Enhancement of charge collection capability by potassium-doped NiO in inverted planar perovskite solar cells

Zhao Xing; Li Dan-Ni; Li Mei-Cheng

doi:10.7498/aps.73.20240974

Abstract

Perovskite solar cells (PSCs) with inverted structures have received significant attention in the field of photovoltaics. NiO is one of the commonly explored hole transport materials (HTMs) because of its excellent chemical stability in comparison with organic materials. Pure NiO is an insulator, but the presence of nickel vacancies can lead to the formation of Ni³⁺ ions, resulting in p-type semiconductor properties. However, the low conductivity and poor interfacial contact between NiO and perovskite thin films still pose challenges in achieving high-performance inverted PSCs. To solve these problems, potassium acetate is used as a potassium source for a nickel precursor, and therefore potassium ions (K⁺) are doped into NiO nanocrystals. The introduction of K⁺ into NiO leads to the formation of Ni³⁺ ions, thereby increasing the conductivity and hole mobility of NiO. Furthermore, K⁺-doped NiO exhibits better interface contact with the perovskite film, facilitating the efficient separation of photo-generated charges and showing a strong photoluminescence quenching effect. Experimental results demonstrate that the optimal concentration of K⁺ doping is 3%, and the PSCs prepared with K⁺-doped NiO exhibit a significant increase in efficiency, from 15.15% to 16.75%, which is attributed primarily to the improvements in the short-circuit current density and fill factor. These improvements highlight the importance of enhanced conductivity and better interfacial contact achieved through K⁺ doping for charge carrier collection, effectively addressing the limitations of NiO in inverted PSCs.

Keywords:

Authors and contacts

State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources, School of New Energy, North China Electric Power University, Beijing 102206, China

Corresponding author: Li Mei-Cheng, mcli@ncepu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 22409061, 52232008, 51972110, 52102245, 52072121), the Beijing Natural Science Foundation, China (Grant Nos. 2222076, 2222077), the Huaneng Group Headquarters Science and Technology Project, China (Grant No. HNKJ20-H88), and the Fundamental Research Funds for the Central Universities (Grant Nos. 2023MS047, 2023MS042).

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References

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Cited By

图 1 不同浓度K⁺掺杂NiO的电池光伏特性参数统计图　(a) J_SC; (b) V_OC; (c) FF; (d) PCE

Figure 1. Statistical photovoltaic parameters of PSCs with different concentrations of K⁺ ions doping into NiO: (a) J_SC; (b) V_OC; (c) FF; (d) PCE.

DownLoad: Full-Size Img PowerPoint

图 2 K⁺掺杂前后电池结构及光伏特性变化　(a)反式PSC结构示意图; (b)能级图; (c)不同浓度K⁺掺杂NiO的电池最佳J-V曲线; (d) 基于NiO和3% K⁺掺杂NiO (K:NiO)的电池正反扫J-V曲线; (e)电池的外量子效率(EQE)曲线; (f) 基于K:NiO空穴传输层的电池最大功率点追踪曲线

Figure 2. Changes in device structure and photovoltaic characteristics before and after K⁺ doping: (a) Schematic device structure of inverted PSC; (b) energy level diagram of inverted PSC; (c) J-V curves of PSCs using NiO before and after K⁺ doping with different molar ratios; (d) J-V curves of PSCs using NiO and 3% K⁺-doped NiO (K:NiO) scanned at forward and reverse scan; (e) external quantum efficiency (EQE) spectra along with the integrated photocurrent density for PSCs; (f) maximum power point tracking of PSC based on K:NiO HTL.

DownLoad: Full-Size Img PowerPoint

图 3 K⁺掺杂前后NiO的光学及晶体结构变化, 即玻璃上NiO和3% K⁺掺杂NiO薄膜的(a)透射率和(b) GIXRD图谱

Figure 3. Changes in optical and crystal structure of NiO films before and after K⁺ doping: (a) Transmittance and (b) GIXRD of NiO and 3% K⁺-doped NiO films deposited on glass.

DownLoad: Full-Size Img PowerPoint

图 4 NiO和3% K⁺掺杂NiO的XPS谱图, 其中(a), (b) K 2p, (c), (d) Ni 2p和(e), (f) O 1s; 不同浓度K⁺掺杂的NiO XPS谱图, 其中(g) K 2p和(h) Ni 2p; (i)不同浓度K⁺掺杂NiO的Ni³⁺/Ni²⁺比值变化曲线

Figure 4. XPS spectra of (a), (b) K 2p, (c), (d) Ni 2p, (e), (f) O 1s for NiO and 3% K⁺-doped NiO; XPS of (g) K 2p and (h) Ni 2p of K doped NiO with various molar ratio; (i) ratio of Ni³⁺/Ni²⁺ of NiO or K doped NiO with various molar ratio.

DownLoad: Full-Size Img PowerPoint

图 5 NiO和掺杂3% K⁺的NiO薄膜的电学性能表征　(a) 暗态I-V曲线; (b) SCLC曲线; 其中NiO厚度为20 nm, 器件结构为FTO/HTL(NiO or K:NiO)/钙钛矿/spiro-MeOTAD/Au

Figure 5. Electrical properties of NiO thin films with and without K⁺ doping: (a) Dark I-V and (b) SCLC curves of NiO films with and without K⁺ doping. The thickness of NiO is 20 nm, and the device structure is FTO/HTL (NiO or K:NiO)/perovskite/spiro-MeOTAD/Au.

DownLoad: Full-Size Img PowerPoint

图 6 K⁺掺杂对MAPbI₃薄膜的影响　(a) NiO和(b) 3% K⁺掺杂NiO薄膜上的MAPbI₃表面形貌图; (c)沉积在NiO和K:NiO基底上的MAPbI₃的粒径分布; K⁺掺杂前后MAPbI₃薄膜的(d)吸光度和(e) XRD谱图

Figure 6. Influence of K⁺ doping on perovskite films: (a), (b) SEM images of MAPbI₃ deposited on (a) NiO and (b) 3% K⁺-doped NiO films; (c) grain size distribution of MAPbI₃ deposited on NiO and K:NiO substrates; (d) absorbance and (e) XRD patterns of MAPbI₃ layers.

DownLoad: Full-Size Img PowerPoint

图 7 MAPbI₃ 沉积在未掺杂NiO和3% K⁺掺杂NiO薄膜上的(a)稳态光致发光光谱(SSPL)和(b)时间分辨光致发光光谱(TRPL)光谱

Figure 7. (a) Steady-state photoluminescence (SSPL) and (b) time-resolved photoluminescence (TRPL) of MAPbI₃ deposited on undoped NiO and 3% K⁺ doped NiO films formed on bare glass.

DownLoad: Full-Size Img PowerPoint

表 1 不同浓度K⁺掺杂NiO的电池最佳光伏特性参数

Table 1. Photovoltaic parameters of the best-performing PSCs using NiO before and after K⁺ ions doping with different molar ratios.

K⁺/% J_SC/(mA·cm^–2) V_OC/V FF PCE/%

0 19.62 1.00 0.77 15.15

1 20.61 0.99 0.78 15.98

3 20.78 1.01 0.79 16.75

5 19.81 1.00 0.78 15.47

7 19.87 1.02 0.75 15.25

DownLoad: CSV

[1]	Kim H S, Lee C R, Im J H, Lee K B, Moehl T, Marchioro A, Moon S J, Humphry-Baker R, Yum J H, Moser J E, Grätzel M, Park N G 2012 Sci. Rep. 2 591 Google Scholar
[2]	Roy P, Kumar Sinha N, Tiwari S, Khare A 2020 Sol. Energy 198 665 Google Scholar
[3]	Li S D, Xiao Y, Su R, Xu W D, Luo D Y, Huang P R, Dai L J, Chen P, Caprioglio P, Elmestekawy K A, Dubajic M, Chosy C, Hu J T, Habib I, Dasgupta A, Guo D Y, Boeije Y, Zelewski S J, Lu Z Y C, Huang T Y, Li Q Y, Wang J M, Yan H M, Chen H H, Li C S, Lewis B A I, Wang D K, Wu J, Zhao L C, Han B, Wang J P, Herz L M, Durrant J R, Novoselov K S, Lu Z H, Gong Q H, Stranks S D, Snaith H J, Zhu R 2024 Nature Doi: 10.1038/s41586-024-08159-5
[4]	Wang Y R, Lin R X, Liu C S Y, Wang X Y, Chosy C, Haruta Y, Bui A D, Li M H, Sun H F, Zheng X T, Luo H W, Wu P, Gao H, Sun W J, Nie Y F, Zhu H S, Zhou K, Nguyen H T, Luo X, Li L D, Xiao C X, Saidaminov M I, Stranks S D, Zhang L J, Tan H R 2024 Nature Doi: 10.1038/s41586-024-08158-6
[5]	Zhao X, Kim H S, Seo J Y, Park N G 2017 ACS Appl. Mater. Interfaces 9 7148 Google Scholar
[6]	Boyd C C, Shallcross R C, Moot T, Kerner R, Bertoluzzi L, Onno A, Kavadiya S, Chosy C, Wolf E J, Werner J, Raiford J A, de Paula C, Palmstrom A F, Yu Z J, Berry J J, Bent S F, Holman Z C, Luther J M, Ratcliff E L, Armstrong N R, McGehee M D 2020 Joule 4 1759 Google Scholar
[7]	Barsoum M W 2002 Fundamentals of Ceramics (Boca Raton: CRC Press
[8]	Zhao X, Chen J, Park N G 2019 Sol. RRL 3 1800339 Google Scholar
[9]	Chen W, Wu Y Z, Yue Y F, Liu J, Zhang W J, Yang X D, Chen H, Bi E B, Ashraful I, Grätzel M, Han L Y 2015 Science 350 944 Google Scholar
[10]	Jung J W, Chueh C C, Jen A K Y 2015 Adv. Mater. 27 7874 Google Scholar
[11]	Chen W, Liu F Z, Feng X Y, Djurišić A B, Chan W K, He Z B 2017 Adv. Energy Mater. 7 1700722 Google Scholar
[12]	Yu S Q, Xiong Z, Zhou H T, Zhang Q, Wang Z H, Ma F, Qu Z H, Zhao Y, Chu X B, Zhang X W, You J B 2023 Science 382 1399 Google Scholar
[13]	Li L, Wei M Y, Carnevali V, Zeng H P, Zeng M M, Liu R R, Lempesis N, Eickemeyer F T, Luo L, Agosta L, Dankl M, Zakeeruddin S M, Roethlisberger U, Grätzel M, Rong Y G, Li X 2024 Adv. Mater. 36 2303869 Google Scholar
[14]	Bai Y, Chen H M, Xiao S, Xue Q F, Zhang T, Zhu Z L, Li Q, Hu C, Yang Y, Hu Z C, Huang F, Wong K S, Yip H L, Yang S H 2016 Adv. Funct. Mater. 26 2950 Google Scholar
[15]	Zhou Y, Huang X, Zhang J, Zhang L, Wu H, Zhou Y, Wang Y, Wang Y, Fu W, Chen H 2024 Adv. Energy Mater. 14 2400616 Google Scholar
[16]	Zhao X, Zhou J J, Wang S Y, Tan L G, Li M H, Li H, Yi C Y 2021 ACS Appl. Energy Mater. 4 6903 Google Scholar
[17]	Zhang Y, Kim S G, Lee D K, Park N G 2018 ChemSusChem 11 1813 Google Scholar
[18]	Manders J R, Tsang S wing W, Hartel M J, Lai T han H, Chen S, Amb C M, Reynolds J R, So F 2013 Adv. Funct. Mater. 23 2993 Google Scholar
[19]	Liu J, Hanson M P, Peters J A, Wessels B W 2015 ACS Appl. Mater. Interfaces 7 24159 Google Scholar
[20]	Zhang J Y, Li W W, Hoye R L Z, MacManus-Driscoll J L, Budde M, Bierwagen O, Wang L, Du Y, Wahila M J, Piper L F J, Lee T L, Edwards H J, Dhanak V R, Zhang K H L 2018 J. Mater. Chem. C 6 2275 Google Scholar
[21]	Jang W L, Lu Y M, Hwang W S, Hsiung T L, Wang H P 2009 Appl. Phys. Lett. 94 062103 Google Scholar
[22]	Wang Y, Ghanbaja J, Bruyère S, Boulet P, Soldera F, Horwat D, Mücklich F, Pierson J F 2016 CrystEngComm 18 1732 Google Scholar
[23]	Grosvenor A P, Biesinger M C, Smart R S C, McIntyre N S 2006 Surf. Sci. 600 1771 Google Scholar
[24]	Liu S Y, Liu R, Chen Y, Ho S, Kim J H, So F 2014 Chem. Mater. 26 4528 Google Scholar
[25]	Zhao X, Qiu Y J, Wang M, Wu D X, Yue X P, Yan H L, Fan B B, Du S X, Yang Y Q, Yang Y Y, Li D N, Cui P, Huang H, Li Y F, Park N G, Li M C 2024 ACS Energy Lett. 9 2659 Google Scholar
[26]	Teo S, Guo Z L, Xu Z H, Zhang C, Kamata Y, Hayase S, Ma T L 2019 ChemSusChem 12 518 Google Scholar

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