Manipulating Crystal Growth and Secondary Phase PbI2 to Enable Efficient and Stable Perovskite Solar Cells with Natural Additives

doi:10.1007/s40820-024-01400-w

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Abstract

In perovskite solar cells (PSCs), the inherent defects of perovskite film and the random distribution of excess lead iodide (PbI₂) prevent the improvement of efficiency and stability. Herein, natural cellulose is used as the raw material to design a series of cellulose derivatives for perovskite crystallization engineering. The cationic cellulose derivative C-Im-CN with cyano-imidazolium (Im-CN) cation and chloride anion prominently promotes the crystallization process, grain growth, and directional orientation of perovskite. Meanwhile, excess PbI₂ is transferred to the surface of perovskite grains or formed plate-like crystallites in local domains. These effects result in suppressing defect formation, decreasing grain boundaries, enhancing carrier extraction, inhibiting non-radiative recombination, and dramatically prolonging carrier lifetimes. Thus, the PSCs exhibit a high power conversion efficiency of 24.71%. Moreover, C-Im-CN has multiple interaction sites and polymer skeleton, so the unencapsulated PSCs maintain above 91.3% of their initial efficiencies after 3000 h of continuous operation in a conventional air atmosphere and have good stability under high humidity conditions. The utilization of biopolymers with excellent structure-designability to manage the perovskite opens a state-of-the-art avenue for manufacturing and improving PSCs.

Key words： Perovskite Solar cells Defect passivation Biomass additives Crystal orientation

Received: 02 January 2024 Published: 29 April 2024

Corresponding Authors: Jinming Zhang, Jizheng Wang

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	Yirong Wang
	Yaohui Cheng
	Chunchun Yin
	Jinming Zhang
	Jingxuan You
	Jizheng Wang
	Jinfeng Wang
	Jun Zhang

Cite this article:

Yirong Wang,Yaohui Cheng,Chunchun Yin, et al. Manipulating Crystal Growth and Secondary Phase PbI₂ to Enable Efficient and Stable Perovskite Solar Cells with Natural Additives[J]. Nano-Micro Letters, 2024, 16(1): 183-.

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https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-024-01400-w OR https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/183

Fig. 1 PSCs passivated with cellulose derivatives: a schematic illustration of PSCs passivated with cellulose derivatives; b SEM images of the surfaces of perovskites passivated with different cellulose derivatives (Scale bar: 500 nm); c cross-sectional SEM images of the control PSC and PSC passivated with C-Im-CN (PVSK/C-Im-CN) (Scale bar: 500 nm); d element contents of the plate-like crystallite and the white flake on the grain surface in PVSK/C-Im-CN; grazing incidence wide-angle X-ray scattering (GIWAXS) patterns of e the control PSC and f PVSK/C-Im-CN; Crystallite orientation fits to the characteristic peaks of PbI2 (orange line) and PVSK (green line) in g the control PSC and h PVSK/C-Im-CN; i crystallite orientation of the control PSC and PVSK/C-Im-CN at (110) and (001)* crystal faces; and j schematic illustration of perovskites passivated with different cellulose derivatives. (Note: (110) and (220) belong to PVSK; (001)* is assigned to PbI2)

Fig. 2 Mechanism of cellulose derivatives passivating perovskite: a chemical structure of C-Im-CN and perovskite; b Pb 4f high-resolution XPS spectra of control and PVSK/C-Im-CN; c I 3d high-resolution XPS spectra of control and PVSK/C-Im-CN; d Raman spectra of control and PVSK/C-Im-CN; e zeta potentials of C-Im-CN, FAI, MACl, MABr, C-Im-CN/FAI, C-Im-CN/MACl, and C-Im-CN/MABr; f mass spectra of PbI2/C-Im-CN solution; g FTIR spectra of PbI2, C-Im-CN, and PbI2/C-Im-CN; h 1H-NMR spectra of PbI2, C-Im-CN, and PbI2/C-Im-CN; i N 1s high-resolution XPS spectra of control and perovskites passivated with cellulose derivatives; j FTIR spectra of FAI, C-Im-CN, and FAI/C-Im-CN; k 1H-NMR spectra of FAI and FAI/C-Im-CN; and (I) schematic illustration of the interactions between C-Im-CN and perovskite

Fig. 3 Photovoltaic performance of control and perovskites passivated with cellulose derivatives: a J-V curves of PSCs; b J-V curves of PSCs measured at reverse and forward scans; c distribution graphs of PCEs (Box plots and normal distribution curves are displayed next to the data points. Each case is collected from 40 independent devices.); d J-V curves of PSCs of PVSK/C-Im-CN plus measured at reverse and forward scans; e IPCE and the integrated JSC of control plus and PVSK/C-Im-CN plus; f maximal steady-state photocurrent and stabilized PCE of PVSK/C-Im-CN plus; and g photovoltaic efficiency of PSCs based on different cellulose additives in recent years

Fig. 4 Characterization of perovskites with or without cellulose derivatives: a steady-state PL spectra of perovskites with or without cellulose derivatives; b PL lifetime spectra of perovskites; c dark J-V curves for the electron only devices with the structure of ITO/SnO2/perovskite/PCBM/Ag; d dark J-V curves for the hole only devices with the structure of ITO/PEDOT:PSS/perovskite/Spiro-OMETAD; e UV-vis absorption spectra of perovskites; f energy level illustration of the main functional layers in PSCs; g Nyquist plots of PSCs; and h VOC and i JSC response under different light intensities

Fig. 5 Device stability test of the control and PVSK/C-Im-CN: a and b SEM images of the surface and cross-section of the control under air environment after 14-30 days (RH = 25%-30%, T = 20-25 °C); c and d SEM images of the surface and cross-section of the PVSK/C-Im-CN under air environment after 14-30 days (RH = 25%-30%, T = 20-25 °C); e XRD spectra of the control and PVSK/C-Im-CN under air environment for different days (RH = 25%-30%, T = 20-25 °C); f Ratio of PbI2/perovskite crystal peak of the control and PVSK/C-Im-CN; g and h Pb 4f high-resolution XPS spectra of the control and PVSK/C-Im-CN before and after the aging period under air environment (RH = 25%-30%, T = 20-25 °C); i Stability of the control and PVSK/C-Im-CN devices under 3,000 h (RH = 25%-30%, T = 20-25 °C); j Stability of the control and the PVSK/C-Im-CN devices under high humidity condition of 300 h (RH = 85±5%, T = 85 °C)

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