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Series and Parallel Module Designing on Large Area Perovskite Solar Cells Lili Gao, Lin Chen, Shiyu Huang, Xiaolei Li, and Guanjun Yang ACS Appl. Energy Mater., Just Accepted Manuscript • DOI: 10.1021/acsaem.9b00531 • Publication Date (Web): 10 Apr 2019 Downloaded from http://pubs.acs.org on April 10, 2019

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ACS Applied Energy Materials

Series and Parallel Module Designing on Large Area Perovskite Solar Cells Lili Gao, Lin Chen, Shiyu Huang, Xiaolei Li, and Guanjun Yang* School of Materials Science and Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, PR China KEYWORDS: perovskite solar cells, series, parallel, perovskite solar module, large area ABSTRACT: Organometal halide perovskites have exhibited a bright future as photovoltaic semiconductor in next generation solar cells due to their unique and promising physicochemical properties. However, large area perovskite solar cells (PSCs) have suffered from problems of low efficiency with large active area and outputting module designing. Herein, we research the influence of the length and width when increasing device areas on outputting performance and design of series and parallel connection for large area PSC modules. The results show that high efficiency of 19.52% and 18.65% for single solar cell of area 0.1 and 1.0 cm2 respectively, are obtained. During the increasing of device area, increasing the length of the device can achieve higher efficiency than increasing the width for single PSCs. By comparing series and parallel connection mode, we come up with that first series and then parallel perovskite module is the best way to obtain high power outputting. The designing research for perovskite modules offer directions for PSC modules in future application. 1. Introduction Organic-inorganic halide perovskites solar cells (PSCs, such as CH3NH3PbI3) have

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attracted widespread attention and achieved high efficiency because of the unique properties of perovskite.1-7 The special optoelectronic properties, (such as, large absorption, long diffusion length, and high mobility)8-15 and the low-cost fabrication methods (for example, vapor deposition and solution spin-coating)16-22 significantly promote the development of PSCs. As a result of excellent preparation methods, device structure optimization, interface engineering, and so on, the efficiency of PSCs has reached as high as 23.3%.23 Thereby, PSCs present a great potential for outdoor photovoltaic applications by utilizing solar energy.24-26

In order to achieve the industrialization of PSCs, there are still many challenges needing to be solved, such as the low efficiency of large area solar cells, preparation of largearea perovskite thin films with high uniformity and reproducibility,27-31 and

the

design of interconnection about single cells to make large modules.32-36 Many works have been down about large area PSCs, as shown in Table S1 in supporting information. Although large perovskite modules have been reported,24,

34, 37-41

the regulation of

designing modules for high power outputting is still unclear. During the process of perovskite film area enlarging, pin-holes are unavoidable. Therefore, it’s necessary to divide the whole film into pieces and connect them into modules. Even though large area silicon solar cells have well used modules design, the modules mode doesn’t suitable for large area perovskite films because of the unavoidable defects during perovskite film formation.42 Therefore, a reasonable and logical piece dividing and module designing are critical for a highly perovskite efficiency. It is also significantly


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for the industrialization of large area PSCs.24, 26, 38, 39

In this manuscript, we firstly research the influence of solar cell shape on single solar cell performance, and we achieved high efficiency of 19.52% and 18.65% for single solar cell with active area 0.1 and 1.0 cm2 respectively. The results reveal that increasing the length is the better way to enlarge solar cell area for high efficiency outputting than increasing the width. Secondly, we compared modules in series and parallel with different areas. The results show that series modules can achieve high open circuit voltage (Voc) but relatively low current outputting. With the area of 6.12 and 10.125 cm2 series modules, we achieve the current density (Jsc) of 18.45 and 16.85 mA cm-2, the Voc of 4.42 and 5.50 V, and the efficiency of 13.14%, 12.31%, respectively. However, parallel modules can output high current and relatively high Voc. With the area of 6.51 cm2 parallel modules, we obtained high Voc of 1.13 V. By comparing the performances, we propose that first series and then parallel perovskite module is the best way to obtain high power outputting.

2. Result and discussion 2.1 Influence of size on single PSCs outputting. Single solar cell is the unit for modules. The designing of single unit is important for efficiency outputting. We firstly prepared single PSC with size of 0.1 and 1.0 cm2, respectively. Small area (＜0.1 cm2) PSCs are the competitive in high efficiency. As shown in Figure 1a, we prepare four small area of 0.1 cm2 on 2.5×2.5 cm2 substrate



one time. The planer structure is shown in Figure 1a, and the photos of completed PSCs is shown in Figure 1b. Perovskite film is prepared by gas pump drying method as reported before.43 Because of the compact perovskite film, we achieved high efficiency of 19.52% with high Voc of 1.11 V, as the J-V cure shown in Figure 1c. It is also worth mentioning that the fill factor (FF) is as high as 0.78, which contributes to the power outputting. The high FF illustrates that the interface recombination of every layer is weak because of the perfect perovskite layer contact well both with electronic and hole transport layer. The forward and reverse scan is also tested and shown in Figure S1a. The results show that the hysteresis is little with forward scan efficiency is 17.12%. The corresponding incident photon-to-electron conversion efficiency (IPCE) is shown in Figure S1b. The integrated current density is as high as 20.62 mA cm-2, which is comparable with the short circuit current from J-V cure. In addition, the reproducibility of small area PSCs are shown in Figure 1d, the output performance showed well repeatability. Thereby, the high performance of small area (0.1 cm2) PSCs offer great potential of large scale solar cells development.


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Figure 1. (a) Schematic diagram of making process and structure of 0.1 cm2 active area device, (b) photo of 0.1 cm2 device, (c) the J-V cure of best efficiency of 0.1 cm2 device, (d) parameters distribution of 0.1 cm2 device.

In laboratory, solar cells with 1 cm2 is generally supposed as the smallest unit for solar cell modularization.44 Therefore, we further prepared PSCs with the mask and structure as shown in Figure 2a and 2b. The device size is rectangular with 0.5 × 2 cm2. We achieved efficiency of 18.65% with high Voc of 1.13 V, as shown in Figure 2c. The forward and reverse scan presents little hysteresis as shown in Figure S2a, and the IPCE is shown in Figure S2b. High reproducibility of 1 cm2 device is also fulfilled, as shown in Figure 2d. We enlarged the device area from 0.1 to 1 cm2 and all obtained well efficiency and reproducibility.



Figure 2. (a) Schematic diagram of making process and structure of 1.0 cm2 active area device, (b) photo of 1.0 cm2 device, (c) the J-V cure of best efficiency of 1.0 cm2 device, (d) parameters distribution of 1.0 cm2 device.

For a rectangular active area device, we can enlarge the area by increasing both its length and width, as shown in Figure 3a to c. In order to make clear the differences, we design a series of device areas enlarged both from the long side and the wide side. Firstly, we investigated the influence of length increasing on device performance. As shown in Figure 4a, the width is set as 2 mm, and the length increases from 5 to 35 mm. The J-V cures (Figure 4b) shows that device with 10 mm length achieved highest efficiency. With the increasing length and active area, the efficiency drops slightly, as shown in Figure 4c. In addition, Jsc dropped by about 14% with length increasing from 5 to 35 mm, while the Voc increased by about 12% with active area increasing from 0.1


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to 0.7 cm2, and the FF changed slightly. The decrease of Jsc can be attributed to the recombination during the carrier transport within increased active areas, as the schematic diagram shown in Figure S3. Large active area would induce more defects inevitably, which result in more recombination. Thereby, the efficiency dropped slightly mainly due to the decreasing of Jsc with length increasing.

Secondly, we set the length as 35 mm, and increase the width from 2 to 8 mm, as shown in Figure 4d. The outputting performance of the devices are shown in Figure 4e and 4f, the Jsc and FF dropped quickly with increasing width, but the Voc increased. However, the increase of Voc can’t offset the seriously decrease of Jsc and FF, thereby, the efficiency dropped quickly with active area increasing. The decrease of Jsc and FF can be attributed to the transportation of carriers at width direction is extended, as shown in Figure S4. Thereby, the chance of recombination increased and the collected current decreased. Compared those two ways of active area enlarging, Voc will not be influenced and Jsc dropped quickly especially with width increasing. Therefore, increasing the length is the best choice when preparing large active area devices.

Figure 3. Schematic diagram of enlargeing device active area, (a) a rectangular active area shape of device (the red section), (b) enlarge the rectangular active area device



from the long side, (c) enlarge the rectangular active area device from the wide side.

Figure 4. (a) Schematic diagram of a seris of devices with active area enlarged from long side, (b) J-V cures of devices with active area enlarged from long side, (c) outputting parameters of devices with active area enlarged from long side, (d)


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Schematic diagram of a seris of devices with active area enlarged from wide side, (e) J-V cures of devices with active area enlarged from wide side, (f) outputting parameters of devices with active area enlarged from wide side. 2.2 Module designing and properties research of perovskite solar cells 2.2.1 Series module designing and properties research For PSCs module, the joint of each unit cell is very important. Series and parallel connections are the most frequently used strategy to fabricate perovskite solar modules.40, 41 For series mode, it means the anode of one device connects with that of the adjacent device. Series mode will increase the Voc of the modules while keep the photocurrent as small as every unit cell.45, 46

We first prepared series perovskite solar modules on 4.5×4.5 cm2 and 5.5×5.5 cm2 substrates. The preparing process and structure are shown in Figure 5a. Figure 5b and c show the photos of perovskite module with series connection on two kinds of size. The size of each unit is 3.4×0.45 cm2, there are 4 units on 4.5×4.5 cm2 substrate with total active area 6.12 cm2. Therefore, the effective using active area is 30.22%. The efficiency of the module with active area 6.12 cm2 is 13.14% with the Voc of 4.42 V, as the J-V cure shown in Figure 5d. And the series modules present well steady-state outputting with 12.51% efficiency, as shown in Figure S5a. When the substrate enlarged to 5.5×5.5 cm2, there are 5 units with size of 4.5×0.45 cm2 each one. Thereby, the total active area is 10.125 cm2, which is 65.44% larger than the active area on 4.5×4.5 cm2 substrate. The effective using active area on 5.5×5.5



cm2 substrate increased to 33.47%. The larger module still hold a comparative higher efficiency of 12.31% with Voc of 5.50 V, as the J-V cure shown in Figure 5e. The high Voc proved that the perovskite film was fully compact in all of the whole layer. And this series module showed 10.57% steady state efficiency, as shown in Figure S5b. The series module all presented well repeatability, as shown in Figure 5f and g. Series connection can almost output high Voc, therefore, series maybe a well mode for large size modules production.


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Figure 5. (a) Series modules producing process and structure, (b) photo of perovskite modules on 4.5×4.5 cm2 substrate, (c) photo of perovskite modules on 5.5×5.5 cm2 substrate, (d) J-V cure of perovskite module with active area of 6.12 cm2, (e) J-V cure of perovskite module with active area of 10.125 cm2, (f) parameters distribution of perovskite modules with active area of 6.12 cm2, (g) parameters distribution of perovskite modules with active area of 10.125 cm2. 2.2.2 Parallel module designing and properties research Despite an ideal Voc can be achieved for perovskite modules connected in series, the desired precision to match Jsc of single cells is still difficult to realize. To solve these problems, parallel connection attracted much more attention, which should connect adjacent cells for modules to minimize the energy loss.47 In parallel designing, the anode of the unit device is connected to the anode of the adjacent unit, and the cathode of the unit device is connected to the cathode of the adjacent unit.

The parallel perovskite modules were also fabricated on 4.5×4.5 cm2 substrate. The size of each unit is 3.1×0.7 cm2, and there are 3 units. Thereby, the total active area of parallel perovskite module is 6.51cm2, and the effective using active area of the parallel module is 32.15%. The effective utilize of parallel module is a little higher than series module on the same size 4.5×4.5 cm2 substrate. The structure is shown in Figure 6a. Figure 6b shows the photo of the parallel perovskite module. The J-V cure with 5.49% efficiency of the parallel perovskite module is shown in Figure 6c. The Jsc and Voc are 15.59 mA cm-2 and 1.13 V, respectively, which are comparatively high outputting.



Therefore, parallel connection would output high Voc and Jsc by coordinating each unit cells. However, as shown in Figure 6c and 6d, the FF only had value of 0.31, indicating the serious outputting loss. The reason is that collection and transportation of carriers were difficult between each unit cell. As a steady- state efficiency, the parallel module outputs 4.48% as shown in Figure S6.

Figure 6. (a) Parallel modules structure, (b) photo of parallel perovskite modules, (c) J-V cure of parallel perovskite module with active area of 6.51 cm2, (d) parameters distribution of parallel perovskite module with active area of 6.51 cm2.

2.2.3 Series and parallel modules properties comparation. Perovskite modules is the connection of single solar cells, thereby, we firstly compare the outputting of single solar cells and series perovskite modules, as shown in Figure 7. Compared with single PSCs with active area of 1.0 cm2, series perovskite modules both with 6.12 and 10.125 cm2 showed considerable Voc and FF, as shown in Figure 7b and


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c. However, the Jsc of series modules is lower than that of single solar cells, which results in relatively low outputting efficiency, as shown in Figure 7a and d. The reason is that the series module outputs the lowest Jsc among all the connected unit devices. Furthermore, we compared the outputting of parallel and series connection, as shown in Figure 8. The Jsc and Voc of parallel connection are comparative with series connection, as shown in Figure 8a and b. However, the FF of parallel is much lower than series, which induced the low efficiency outputting, as shown in Figure 8c and d. The reason for the lower FF can be attributed to the bad connection between each unit device, which reduce carrier collection and transportation difficult. Based on the comparison, we can combine the advantages of both connections. First series connection, we can obtain a high outputting Voc, and then parallel connection, we can obtain a high outputting Jsc. Therefore, the combined mode can be employed the for large scale perovskite modules. The series connection is the first to achieve a high Voc outputting and then parallel connection is followed to obtain a high Jsc outputting. We connected four series perovskite mode with active area of 6.12 cm2 by parallel mode. Excitingly, it can drive an air fan working, as shown in supporting information.



Figure 7. Parameters comparation of single solar cells with 1.0 cm2, series perovskite modules with 6.12 cm2 and 10.125 cm2, (a) Jsc, (b) Voc, (c) FF, and (d) PCE.


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Figure 8. Parameters comparation of parallel perovskite modules with 6.51 cm2, series perovskite modules with 6.12 cm2 and 10.125 cm2, (a) Jsc, (b) Voc, (c) FF, and (d) PCE. 3. Conclusions In conclusion, we achieved high efficiency of 19.52% and 18.65% for single solar cells with active area 0.1 and 1.0 cm2 respectively. For large area single PSCs, increasing the length of the device can achieve higher efficiency than increasing the width. For perovskite solar modules, we compared the outputting properties of series and parallel connection mode. The results show that series modules can achieve high Voc and parallel modules can obtain high Jsc. With the area of 6.12 and 10.125 cm2 series modules, we achieve Voc of 4.42 and 5.50 V, respectively. With the area of 6.51 parallel modules, we obtained high Jsc of 15.59 mA cm-2. Thereby, we come up with that first



series and then parallel perovskite module is the best way to obtain high power outputting. The designing research for perovskite modules is significantly to promote the development of PSCs.

4. Experiments

Materials Preparation Lead iodide (PbI2, 99.99%) and iodine methylamine (CH3NH3I) were purchased from Xi’an Polymer Light Technology Corp. N, N-dimethylformamide (DMF, 99.8%), were purchased from National drug group chemical reagents Co., Ltd. All the materials were used as received.

Device Fabrication The designed shapes of all devices were controlled by FTO, which etched by laser. The FTO coated glass (Pilkington, 15Ωsq-1) was cleaned through an ultrasonic bath sequentially with acetone, ethyl alcohol, and deionized water for 15 min, respectively, and then dried by Nitrogen. The TiO2 compact layer was coated by bath hydrolysis of TiCl4 as reported.48 Before perovskite layer fabrication, FTO substrates were treated in UV Ozone for 30 min. then perovskite layer was prepared by gas pump method after spin coating at 2000 rpm 10 s, and the dried mirror-black thin film was heated at the hot-plate for 10 min. Then the spiro-OMeTOD transport layer, by dissolving 72.3mg of spiro-MeOTAD in 1 ml of chlorobenzene, to which 28.8 mL of 4-tert-butylpyridine,


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and 17.5 mL of lithiumbis(trifluoromethanesulfonyl)imide(Li-TFSI) solution (520mg LI-TSFI in 1mL acetonitrile, Sigma–Aldrich, 99.8%) added, was spin coated at 3000rpm for 30s. Finally, Au was evaporated, as the electrode, with thickness of 80 nm.

Characterization The J–V curves (reverse and forward) were measured with a 2400 series source meter, Keithley Instruments, under the illumination of simulated air-mass (AM) 1.5 sunlight at100mW cm-2 (Class AAA solar Sol3A, Oriel Instruments). The IPCE spectra were measured by using a Qtest Station 1000ADX system (Growntech, Inc.) in air without bias light. The illumination spot size was slightly smaller than the active area of the test cells. The IPCE photocurrents were recorded under short-circuit conditions using a Keithley 2400 source meter. The monochromatic photon flux was quantified by means of a calibrated silicon photodiode.

ASSOCIATED CONTENT Supporting Information. J–V curves, IPCE and integrated current density spectrum of the PSC with active area of 0.1 cm2 and 1.0 cm2 (reverse and forward scans). Schematic diagram of original device area and enlarged device area from length and width. Steady-state photocurrent and their corresponding device power output for series and parallel modules. Some other reports on large area PSCs. Video for air fan moving driven by series and parallel connected



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perovskite modules.

AUTHOR INFORMATION Corresponding Author *E-mail: [email protected]. Competing Interests The authors declare no competing financial interests. ACKNOWLEDGMENT The authors thank the financial support of the National Program for Support of Topnotch Young Professionals.

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