSS/PVK/C₆₀/BCP/Ag	1.272	0.888	28.72	74.6	19.03	[53]
2018	(FASnI₃)_0.6(MAPbI₃)_0.4	ITO/PEDOT:PSS/PVK/C₆₀/BCP/Ag	1.25	0.841	29.0	74.4	18.1	[30]
2018	FAPb_0.7Sn_0.3I₃	ITO/PEDOT:PSS/PVK/PEAI/PC₆₁BM/BCP/Ag	1.34	0.78	26.46	79	16.26	[54]
2018	FAPb_0.75Sn_0.25I₃	ITO/NiO_X/PVK/PC₆₀BM/BCP/Ag	1.36	0.81	28.23	75.4	17.25	[27]
2018	(FASnI₃)_0.6(MAPbI₃)_0.4	ITO/PEDOT:PSS/PBDBT:ITIC/PVK/C₆₀/BCP/Ag	1.25	0.86	27.92	75.1	18.03	[82]
2019	FA_0.8MA_0.2Sn_0.5Pb_0.5I₃	ITO/PEDOT:PSS/PVK/PCBM/BCP/Ag	1.27	0.81	30	75	18.2	[61]
2019	(FAPb_0.6Sn_0.4I₃)_0.85(MAPb_0.6Sn_0.4Br₃)_0.15	ITO/PEDOT:PSS/PVK/PCBM/BisC₆₀/Ag	1.28	0.87	26.45	79.1	18.21	[39]
2019	FA_0.7MA_0.3Pb_0.5Sn_0.5I₃	ITO/PEDOT:PSS/PVK/PC₆₀BM/BCP/Cu	1.22	0.831	31.4	80.8	21.1	[18]
2019	Cs_0.1MA_0.2FA_0.7Pb_0.5Sn_0.5I₃	ITO/NiO_X/PVK/C₆₀/BCP/Cu	1.2	0.771	31.1	73.3	17.6	[52]
2019	FA_0.75Cs_0.25Sn_0.4Pb_0.6I₃	ITO/PVK/C₆₀/BCP/Ag	1.25	0.72	32.59	69.8	16.4	[51]
2019	(FASnI₃)_0.6(MAPbI₃)_0.4	ITO/PEDOT:PSS/PVK/C₆₀/BCP/Ag	1.25	0.834	30.4	80.8	20.5	[55]
2019	Cs_0.1MA_0.2FA_0.7Sn_0.5Pb_0.5I₃	ITO/NiO_X/PVK/C₆₀/BCP/Cu	1.2	0.771	31.1	73.3	17.6	[52]
2020	(MAPbI₃)_0.75(FASnI₃)_0.25	ITO/PEDOT:PSS/PVK/BCP/Ag	1.33	0.79	28.42	78	17.51	[44]
2020	Cs_0.1MA_0.2FA_0.7Pb_0.5Sn_0.5I₃	ITO/PEDOT:PSS/PVK/PCBM/PEIE/Ag	1.25	0.81	30.3	78.9	19.4	[42]
2020	FA_0.83Cs_0.17Pb_0.7Sn_0.3I₃	ITO/PEDOT:PSS/PVK/PCBM/BCP/Ag	1.3	0.82	30.3	78.4	18.1	[9]
2020	FA_0.7MA_0.3Pb_0.7Sn_0.3I₃	ITO/PEDOT:PSS(EMIC)/PVK/S-acetylthiocholine chlorde/C₆₀/BCP/Ag	1.35	1.02	26.61	76	20.63	[66]
2020	FA_0.66MA_0.34Pb_0.5Sn_0.5I₃	ITO/PEDOT:PSS/PVK/C₆₀/BCP/Ag	1.23	0.78	27.8	73	15.8	[54]
2020	FA_0.5MA_0.45Cs_0.05Pb_0.5Sn_0.5I₃	ITO/PEDOT:PSS/PTAA/Cd-PVK/C₆₀/BCP/Cu	1.22	0.85	30.2	79	20.3	[68]
2020	FA_0.7MA_0.3Pb_0.5Sn_0.5I₃	ITO/PEDOT:PSS/PVK/C₆₀/BCP/Cu	1.24	0.85	31.6	80.8	21.7	[4]

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