氧化锆间隔层的低温喷涂制备...太阳能电池应用性能(英文)_张万文.pdf
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1、第 38 卷 第 2 期 无 机 材 料 学 报 Vol.38 No.2 2023 年 2 月 Journal of Inorganic Materials Feb.,2023 Received date:2022-03-21;Revised date:2022-07-21;Published online:2022-08-04 Foundation item:National Natural Science Foundation of China(52162020);Jiangxi Provincial Natural Science Foundation(20202BABL203012);
2、Jiangxi Province Key Laboratory of Synthetic Chemistry(202005)Biography:ZHANG Wanwen(1994),male,Master candidate.E-mail: 张万文(1994),男,硕士研究生.E-mail: Corresponding author:LUO Jianqiang,professor.E-mail:;YANG Songwang,professor.E-mail: 罗建强,教授.E-mail:;杨松旺,研究员.E-mail: Article ID:1000-324X(2023)02-0213-06
3、DOI:10.15541/jim20220155 Zirconia Spacer:Preparation by Low Temperature Spray-coating and Application in Triple-layer Perovskite Solar Cells ZHANG Wanwen1,LUO Jianqiang1,LIU Shujuan1,MA Jianguo1,ZHANG Xiaoping1,YANG Songwang2(1.Jiangxi Province Key Laboratory of Synthetic Chemistry,East China Univer
4、sity of Technology,Nanchang 330013,China;2.CAS Key Laboratory of Materials for Energy Conversion,Shanghai Institute of Ceramics,Chinese Academy of Sciences,Shanghai 201899,China)Abstract:Perovskite solar cells(PSCs)with structure of TiO2/ZrO2/carbon triple-layer are attractive recently because of th
5、eir inexpensive raw materials,scalable fabrication process,and outstanding stability.But little progress has been made in the low temperature fabrication of TiO2/ZrO2/carbon triple-layer structured PSCs.A major reason is that it is rather difficult to construct the ZrO2 spacer layer at low temperatu
6、re.Herein,we report a facile low-temperature spray-coating method to prepare effective ZrO2 spacer layer in TiO2/ZrO2/carbon triple-layer PSCs using urea to tune the porosity.After optimizing the amount of urea and the thickness of zirconia to 1100 nm,power conversion efficiencies(PCE)of 14.7%for a
7、single cell and 10.8%for a module with 5 cells connected in series(50.9 cm 2.5 cm)were achieved.Furthermore,the PSCs could be stable for 200 d at constant temperature(25)and humidity(40%).With this spray coating method,the zirconia layer on flexible substrate can endure 50 times of bending without a
8、ny cracking.Compared to the conventional screen-printing method of ZrO2 spacer layer,the spray-coating alternative developed in this work shows advantages of more convenient to process,preparation under lower temperature,and compatibility to flexible substrate.Key words:perovskite solar cell;triple-
9、layer structure;low-temperature;zirconia;spray-coating Perovskite solar cells(PSCs),firstly reported by Miyasaka,et al.1 in 2009,has drawn tremendous atten-tions2-5.After years of intensive studies,PSCs showed great improvements on both power conversion efficiency(PCE)and stability6-9.PSCs are gener
10、ally composed of the electron transporting layer,the perovskite light-absorbing layer,the hole transporting layer and two contact electrodes.Several architectures of PSCs were developed,such as fully-printable triple-layer PSCs,planar and inverted structured PSCs10-14.Among them,the fully-printable
11、TiO2/ZrO2/carbon triple-layer PSCs own advantages of inexpensive raw materials,scalable fabrication process,and outstanding stability15-17.How-ever,TiO2/ZrO2/carbon triple-layer PSCs requires deli-cate steps to fabricate screen printable pastes of TiO2,ZrO2 and carbon,including addition of organic a
12、dditives,adjustment of viscosity,homogenization,etc.The pastes were then screen printed sequentially on substrate,and high temperature calcination is necessary to remove the organics.The high temperature process is incompatible with plastic flexible substrate,limiting the potential app-lication of t
13、he TiO2/ZrO2/carbon triple-layer PSCs.In the PSCs research community,flexible substrate-compatible fabrication process is appealing18-19.In this context,a number of techniques were developed for building flexible planar or inverted structured PSCs,including sputtering,evaporation,low-temperature sin
14、te-ring20-24.But none of these methods are applicable to fabricate the TiO2/ZrO2/carbon triple-layer flexible PSCs.Chemical sintering of mesoporous titania layer at low-temperature were widely reported in dye-sensitized solar cells25.Recently,a low temperature method was developed to fabricate the c
15、arbon layer26.However,it is still challenging to fabricate the ZrO2 layer at low temperature for triple-layer PSCs.In order to assemble flexible triple-layer PSCs,a low-214 无 机 材 料 学 报 第 38 卷 temperature method to fabricate ZrO2 layer is necessary.In this work,a facile spray coating method was devel
16、oped to fabricate porous ZrO2 layer for TiO2/ZrO2/carbon triple-layer PSCs at low temperature using urea as poro-sity adjustor,which was well-compatible with flexible substrates,and easier to be scaled up than the conven-tional screen-printing method.1 Experimental 1.1 Materials Lead(II)iodide(PbI2,
17、99%),methylammonium iodide(MAI,99%),anhydrous N,N-dimethylformamide(DMF),titanium diisopropoxide bis(acetylace tonate)(75%in isopropanol),isopropanol,urea,SrCl2 were purchased from Sigma-Aldrich.Zirconia was purchased from Aladdin.All chemicals were used as-received without further purification.1.2
18、Perovskite solution The perovskite solution was made by dissolving 0.159 g MAI,0.461 g PbI2 and 16 mg SrCl2 in 1 mL DMF.1.3 Zirconia ink for spray coating 0.5 g of ZrO2 powder was dispersed in a mixed solu-tion containing 5 mL H2O and 5 mL isopropanol by soni-fication for 3 h.Urea was then added int
19、o the solution with w(ZrO2):w(urea)=2:1.1.4 Titania,zirconia and carbon pastes for screen-printing Titania,zirconia and carbon pastes were prepared according to the previous report27.Typically,1 g powder was dispersed in 20 mL ethanol under sonification.0.5 g ethyl cellulose was dissolved in 4.5 g e
20、thanol and 5 g terpineol.They were mixed together and then homoge-nized with ultra-sonification and ball milling for 10 h.Finally,ethanol was removed through rotary evaporation to form the paste.1.5 Device fabrication The solar cells were fabricated at room temperature under ambient air condition wi
21、thout using glove-box.Fluorine-doped tin dioxide(FTO)coated glass was patterned by 2 mol/L HCl solution and zinc powder,cleaned sequentially by detergent,deionized water and isopropanol,each for 30 min under ultrasonication.The compact titania(c-TiO2)layer was prepared by spraying titanium diisoprop
22、oxide bis(acetylacetonate)in isopro-panol(1:10(in volume)at 500 and annealed for 30 min.The mesoporous TiO2(m-TiO2)layer was screen-printed on the c-TiO2 layer and then annealed at 500 for 30 min.The zirconia ink was sprayed on the m-TiO2 layer at 180 for 1020 cycles,followed by washing in water.Aft
23、erwards,carbon paste was screen-printed on the ZrO2 layer and sintered at 400 for 30 min.The titania and carbon layer were optimized to be 700 nm and 10 m,respectively.Finally,PSCs were accomplished by drip-casting perovskite solution onto the carbon electrode and dried at 50 for 1 h(Fig.S1).For com
24、parison,screen-printing method was used to fabricate the zirconia layer with the zirconia paste and sintered at 500 for 30 min.To build a PSC module,a 5-cell series was designed on a single FTO substrate as the previous report27.Zirconia layer was sprayed on the substrate covered with a metal patter
25、ned mask.The other fabrication process of the PSC module was the same to that of the single cell.The spray-coating was done with an Iwata HP-BP spray pen(3105 Pa).2 Results and discussion Fig.1(a)shows the structural schematic illustration of TiO2/ZrO2/carbon triple-layer PSCs,and the correspon-ding
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