Effect of Passivation Layer on Trap Assisted Recombination in Inverted Perovskite Solar Cells

Song WANG; You-zheng HOU; Fan ZHANG; Shuai YE; Jun SONG

doi:10.37188/CJL.20210103

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Effect of Passivation Layer on Trap Assisted Recombination in Inverted Perovskite Solar Cells

Device Fabrication and Physics | Updated：2021-07-22

- Effect of Passivation Layer on Trap Assisted Recombination in Inverted Perovskite Solar Cells Enhanced Publication
- Chinese Journal of Luminescence Vol.42, Issue 7, (2021)
- Affiliations：
  
  Key Laboratory of Optoelectronic Devices and Systems, College of Physics and Optoelectronic Engineering, Shenzhen University,Shenzhen,China,518000
- Author bio：
- Funds：
  
  National Natural Science Foundation of China(61804099)
- DOI：10.37188/CJL.20210103 CLC： TM914.4
- Published：01 July 2021，
  
  Received：23 March 2021，
  
  Revised：15 April 2021，
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Song WANG, You-zheng HOU, Fan ZHANG, et al. Effect of Passivation Layer on Trap Assisted Recombination in Inverted Perovskite Solar Cells. [J]. Chinese Journal of Luminescence 42(7):1029-1039(2021)
DOI：

Song WANG, You-zheng HOU, Fan ZHANG, et al. Effect of Passivation Layer on Trap Assisted Recombination in Inverted Perovskite Solar Cells. [J]. Chinese Journal of Luminescence 42(7):1029-1039(2021) DOI： 10.37188/CJL.20210103.

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E-mail: fanzhang@szu.edu.cn", "data": [ { "name": "text", "data": "* Corresponding Author, E-mail: fanzhang@szu.edu.cn" } ] } ], "bio": [ { "lang": "zh", "text": [ "张帆(1990-)，男，山西侯马人，博士，副研究员，2017年于太原理工大学获得博士学位，主要从事高性能钙钛矿太阳能电池的研究。E-mail: fanzhang@szu.edu.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352312&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352317&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352321&type=" } ], "data": [ [ { "name": "text", "data": "张帆" }, { "name": "text", "data": "(1990-)，男，山西侯马人，博士，副研究员，2017年于太原理工大学获得博士学位，主要从事高性能钙钛矿太阳能电池的研究。E-mail: " }, { "name": "text", "data": "fanzhang@szu.edu.cn" } ] ] } ], "email": "fanzhang@szu.edu.cn", "deceased": false }, { "name": [ { "lang": "zh", "surname": "叶", "givenname": "帅", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "YE", "givenname": "Shuai", "namestyle": 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] } ] } ] }, "abstracts": [ { "lang": "zh", "data": [ { "name": "p", "data": [ { "name": "text", "data": "有机-无机卤化铅钙钛矿多晶薄膜太阳能电池在近几年的研究中实现了光电转换效率的快速增长。然而，其多晶结构的活性层导致器件仍然遭受到表面和晶界位置缺陷引起的性能衰减。本研究借助两种有机氢碘酸盐，即苯乙基碘化胺(Phenethylammonium iodide,PEAI)和邻氟苯乙胺碘(2-Fluorophenylethylammonium iodide,o-F-PEAI)，在CH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "NH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿多晶薄膜表面形成钝化层。扫描电子显微镜和原子力显微镜分析结果显示，PEAI和o-F-PEAI处理后的钙钛矿薄膜晶界被钝化层明显填充，表面粗糙度也显著下降。另外，荧光寿命成像分析结果显示钝化后的钙钛矿薄膜具有更多的光子数和更长的荧光寿命。上述结果表明，PEAI和o-F-PEAI诱导的钝化层可以有效抑制多晶薄膜表面和晶界位置的缺陷复合行为。因此，钝化后的倒置结构钙钛矿太阳能电池器件功率转换效率(Power conversion efficiency,PCE)可以达到21%。此外，o-F-PEAI钝化处理后的器件由于氟离子的作用表现出更好的器件稳定性。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "Organic-inorganic lead halide perovskite polycrystalline thin film solar cells have achieved rapid growth in photoelectric conversion efficiency in recent years of research. However, the active layer of its polycrystalline structure causes the device to still suffer performance degradation caused by defects in the surface and grain boundary positions. In this study, two organic salts, namely, phenethylammonium iodide(PEAI) and 2-fluorophenylethylammonium iodide(o-F-PEAI), were used to form a passivation layer on the surface of perovskite film. Scanning electron microscopy(SEM) and atomic force microscopy(AFM) analysis results show that the grain boundaries of the perovskite film treated with PEAI and o-F-PEAI are obviously filled with passivation layer, and the surface roughness is also significantly reduced. In addition, the fluorescence lifetime imaging(FLIM) analysis results show that the passivated perovskite film has more photons and longer fluorescence lifetime. The above results indicate that the passivation layer induced by PEAI and o-F-PEAI can effectively inhibit the composite behavior of defects on the surface and grain boundary of the polycrystalline film. Therefore, the power conversion efficiency(PCE) of the inverted structure perovskite solar cell device after passivation can reach 21%. In addition, the devices after o-F-PEAI passivation show better device stability due to the effect of fluoride ions." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "荧光寿命显微成像" } ], [ { "name": "text", "data": "倒置钙钛矿太阳能电池" } ], [ { "name": "text", "data": "表面钝化" } ], [ { "name": "text", "data": "PEAI" } ], [ { "name": "text", "data": "o-F-PEAI" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "fluorescence-lifetime imaging microscopy" } ], [ { "name": "text", "data": "inverted perovskite solar cell" } ], [ { "name": "text", "data": "surface passivation" } ], [ { "name": "text", "data": "PEAI" } ], [ { "name": "text", "data": "o-F-PEAI" } ] ] } ], "highlights": [], "body": [ { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "1　引言" } ], "level": "1", "id": "s1" } }, { "name": "p", "data": [ { "name": "text", "data": "有机-无机卤化铅钙钛矿太阳能电池因为其高吸光系数、低激子结合能、长载流子扩散长度以及快速提高的功率转换效率(Power conversion efficiency,PCE)，而成为光伏领域的热门研究方向" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "1", "type": "bibr", "rid": "R1", "data": [ { "name": "text", "data": "1" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "5", "type": "bibr", "rid": "R5", "data": [ { "name": "text", "data": "5" } ] } } ], "rid": [ "R1", "R2", "R3", "R4", "R5" ], "text": "1-5", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。如今，钙钛矿太阳能电池的短路电流密度(Short circuit current density," }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "SC" } ] }, { "name": "text", "data": ")已经接近材料(1.55 eV的钙钛矿活性层材料)的理论预测极限26 mA·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "，然而器件的开路电压(Open-circuit voltage," }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "OC" } ] }, { "name": "text", "data": ")距离其热力学极限还有很大的进步空间。因此，科研工作者有望通过提高器件的开路电压进一步推动钙钛矿太阳能电池达到自身PCE的预测极限" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "6", "type": "bibr", "rid": "R6", "data": [ { "name": "text", "data": "6" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "9", "type": "bibr", "rid": "R9", "data": [ { "name": "text", "data": "9" } ] } } ], "rid": [ "R6", "R7", "R8", "R9" ], "text": "6-9", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "钙钛矿太阳能电池中，多晶结构的活性层导致器件仍然遭受到表面和晶界位置缺陷引起的性能衰减。为了解决这一问题，一个十分有效的方法就是对活性层的表面缺陷进行钝化处理" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "12", "type": "bibr", "rid": "R12", "data": [ { "name": "text", "data": "12" } ] } } ], "rid": [ "R10", "R11", "R12" ], "text": "10-12", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。研究人员已经提出了一系列的钙钛矿表面改善策略。例如，在钙钛矿表面生长绝缘钝化层，包括聚苯乙烯(Polystyrene,PS)、聚甲基丙烯酸甲酯(Polymethyl methacrylate,PMMA)和聚乙二醇(Polyethylene glycol,PEG)，以抑制表面电荷复合，从而增加器件的开路电压" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } } ], "rid": [ "R13", "R14", "R15" ], "text": "13-15", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。这些绝缘钝化层应有合适的厚度，以允许电子隧穿。还有一些二维钙钛矿薄膜，例如丁铵碘化铅(Butylammonium lead iodide,BA" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": ")和苯乙胺碘化铅(Phenethylammonium lead iodide,PEA" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": ")可以在钙钛矿薄膜表面形成渐变的2D/3D结构，从而钝化钙钛矿活性层表面的缺陷" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "16", "type": "bibr", "rid": "R16", "data": [ { "name": "text", "data": "16" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "17", "type": "bibr", "rid": "R17", "data": [ { "name": "text", "data": "17" } ] } } ], "rid": [ "R16", "R17" ], "text": "16-17", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此外，中科院半导体所的游经碧课题组报道，在混合阳离子钙钛矿表面沉积苯乙基碘化胺(Phenethylammonium iodide, PEAI)有机盐相比于所生成的二维PEA" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": "可以更有效地钝化表面缺陷" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "18", "type": "bibr", "rid": "R18", "data": [ { "name": "text", "data": "18" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。上述研究表明，合适的表面钝化策略可以通过抑制表面缺陷复合，进一步提高钙钛矿太阳能电池的光伏性能。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本研究借助两种有机氢碘酸盐，即 PEAI和邻氟苯乙胺碘(2-Fluorophenylethylammonium iodide,o-F-PEAI)，其结构式如下:PEAI(" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352326&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352335&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352332&type=" } } } ] }, { "name": "text", "data": ")和o-F-PEAI(" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352341&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352352&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352346&type=" } } } ] }, { "name": "text", "data": ")，在CH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "NH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿多晶薄膜表面形成钝化层。研究发现，PEAI和o-F-PEAI处理后的钙钛矿薄膜晶界被钝化层明显填充，表面粗糙度也显著下降。另外，借助荧光寿命成像研究了钙钛矿活性层中的缺陷复合行为。结果显示，两种钝化后的钙钛矿薄膜具有更多的光子数和更长的荧光寿命。这个结果说明，PEAI和o-F-PEAI诱导的钝化层都可以有效抑制多晶薄膜表面和晶界位置的缺陷复合行为。本文基于倒置结构，构建了太阳能电池光伏器件。钝化后的钙钛矿太阳能电池器件都显示出更高的光电转换效率，最高可以达到21%，而且没有电流迟滞效应出现。研究发现，苯环上被单个疏水性氟离子取代后，钙钛矿薄膜有更好的耐湿性和荧光寿命，钝化后器件表现出更好的PCE。最后经过稳定性测试，o-F-PEAI钝化处理后的器件表现出更好的器件稳定性。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2　实验" } ], "level": "1", "id": "s2" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.1　器件制备" } ], "level": "2", "id": "s2a" } }, { "name": "p", "data": [ { "name": "text", "data": "首先，氧化铟锡(Indium tin oxide,ITO)玻璃分别使用去离子水、丙酮、异丙醇进行超声处理15 min。玻璃基底清洗干净后，用压缩空气吹干，然后进行15 min紫外臭氧处理。将5 mg/mL Poly[bis(4-phenyl)(2,4,6-triMethylphenyl)aMine](PTAA)和0.25 mg/mL 2,3,5,6-Tetrafluoro-7,7,8,8-tetracyanoquinodimethane(F4-TCNQ)溶解在氯苯中配制成溶液，然后在ITO表面以转速为4 000 r/min旋涂20 s，并在100 ℃的加热台上退火2 min。将0.5 mg/mL的PMMA溶解在乙酸乙酯中，PMMA溶液在ITO/PTAA-F4-TCNQ表面以6 000 r/min的转速旋涂20 s，然后在100 ℃的加热台上退火1 min。将922 mg 碘化铅(Lead(Ⅱ) iodide,PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")和327.5 mg 甲基碘化胺(Methylammonium iodide,MAI)(量比为1∶1.03)溶解在0.9 mL N,N二甲基甲酰胺(N,N-Dimethylformamide,DMF)和0.1 mL二甲基亚砜(Dimethyl sulfoxide,DMSO)的混合溶剂中，配制成钙钛矿前驱体溶液。把100 μL钙钛矿溶液滴加在ITO/PTAA∶F4-TCNQ/PMMA表面，以6 000 r/min的转速旋涂20 s。在旋涂进行到6~7 s时，把300 μL的仲丁醇清洗反溶剂滴加到湿膜表面，此时薄膜从黄色快速转变成棕黑色。旋涂程序结束后把钙钛矿薄膜在100 ℃下退火1 min。对于PEAI和o-F-PEAI处理的钙钛矿薄膜，在钙钛矿薄膜表面以6 000 r/min、20 s沉积不同浓度PEAI和o-F-PEAI的仲丁醇溶液。钙钛矿薄膜在100 ℃的加热台上退火10 min。" } ] }, { "name": "table", "data": { "id": "T1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "表1" } ], "title": [ { "name": "text", "data": "本工作主要材料和试剂信息" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Tab.1" } ], "title": [ { "name": "text", "data": "Information of materials and reagents used in this work" } ] } ], "note": [], "table": [ { "head": [ [ { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "材料名称" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "规格和纯度" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "厂家" } ] } ] ], "body": [ [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "碘化铅(PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.99%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "TCI" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "甲基胺碘化铅(MAI)" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.8%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "TCI" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "N,N二甲基甲酰胺(DMF)" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.5%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "Sigma-Aldrich" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "二甲基亚砜(DMSO)" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.5%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "Sigma-Aldrich" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "氯苯(CB)" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "Sigma-Aldrich" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "o-F-PEAI" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.99%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "西安宝莱特" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "PEAI" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.99%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "西安宝莱特" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "仲丁醇(2-butanol)" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.5%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "Sigma-Aldrich" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "乙酸乙酯" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.5%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "Sigma-Aldrich" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "乙醇" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.5%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "Sigma-Aldrich" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "F4-TCNQ" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.5%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "Nichem" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "Bphen" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.5%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "Nichem" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "PTAA" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.5%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "Nichem" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "PMMA" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "99.5%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "TCI" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "left", "style": "border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "PCBM" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "style": "border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "99.5%" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "style": "border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "Nichem" } ] } ] ], "foot": [] } ], "graphics": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352363&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352357&type=" } } }, { "name": "p", "data": [ { "name": "text", "data": "接着在钙钛矿薄膜表面以2 500 r/min和6 000 r/min旋涂[6,6]-phenyl-C61-butyric acid methyl ester(PCBM)(20 mg/mL，氯苯)和4,7-Diphenyl-1,10-phenanthroline(Bphen)(0.7 mg/mL，乙醇)薄膜。上述薄膜制备过程全部在氮气手套箱中完成。最后，使用真空蒸镀100 nm金属铝作为钙钛矿太阳能电池的阴极。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.2　样品表征" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "我们使用太阳光模拟器(Zolix Sirius-SS)提供测试光源，利用标准硅太阳能电池(ABET technology)进行校准光源强度，使用数字源表(keithley2400)测量电池器件的" }, { "name": "italic", "data": [ { "name": "text", "data": "J-V" } ] }, { "name": "text", "data": "特性曲线，包括正反扫" }, { "name": "italic", "data": [ { "name": "text", "data": "J-V" } ] }, { "name": "text", "data": "特性曲线以及稳态曲线。外量子效率(External quantum efficiency, EQE)曲线使用实验室自制设备测试。我们使用分光仪(卓立汉光，Omni-" }, { "name": "italic", "data": [ { "name": "text", "data": "λ" } ] }, { "name": "text", "data": "300)把太阳能光模拟器(Zolix Sirius-SS)的光源进行分光，得到300~850 nm单色光。通过数字源表(keithley2400)采集数据。钙钛矿太阳能电池的有效面积为0.06 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "。以上所有测试均在湿度大约60%的超净环境中进行。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "钙钛矿薄膜表面形貌使用德国Zeiss Supra 55扫描电子显微镜(Scanning electron microscope, SEM)和美国布鲁克的原子力显微镜(Atomic force microscope,AFM)测量。钙钛矿薄膜的X射线衍射谱使用日本Rigaku的X射线衍射仪(X-ray diffraction,XRD)测得。荧光寿命成像使用德国Becker&Hickl GmbH荧光寿命成像显微镜(Fluorescence-lifetime imaging microscopy,FLIM)测试。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3　结果与讨论" } ], "level": "1", "id": "s3" } }, { "name": "p", "data": [ { "name": "xref", "data": { "text": "图1(a)~(c)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(a)~(c)" } ] } }, { "name": "text", "data": "为未经钝化(control)、经PEAI(0.5 mg/mL)和o-F-PEAI(0.5 mg/mL)处理后的钙钛矿薄膜表面SEM形貌图。未经过钝化处理的钙钛矿薄膜显示出致密且无针孔的形态，同时钙钛矿晶粒粗大且有明显的晶界;经过PEAI和o-F-PEAI盐覆盖的钙钛矿薄膜显示出比未经处理更加致密光滑的表面形貌，且晶界更不明显。为了进一步了解以上不同类型的钙钛矿薄膜晶体特性，我们统计了钙钛矿薄膜晶粒的尺寸大小(" }, { "name": "xref", "data": { "text": "图1(d)~(f)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(d)~(f)" } ] } }, { "name": "text", "data": ")，结果显示未经过处理的钙钛矿薄膜晶粒平均尺寸是(411.7±166.5) nm，经过PEAI处理的为(284.5±129.6) nm，经过o-F-PEAI的为(293.7±139.0) nm。钝化层的加入导致钙钛矿晶粒尺寸有所下降。在钙钛矿上旋涂PEAI和o-F-PEAI，它们经过共同后退火处理。退火过程是钙钛矿晶粒长大过程，然而，PEAI和o-F-PEAI会沉积在钙钛矿薄膜晶界位置。虽然明显填补了晶界，但是不可避免地会阻碍晶粒生长变大。值得庆幸的是，从3种钙钛矿薄膜截面SEM图中发现(" }, { "name": "xref", "data": { "text": "图1(h)~(g)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(h)~(g)" } ] } }, { "name": "text", "data": ")，薄膜纵向没有明显的晶粒增加。也就是说，光生载流子可以在单个晶粒中生成、传输和被传输层收集，不用经过晶界的阻隔，这是钙钛矿太阳能电池高性能的基础。而钝化晶粒尺寸减小所导致的晶界数量增加，也会被钝化层填补和覆盖。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "对照组((a)、(b)、(h))、PEAI处理((b)、(e)、(i))和o-F-PEAI处理((c)、(f)、(g))后钙钛矿薄膜的表面形貌图、晶粒尺寸统计直方图和截面形貌图。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.1" } ], "title": [ { "name": "text", "data": "Top-view SEM images, grain sizes distribution, and cross-section SEM images of control ((a), (b), (h)), PEAI((b), (e), (i)), and o-F-PEAI((c), (f), (g)) treated perovskite films, respectively." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352367&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352372&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352369&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "为了进一步说明这个问题，我们进行了AFM测试。" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "是3种钙钛矿薄膜的表面AFM图。从" }, { "name": "xref", "data": { "text": "图2(a)、(d)", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2(a)、(d)" } ] } }, { "name": "text", "data": "可以看到，Control样品的表面起伏最为明显，表面粗糙度同样最大，为9.1 nm。经过PEAI(0.5 mg/mL)和o-F-PEAI(0.5 mg/mL)钝化处理以后，钙钛矿薄膜表面起伏都显著下降，表面粗糙度分别降低为5.0 nm和4.6 nm。我们沿着AFM 二维表面形貌图的划线给出了高度起伏曲线，如" }, { "name": "xref", "data": { "text": "图2(g)", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2(g)" } ] } }, { "name": "text", "data": "所示。Control样品表面起伏很大，尤其是薄膜表面晶界位置的最大起伏高度可以达到60 nm。而PEAI和o-F-PEAI处理后的钙钛矿薄膜最大起伏高度分别只有20 nm和15 nm。实验结果表明，PEAI和o-F-PEAI钝化层可以有效填补钙钛矿晶界，降低表面粗糙度。已有报道显示，不完美的钙钛矿表面和晶界会诱导大量深能级缺陷态，导致器件性能和稳定性下降" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "19", "type": "bibr", "rid": "R19", "data": [ { "name": "text", "data": "19" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，PEAI和o-F-PEAI的钝化处理有望抑制深能级缺陷态的产生。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "(a)~(c)对照组、PEAI处理和o-F-PEAI处理后钙钛矿薄膜的AFM二维表面形貌图;(d)~(f)3种钙钛矿薄膜的AFM三维表面形貌图;(g)3种钙钛矿薄膜的表面高度曲线。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.2" } ], "title": [ { "name": "text", "data": "(a)-(c)2D AFM images of control, PEAI, and o-F-PEAI treated perovskite films, respectively. (d)-(f)3D ADM images of the three kinds of perovskite films. (g)Height profiles of the three kinds of perovskite films" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352376&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352382&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352379&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "接下来借助X射线衍射仪对3种钙钛矿薄膜的晶体结构和成分进行了深入表征。" }, { "name": "xref", "data": { "text": "图3(a)、(b)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(a)、(b)" } ] } }, { "name": "text", "data": "分别是不同浓度PEAI和o-F-PEAI处理后钙钛矿薄膜的X射线衍射图。" }, { "name": "xref", "data": { "text": "图3(c)、(d)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(c)、(d)" } ] } }, { "name": "text", "data": "分别是" }, { "name": "xref", "data": { "text": "图3(a)、(b)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(a)、(b)" } ] } }, { "name": "text", "data": "的细节放大图。所有的样品都在14.5°、28.8° 和32.3°出现3个特别强的衍射峰，分别对应于CH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "NH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿的 [110]、[220]" }, { "name": "text", "data": " 和 [310]衍射峰。在未处理的钙钛矿样品中，在12.5°出现一个不属于钙钛矿的新衍射峰，对应于钙钛矿的前驱体碘化铅(PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")。这个结果说明control钙钛矿薄膜中还存在着未反应的PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "。随着PEAI和o-F-PEAI的覆盖，钙钛矿薄膜中的PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "衍射峰在不断地下降，到浓度为0.5 mg/mL时完全消失。此时，两种钝化处理的钙钛矿薄膜XRD衍射谱中没有出现新的PEAI盐和2D PEA" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": "的衍射峰，还不能判断PEAI和o-F-PEAI与未反应的PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "生成了二维钙钛矿还是维持有机盐本身。通过加大两种有机盐的浓度到5 mg/mL,XRD衍射谱中依然没有新的衍射峰出现，同时钙钛矿110向的衍射峰出现了明显的下降，如" }, { "name": "xref", "data": { "text": "图3(d)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(d)" } ] } }, { "name": "text", "data": "所示，说明3D钙钛矿的含量在减少。上述实验结果说明，PEAI和0-F-PEAI在钙钛矿薄膜表面诱导的钝化层没有形成2D钙钛矿和维持有机盐本身，而是与钙钛矿薄膜中未反应的PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "和[PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "6" } ] }, { "name": "text", "data": "]相结合，生成准二维结构或者非晶的钝化覆盖层，这与Bai等以及我们之前的工作是一致的" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "21", "type": "bibr", "rid": "R21", "data": [ { "name": "text", "data": "21" } ] } } ], "rid": [ "R20", "R21" ], "text": "20-21", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "(a)不同浓度PEAI处理后钙钛矿薄膜的X射线衍射图，左上角为PEAI盐和PEA" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": "的X射线衍射图;(b)不同浓度o-F-PEAI处理后钙钛矿薄膜的X射线衍射图;(c)和(d)分別是(a)和(b)的局部放大图。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.3" } ], "title": [ { "name": "text", "data": "(a)XRD pattern of perovskite films with different PEAI concentration. (b)XRD pattern of perovskite films with different o-F-PEAI concentration. (c), (d)Locally enlarged graphs of (a) and (b), respectively." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352386&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352391&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352389&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "为了研究钝化层对钙钛矿薄膜缺陷复合行为的影响，我们使用荧光寿命显微镜对3种钙钛矿薄膜进行了荧光寿命成像，结果如" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "所示。" }, { "name": "xref", "data": { "text": "图4(a)~(c)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(a)~(c)" } ] } }, { "name": "text", "data": "是3种钙钛矿薄膜的荧光寿命成像结果。图中不同的颜色代表不同的荧光寿命，图片的亮度代表荧光强度。" }, { "name": "xref", "data": { "text": "图4(d)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(d)" } ] } }, { "name": "text", "data": "是3种钙钛矿薄膜的荧光寿命统计直方图，" }, { "name": "xref", "data": { "text": "图4(e)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(e)" } ] } }, { "name": "text", "data": "是代表性的时间分辨荧光衰减曲线。荧光寿命成像技术使用488 nm的脉冲激光作为激发光，在700~800 nm的探测范围，对钙钛矿薄膜进行荧光寿命成像。值得注意的是，钙钛矿在短波长范围具有很强的光吸收强度，因此短波长激发光(488 nm)通常只有100 nm的穿透深度，相比于薄膜厚度相差很多。因此，荧光成像测试主要表征了钝化层对钙钛矿薄膜表面的钝化结果。荧光寿命显微镜通过对荧光信号进行时间分辨单光子计数，得到每个像素点的荧光衰减曲线，如" }, { "name": "xref", "data": { "text": "图4(e)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(e)" } ] } }, { "name": "text", "data": "所示。曲线前1.5 μs 为薄膜荧光的充分激发区域，是为了使脉冲激光充分激发样品，得到更可靠的结果。在激发光撤销后，由于每个荧光分子处于激发态的时间长短不一，所以荧光强度整体呈指数衰减。因此，可以对荧光衰减曲线进行单指数拟合获得荧光寿命:" } ] }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "(a)~(c)对照组、PEAI处理和o-F-PEAI处理后钙钛矿薄膜的荧光寿命成像;(d)3种钙钛矿薄膜荧光寿命统计直方图;(e)3种钙钛矿薄膜单个像素点时间分辨荧光衰减曲线。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.4" } ], "title": [ { "name": "text", "data": "(a)-(c)PL lifetime images of control, PEAI, and o-F-PEAI treated perovskite films, respectively. (d)Statistical histograms of PL lifetimes from FLIM images of the three kinds of perovskite films. (e)Representative PL decay curves of the three kinds of perovskite films." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352392&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352396&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352394&type=" } ] } }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "(1)" } ], "data": [ { "name": "text", "data": " " }, { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352398&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352400&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352401&type=" } } }, { "name": "text", "data": " " }, { "name": "text", "data": " " } ], "id": "DF1" } }, { "name": "p", "data": [ { "name": "text", "data": "其中，当荧光强度衰减为初始强度" }, { "name": "italic", "data": [ { "name": "text", "data": "I" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "的1/e时所用的时间称为荧光寿命" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "text", "data": "，用于表征荧光分子在激发态的平均停留时间，是荧光分子固有的一个特征参数，和发光强度大小无关。根据荧光寿命成像结果可以发现，没有钝化的control样品荧光寿命都集中在250 ns左右，而PEAI(0.5 mg/mL)和o-F-PEAI(0.5 mg/mL)钝化处理后荧光寿命分别增加到340 ns和345 ns左右。此外，" }, { "name": "xref", "data": { "text": "图4(d)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(d)" } ] } }, { "name": "text", "data": "中显示PEAI和o-F-PEAI钝化处理后钙钛矿薄膜中的光子数也有所增加。通常钙钛矿薄膜中的缺陷态是作为载流子非辐射复合中心，导致荧光强度明显下降和寿命显著降低。PEAI和o-F-PEAI钝化处理后的钙钛矿薄膜具有较多的光子数和较长的荧光寿命，说明钙钛矿薄膜中的缺陷态密度有了明显下降，缺陷诱导的光生载流子的非辐射复合行为也因此被钝化层明显抑制。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "为了进一步了解钝化层对钙钛矿太阳能电池光伏性能的影响，构建了倒置结构钙钛矿太阳能电池器件。器件结构如" }, { "name": "xref", "data": { "text": "图5(a)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(a)" } ] } }, { "name": "text", "data": "所示:ITO/PTAA∶F4-TCNQ/PMMA/CH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "NH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "/Passivation layer/PCBM/Bphen/Al，整个器件的SEM截面图显示在" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": "(a)本研究中钙钛矿太阳能电池的器件结构图;(b)PEAI处理后器件的界面SEM图;(c)Control,PEAI,o-F-PEAI处理后性能最高的钙钛矿太阳能电池短路电流密度-电压曲线;(d)3种器件的外量子效率曲线;(e)3种器件的稳态效率输出曲线;(f)3种器件的光伏性能箱式图" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.5" } ], "title": [ { "name": "text", "data": "(a)Schematic representation device structure of the perovskite solar cells. (b)Cross-section SEM image of the full device. (c)" }, { "name": "italic", "data": [ { "name": "text", "data": "J-V" } ] }, { "name": "text", "data": " curves of the best-performing control, PEAI-treated, and o-F-PEAI-treated perovskite solar cells. (d)EQE spectra of the three kinds of perovskite solar cells. (e)Steady-state power output of the three kinds of perovskite solar cells. (e)Box diagram of photovoltaic performance for the three kinds of perovskite solar cells." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352403&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352407&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352405&type=" } ] } }, { "name": "p", "data": [ { "name": "xref", "data": { "text": "图5(b)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(b)" } ] } }, { "name": "text", "data": "。在整个钙钛矿太阳能电池器件中，透明ITO作为器件阳极，PTAA掺杂F4-TCNQ作为器件的空穴传输层，薄层PMMA作为空穴界面钝化层，CH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "NH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "作为器件的活性层，PEAI和o-F-PEAI作为表面钝化层，PCBM作为电子传输层，Bphen作为阴极界面修饰层，最后蒸镀金属铝作为器件的阴极。" } ] }, { "name": "p", "data": [ { "name": "xref", "data": { "text": "图5(c)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(c)" } ] } }, { "name": "text", "data": "是最优性能的Control,PEAI,o-F-PEAI器件的" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "曲线，器件的光伏性能参数汇总在" }, { "name": "xref", "data": { "text": "表2", "type": "table", "rid": "T2", "data": [ { "name": "text", "data": "表2" } ] } }, { "name": "text", "data": "中。未经过处理的Control器件，在正向扫描(或反向扫描)下，具有22.8 mA/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "(22.9 mA/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")的" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "SC" } ] }, { "name": "text", "data": "、1.04 V(1.04 V)的开路电压、0.74(0.77)的填充因子(Fill Factor,FF)以及 17.5%(18.3%)的PCE。Control器件由于较大的表面缺陷浓度，导致" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "迟滞效应存在。使用浓度为0.5 mg/mL的PEAI对钙钛矿薄膜进行处理以后，PEAI器件获得了最佳的光伏性能。正向扫描(或反向扫描)下，PEAI器件的" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "SC" } ] }, { "name": "text", "data": "为23.5 mA/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "(23.6 mA/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")," }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "OC" } ] }, { "name": "text", "data": "为1.15 V(1.15 V),FF为0.78(0.78),PCE为20.9%(21.0%)。使用浓度为0.5 mg/mL的o-F-PEAI对钙钛矿薄膜进行处理以后，o-F-PEAI器件获得了最佳的光伏性能。正向扫描(或反向扫描)下，o-F-PEAI器件的" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "SC" } ] }, { "name": "text", "data": "为23.9 mA/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "(23.7 mA/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")," }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "OC" } ] }, { "name": "text", "data": "为1.15 V(1.15 V),FF为0.77(0.77),PCE为21.1%(21.1%)。十分明显地，PEAI和o-F-PEAI处理以后，器件性能由于表面和晶界位置的缺陷钝化导致器件性能明显提高，同时" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "迟滞效应也被明显抑制。" }, { "name": "xref", "data": { "text": "图5(d)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(d)" } ] } }, { "name": "text", "data": "是3种器件外量子效率曲线，根据外量子效率曲线积分，" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "SC" } ] }, { "name": "text", "data": "分别为22.1,22.6,22.9 mA/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "，这些数值与" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "曲线测量的结果相当吻合。此外，测试了3种器件最大功率点的稳态输出曲线，如" }, { "name": "xref", "data": { "text": "图5(e)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(e)" } ] } }, { "name": "text", "data": "所示。Control器件在持续光照条件下有微弱的性能衰减，从18.6%下降到17.9%。而PEAI和o-F-PEAI钝化后的器件几乎没有性能衰减。钝化后的器件表现出更好的光照稳定性。此外，绘制了3种器件(6个)的" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "OC" } ] }, { "name": "text", "data": "、" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "SC" } ] }, { "name": "text", "data": "、FF和PCE箱式图，如" }, { "name": "xref", "data": { "text": "图5(f)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(f)" } ] } }, { "name": "text", "data": "所示。其结果进一步确认了钝化层对钙钛矿太阳能电池光伏性能的提高作用。" } ] }, { "name": "table", "data": { "id": "T2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "表2" } ], "title": [ { "name": "text", "data": "Control、PEAI、o-F-PEAI处理后性能最高的钙钛矿太阳能电池的光伏性能参数" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Tab.2" } ], "title": [ { "name": "text", "data": "Photovoltaic performance parameters of best-performing control, PEAI treated and o-F-PEAI treated perovskite solar cells" } ] } ], "note": [], "table": [ { "head": [ [ { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "器件" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "方向" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "OC" } ] }, { "name": "text", "data": "/V" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "SC" } ] }, { "name": "text", "data": "/(mA·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": ")" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "FF" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "PCE/%" } ] } ] ], "body": [ [ { "colspan": "1", "rowspan": "2", "align": "center", "data": [ { "name": "text", "data": "Control" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "正向" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "1.04" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "22.8" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "0.74" } ] }, { "colspan": "1", "rowspan": "1", "align": "left", "data": [ { "name": "text", "data": "17.5" } ] } ], [ { 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] ], "foot": [] } ], "graphics": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352411&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352409&type=" } } }, { "name": "p", "data": [ { "name": "text", "data": "更多的光电测试被用于进一步分析钝化层对钙钛矿太阳能电池的器件性能影响。" }, { "name": "xref", "data": { "text": "图6(a)、(b)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(a)、(b)" } ] } }, { "name": "text", "data": "分别显示了3种器件的开路电压与不同光强的响应关系和尼奎斯特曲线。在不同光强度下，测试" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "OC" } ] }, { "name": "text", "data": "响应可以获取器件的理想因子。理想因子与器件中的陷阱辅助重组密切相关，理想因子越靠近1则说明器件的缺陷越少。可以看到未处理的器件理想因子为1.36，明显大于PEAI和o-F-PEAI器件的1.21和1.20。这个结果进一步证实，PEAI和o-F-PEAI钝化处理有效地降低了器件的" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "OC" } ] }, { "name": "text", "data": "损失，说明表面钝化层对提高器件的效率具有重要意义。" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "显示了3种器件的尼奎斯特曲线，测试是在暗态环境加0.9 V的偏压下完成。曲线可以被" }, { "name": "xref", "data": { "text": "图6(b)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(b)" } ] } }, { "name": "text", "data": "上部的等效电路图很好地拟合，从而获得器件的串联电阻和复合电阻。Control,PEAI,o-F-PEAI处理后钙钛矿太阳能电池串联电阻没有出现明显的增大，分别为29.9,31.1,32.0 Ω。而PEAI和o-F-PEAI处理后器件的复合电阻从6.1 kΩ分别增加到7.1 kΩ和7.9 kΩ。复合电阻的提高说明钝化层对器件缺陷诱导的非辐射复合有明显抑制作用。" } ] }, { "name": "fig", "data": { "id": "F6", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图6" } ], "title": [ { "name": "text", "data": "(a)Control,PEAI,o-F-PEAI处理后钙钛矿太阳能电池开路电压与不同光强的响应关系;(b)3种器件的尼奎斯特曲线。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.6" } ], "title": [ { "name": "text", "data": "(a)Open-circuit voltage " }, { "name": "italic", "data": [ { "name": "text", "data": "versus" } ] }, { "name": "text", "data": " light intensity for the control, PEAI treated and o-F-PEAI treated perovskite solar cells. (b)Nyquist plots measured at 0.9 V applied voltage for the three kinds of devices." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352413&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352419&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352416&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "最后，详细研究和分析了3种器件的稳定性。" }, { "name": "xref", "data": { "text": "图7", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7" } ] } }, { "name": "text", "data": "是Control,PEAI,o-F-PEAI处理后钙钛矿太阳能电池的效率随时间衰减曲线。在没有测试时把器件保存在湿度为30%左右的暗箱中，测试时在60%的空气中测试。没有钝化的器件在空气中表现出最差的空气稳定性。由于铝电极的活性很高，在潮湿环境下很快与钙钛矿反应，导致器件快速衰减。因此，Control器件在存放24 h以后剩下自身0.1%的效率。PEAI钝化以后器件表现出更好的环境稳定性，在24 h存储后还拥有自身41%的光电转换效率。这是因为，PEAI盐拥有更长的烷基链，相比于MA" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "离子更为疏水，PEA" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "离子与钙钛矿[PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "6" } ] }, { "name": "text", "data": "]单元之间的范德华相互作用更强" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "22", "type": "bibr", "rid": "R22", "data": [ { "name": "text", "data": "22" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "23", "type": "bibr", "rid": "R23", "data": [ { "name": "text", "data": "23" } ] } } ], "rid": [ "R22", "R23" ], "text": "22-23", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，PEAI器件相比于Control器件表现出更好的环境稳定性。研究还发现，o-F-PEAI钝化处理后的器件，由于氟离子的作用拥有更好的环境稳定性，在24 h存储以后还拥有初始64%的效率，这个结果符合对F元素的预期。因为有报道显示疏水性氟化分子具有疏水特性，可以用于增强钙钛矿的湿度稳定性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "24", "type": "bibr", "rid": "R24", "data": [ { "name": "text", "data": "24" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "26", "type": "bibr", "rid": "R26", "data": [ { "name": "text", "data": "26" } ] } } ], "rid": [ "R24", "R25", "R26" ], "text": "24-26", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。尽管耐湿性还与薄膜质量有关，但对比PEAI和o-F-PEAI钝化处理后的两种质量相似的薄膜时，氟化钝化层比非氟化明显具有更高的湿度稳定性。" } ] }, { "name": "fig", "data": { "id": "F7", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图7" } ], "title": [ { "name": "text", "data": "Control,PEAI,o-F-PEAI处理后钙钛矿太阳能电池的效率随时间衰减曲线，器件保存在温度为25 ℃、湿度为30%的暗箱中。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.7" } ], "title": [ { "name": "text", "data": "Efficiency degradation tracking of the unencapsulated control, PEAI treated, and o-F-PEAI treated perovskite solar cells under 30% relative humidity(RH) at 25 ℃ in a dark chamber." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352421&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352424&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21352423&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4　结论" } ], "level": "1", "id": "s4" } }, { "name": "p", "data": [ { "name": "text", "data": "本研究发现，苯乙基碘化胺(PEAI)和邻氟苯乙胺碘(o-F-PEAI)可以在CH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "NH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿多晶薄膜表面形成钝化层，通过表面覆盖和填补晶界降低钙钛矿薄膜的表面粗糙度。其次，借助荧光寿命成像测试结果，还发现钝化后的钙钛矿薄膜具有更多的光子数和更长的荧光寿命，进一步说明PEAI和o-F-PEAI诱导的钝化层可以有效抑制多晶薄膜表面和晶界位置的缺陷复合行为。基于倒置结构构建了太阳能电池光伏器件。钝化后的钙钛矿太阳能电池器件显示出更高的光电转换效率，最高可以达到21.1%，并且没有电流迟滞效应出现。最后，发现o-F-PEAI中的F离子为钙钛矿薄膜提供了更好的稳定性，因此在24 h存储以后还拥有初始64%的效率。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文专家审稿意见及作者回复内容的下载地址:http://cjl.lightpublishing.cn/thesisDetails#10.37188/CJL.20210103." } ] } ] } ], "footnote": [], "reflist": { "title": [ { "name": "text", "data": "参考文献:" } ], "data": [ { "id": "R1", "label": "[1]", "citation": [ { "lang": "en", "text": [ { "name": "text", "data": "KOJIMA A" }, { "name": "text", "data": ", " }, { "name": "text", "data": "TESHIMA K" }, { "name": "text", "data": ", " }, { "name": "text", "data": "SHIRAI Y" }, { "name": "text", "data": ", " }, { "name": "text", "data": "et al" }, { "name": "text", "data": ". 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