金属离子替换的有机-无机钙钛矿太阳能电池及其迟滞现象
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摘要
注入金属离子替换有机-无机钙钛矿中参与成键的Pb~(2+)可以有效调控其结晶动力学、薄膜形貌和光电特性,因此,通过优化Pb~(2+)替换比例提高钙钛矿太阳能电池性能是当前的研究热点之一.但是, Pb~(2+)替换对器件异常迟滞现象的影响却缺乏深入的研究.本文采用Cd~(2+)替换的MAPbI_3为模型体系,研究了不同Cd~(2+)浓度下MAPbI_3材料性质及其平面异质结光伏器件(结构为ITO/NiO_x/Cd-MAPbI_3/PCBM/Ag)性能的变化趋势.研究结果表明,优化比例(0.5%)的Cd~(2+)可以有效增强材料结晶性、改善薄膜形貌,降低非辐射复合,提高光生载流子寿命,从而大幅提高器件性能.而Cd~(2+)替换比例过高(>2.5%)时,钙钛矿薄膜中不仅会出现相分离阻碍电荷传输,而且其非辐射复合加剧,光生载流子寿命降低,最终导致器件性能下降.与此同时,过量的Cd~(2+)注入还会引起严重的迟滞现象,利用扫描开尔文探针显微镜(SKPM)证实这一现象与钙钛矿薄膜中显著的离子迁移有关.
Due to long carrier diffusion length,high defect tolerance and adjustable absorption spectra,organic-inorganic perovskite with chemical formula of ABX_3(A=CH_3NH_3(MA) or HC(NH_2)_2(FA);M=Pb;X=Cl,Br,I) is one of the most promising candidates for low-cost solar energy harvesting.The power conversion efficiency(PCE) of the perovskite solar cells has experienced skyrocket increasing from 3.8% to over 23% in just 10 years after they showed up,which has already outperformed than that of multicrystalline Si.Based on ab initio calculation,it demonstrates that Pb~(2+),taking part in bonding,is one of the most important factors that determines the crystallization,energy level,charge carrier dynamics as well as film morphology.Thus,a large number of metal ions have been reported to partial substitute Pb~(2+),including isovalent substitution(Sn~(2+),Sr~(2+),Cd~(2+),Ca~(2+),Mn~(2+),Fe~(2+),Co~(2+),Ni~(2+),Cu~(2+),Ba~(2+),Zn~(2+),Se~(2+) and Eu~(2+),etc.)and anisovalent substitution(Cu~+,Na~+,Ag~+,In~(3+),Sb~(3+),Al~(3+) and Bi~(3+),etc.),which improved perovskite properties and device performance significantly.However,the effects of Pb~(2+) substitution on the anomalous hysteresis of perovskite solar cells have not been fully explored yet.In this manuscript,isovalent Cd~(2+) substituted MAPbI_3 was employed as the model system,which excluded the interference of halogen ion defect formation if Pb~(2+) was substituted by isovalent metal ions.It is found that the crystallinity,morphology and photogenerated charge carrier dynamics of MAPbI_3 were tuned with different concentrations of Cd~(2+).When the concentration of Cd~(2+) increased from 0% to 0.5%,the crystallinity and the morphology of perovskite films improved significantly,resulting suppressed non-radiative recombination and increased photogenerated charge carrier lifetime.The PCE of planar heterojunction photovoltaic devices with structure of ITO/NiO_x/Cd-MAPbI_3/PCBM/Ag enhanced from 15.4% to 17.0%.Importantly,there is negligible hysteresis between forward and reverse current density-voltage(J-V)scan at different scan rate of 0.01,0.1 and 1.0 V/s.By further increasing concentration of Cd~(2+)from 1.0% to 5.0%,the crystallinity of perovskite films deteriorated gradually,leading to higher non-radiative recombination and lower photogenerated charge carrier lifetime.The morphology of perovskite films also became worse,i.e.,generated insulate phases and pin-holes,which prohibited charge transport.Even worse,incorporating high concentration of Cd~(2+)(2.5%-5.0%) not only deteriorated the device performance,but also led to serious hysteresis between forward and reverse J-V scan.In order to further understand the hysteresis behavior under high concentration of Cd~(2+),two-pass scanning Kelvin probe microscopy(SKPM) with additional DC bias(V_(bias)) applied in the first-pass topography scan have been employed.It is found that the average surface potential(SP) of the perovskite did not change with V_(bias) under Cd~(2+) concentration of 0% and 0.5%.Interestingly,the average SP of the perovskite changed significantly with V_(bias) under Cd~(2+) concentration of 5.0%,indicating significant ion migration and accumulation.Our work provides a promising way to understand the device performance and hysteresis behavior in metal-substituted perovskite,which benefits the development of perovskite photovoltaic devices,light-emitting diodes,photodetectors etc.with metal ions engineering in future.
Due to long carrier diffusion length,high defect tolerance and adjustable absorption spectra,organic-inorganic perovskite with chemical formula of ABX_3(A=CH_3NH_3(MA) or HC(NH_2)_2(FA);M=Pb;X=Cl,Br,I) is one of the most promising candidates for low-cost solar energy harvesting.The power conversion efficiency(PCE) of the perovskite solar cells has experienced skyrocket increasing from 3.8% to over 23% in just 10 years after they showed up,which has already outperformed than that of multicrystalline Si.Based on ab initio calculation,it demonstrates that Pb~(2+),taking part in bonding,is one of the most important factors that determines the crystallization,energy level,charge carrier dynamics as well as film morphology.Thus,a large number of metal ions have been reported to partial substitute Pb~(2+),including isovalent substitution(Sn~(2+),Sr~(2+),Cd~(2+),Ca~(2+),Mn~(2+),Fe~(2+),Co~(2+),Ni~(2+),Cu~(2+),Ba~(2+),Zn~(2+),Se~(2+) and Eu~(2+),etc.)and anisovalent substitution(Cu~+,Na~+,Ag~+,In~(3+),Sb~(3+),Al~(3+) and Bi~(3+),etc.),which improved perovskite properties and device performance significantly.However,the effects of Pb~(2+) substitution on the anomalous hysteresis of perovskite solar cells have not been fully explored yet.In this manuscript,isovalent Cd~(2+) substituted MAPbI_3 was employed as the model system,which excluded the interference of halogen ion defect formation if Pb~(2+) was substituted by isovalent metal ions.It is found that the crystallinity,morphology and photogenerated charge carrier dynamics of MAPbI_3 were tuned with different concentrations of Cd~(2+).When the concentration of Cd~(2+) increased from 0% to 0.5%,the crystallinity and the morphology of perovskite films improved significantly,resulting suppressed non-radiative recombination and increased photogenerated charge carrier lifetime.The PCE of planar heterojunction photovoltaic devices with structure of ITO/NiO_x/Cd-MAPbI_3/PCBM/Ag enhanced from 15.4% to 17.0%.Importantly,there is negligible hysteresis between forward and reverse current density-voltage(J-V)scan at different scan rate of 0.01,0.1 and 1.0 V/s.By further increasing concentration of Cd~(2+)from 1.0% to 5.0%,the crystallinity of perovskite films deteriorated gradually,leading to higher non-radiative recombination and lower photogenerated charge carrier lifetime.The morphology of perovskite films also became worse,i.e.,generated insulate phases and pin-holes,which prohibited charge transport.Even worse,incorporating high concentration of Cd~(2+)(2.5%-5.0%) not only deteriorated the device performance,but also led to serious hysteresis between forward and reverse J-V scan.In order to further understand the hysteresis behavior under high concentration of Cd~(2+),two-pass scanning Kelvin probe microscopy(SKPM) with additional DC bias(V_(bias)) applied in the first-pass topography scan have been employed.It is found that the average surface potential(SP) of the perovskite did not change with V_(bias) under Cd~(2+) concentration of 0% and 0.5%.Interestingly,the average SP of the perovskite changed significantly with V_(bias) under Cd~(2+) concentration of 5.0%,indicating significant ion migration and accumulation.Our work provides a promising way to understand the device performance and hysteresis behavior in metal-substituted perovskite,which benefits the development of perovskite photovoltaic devices,light-emitting diodes,photodetectors etc.with metal ions engineering in future.
引文
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2 Dong Q,Fang Y,Shao Y,et al.Electron-hole diffusion lengths>175μm in solution-grown CH3NH3PbI3single crystals.Science,2015,347:967-970
3 Yin W J,Shi T,Yan Y.Unique properties of halide perovskites as possible origins of the superior solar cell performance.Adv Mater,2014,26:4653-4658
4 Protesescu L,Yakunin S,Bodnarchuk M I,et al.Nanocrystals of cesium lead halide perovskites(CsPbX3,X=Cl,Br,and I):Novel optoelectronic materials showing bright emission with wide color gamut.Nano Lett,2015,15:3692-3696
5 Kojima A,Teshima K,Shirai Y,et al.Organometal halide perovskites as visible-light sensitizers for photovoltaic cells.J Am Chem Soc,2009,131:6050-6051
6 Liu M,Johnston M B,Snaith H J.Efficient planar heterojunction perovskite solar cells by vapour deposition.Nature,2013,501:395-398
7 Chen Q,Zhou H,Hong Z,et al.Planar heterojunction perovskite solar cells via vapor-assisted solution process.J Am Chem Soc,2014,136:622-625
8 Jeon N J,Noh J H,Kim Y C,et al.Solvent engineering for high-performance inorganic-organic hybrid perovskite solar cells.Nat Mater,2014,13:897-903
9 Chen L,Tang F,Wang Y,et al.Facile preparation of organometallic perovskite films and high-efficiency solar cells using solid-state chemistry.Nano Res,2015,8:263-270
10 Chen W,Wu Y,Yue Y,et al.Efficient and stable large-area perovskite solar cells with inorganic charge extraction layers.Science,2015,350:944-948
11 Yang Y M,Chen Q,Hsieh Y T,et al.Multilayer transparent top electrode for solution processed perovskite/Cu(In,Ga)(Se,S)2four terminal tandem solar cells.ACS Nano,2015,9:7714-7721
12 Wang Z K,Gong X,Li M,et al.Induced crystallization of perovskites by a perylene underlayer for high-performance solar cells.ACS Nano,2016,10:5479-5489
13 Li Z A,Zhu Z,Chueh C C,et al.Rational design of dipolar chromophore as an efficient dopant-free hole-transporting material for perovskite solar cells.J Am Chem Soc,2016,138:11833-11839
14 Jiang Q,Zhang L Q,Wang H L,et al.Enhanced electron extraction using SnO2high-efficiency planar-structure HC(NH2)2PbI3-based perovskite solar cells.Nat Energy,2016,2:1-7
15 Li Z,Zhu Z,Chueh C C,et al.Facile thiol-ene thermal crosslinking reaction facilitated hole-transporting layer for highly efficient and stable perovskite solar cells.Adv Energy Mater,2016,6:1601165
16 Wu Y,Yang X,Chen W,et al.Perovskite solar cells with 18.21%efficiency and area over 1 cm2fabricated by heterojunction engineering.Nat Energy,2016,1:16148
17 Chen H,Ye F,Tang W T,et al.A solvent-and vacuum-free route to large-area perovskite films for efficient solar modules.Nature,2017,550:92-95
18 Wu C C,Sun W H,Chen Z J,et al.Large-area thin film deposition technologies for fabricating hybrid perovskite solar cells(in Chinese).Chin Sci Bull,2017,62:1457-1463[吴存存,孙伟海,陈志坚,等.钙钛矿太阳能电池的大面积成膜方法.科学通报,2017,62:1457-1462]
19 Li Y Q,Zhu N,Liu G H,et al.Perovskite solar cells fabricated by flash method(in Chinese).Chin Sci Bull,2018,63:2167-2172[李英强,朱宁,刘罡宏,等.基于闪蒸法制备平面钙钛矿光伏器件.科学通报,2018,63:2167-2172]
20 Xu G,Xue R,Chen W,et al.New strategy for two-step sequential deposition:incorporation of hydrophilic fullerene in second precursor for highperformance p-i-n planar perovskite solar cells.Adv Energy Mater,2018,8:1703054
21 Zhu Z,Zhao D,Chueh C C,et al.Highly efficient and stable perovskite solar cells enabled by all-crosslinked charge-transporting layers.Joule,2018,2:168-183
22 Wang P,Jiang Q,Zhao Y,et al.Synergistic improvement of perovskite film quality for efficient solar cells via multiple chloride salt additives.Sci Bull,2018,63:726-731
23 Mosconi E,Amat A,Nazeeruddin M K,et al.First-principles modeling of mixed halide organometal perovskites for photovoltaic applications.JPhys Chem C,2013,117:13902-13913
24 Umari P,Mosconi E,De Angelis F.Relativistic GW calculations on CH3NH3PbI3and CH3NH3SnI3perovskites for solar cell applications.Sci Rep,2014,4:4467
25 Rajagopal A,Liang P W,Chueh C C,et al.Defect passivation via a graded fullerene heterojunction in low-bandgap Pb-Sn binary perovskite photovoltaics.ACS Energy Lett,2017,2:2531-2539
26 Xu G,Bi P,Wang S,et al.Integrating ultrathin bulk-heterojunction organic semiconductor intermediary for high-performance low-bandgap perovskite solar cells with low energy loss.Adv Funct Mater,2018,28:1804427
27 Lyu M,Zhang M,Cooling N A,et al.Highly compact and uniform CH3NH3Sn0.5Pb0.5I3films for efficient panchromatic planar perovskite solar cells.Sci Bull,2016,61:1558-1562
28 Yang Z,Rajagopal A,Jen A K Y.Ideal bandgap organic-inorganic hybrid perovskite solar cells.Adv Mater,2017,29:1704418
29 Pérez-Del-Rey D,Forgács D,Hutter E M,et al.Strontium insertion in methylammonium lead iodide:Long charge carrier lifetime and high fillfactor solar cells.Adv Mater,2016,28:9839-9845
30 Williams S T,Rajagopal A,Jo S B,et al.Realizing a new class of hybrid organic-inorganic multifunctional perovskite.J Mater Chem A,2017,5:10640-10650
31 Jahandar M,Heo J H,Song C E,et al.Highly efficient metal halide substituted CH3NH3I(PbI2)1-x(CuBr2)xplanar perovskite solar cells.Nano Energy,2016,27:330-339
32 Zhang H,Shang M,Zheng X,et al.Ba2+doped CH3NH3PbI3to tune the energy state and improve the performance of perovskite solar cells.Electrochim Acta,2017,254:165-171
33 Chen R,Hou D,Lu C,et al.Zinc ion as effective film morphology controller in perovskite solar cells.Sustain Energy Fuels,2018,2:1093-1100
34 Wu X,Li H,Wang K,et al.CH3NH3Pb1-xEuxI3mixed halide perovskite for hybrid solar cells:The impact of divalent europium doping on efficiency and stability.RSC Adv,2018,8:11095-11101
35 Abdi-Jalebi M,Dar M I,Sadhanala A,et al.Impact of monovalent cation halide additives on the structural and optoelectronic properties of CH3NH3PbI3perovskite.Adv Energy Mater,2016,6:1502472
36 Chen Q,Chen L,Ye F,et al.Ag-incorporated organic-inorganic perovskite films and planar heterojunction solar cells.Nano Lett,2017,17:3231-3237
37 Wang Z K,Li M,Yang Y G,et al.High efficiency Pb-In binary metal perovskite solar cells.Adv Mater,2016,28:6695-6703
38 Zhang J,Shang M,Wang P,et al.n-Type doping and energy states tuning in CH3NH3Pb1-xSb2x/3I3perovskite solar cells.ACS Energy Lett,2016,1:535-541
39 Wang J T W,Wang Z,Pathak S,et al.Efficient perovskite solar cells by metal ion doping.Energy Environ Sci,2016,9:2892-2901
40 Yun J S,Seidel J,Kim J,et al.Critical role of grain boundaries for ion migration in formamidinium and methylammonium lead halide perovskite solar cells.Adv Energy Mater,2016,6:1600330
41 Luo D,Yang W,Wang Z,et al.Enhanced photovoltage for inverted planar heterojunction perovskite solar cells.Science,2018,360:1442-1446
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