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. 2025 Aug 22;11(34):eady3621.
doi: 10.1126/sciadv.ady3621. Epub 2025 Aug 20.

Imprisoning 2H intermediate phases in blade-coated wide-bandgap perovskites for efficient all-perovskite tandem solar cells

Dexin Pu  1   2 , Xuhao Zhang  3 , Hongyi Fang  1 , Weichen Shen  3 , Guoyi Chen  1 , Weiqing Chen  1 , Peng Jia  1 , Guang Li  3 , Hongling Guan  1 , Lishuai Huang  1 , Yuan Zhou  3 , Jiahao Wang  1 , Wenwen Zheng  3 , Weiwei Meng  4 , Guojia Fang  1 , Weijun Ke  1   2
Affiliations

Imprisoning 2H intermediate phases in blade-coated wide-bandgap perovskites for efficient all-perovskite tandem solar cells

Dexin Pu et al. Sci Adv. .

Abstract

Scalable fabrication of high-efficiency all-perovskite tandem solar cells (TSCs) remains challenging due to notable voltage deficits in wide-bandgap perovskite solar cells, primarily driven by severe halide segregation during the large-scale blade coating process. Here, we introduce 4-aminobenzylphosphonic acid as a functional "2H-imprison" additive that selectively bypasses the formation of the 2H phase (an iodine-rich structure) and promotes the direct crystallization of the desired 3C phase, resulting in a homogeneous phase and halide distribution. Consequently, blade-coated 1.77-electron volt-bandgap perovskite solar cells achieved a power conversion efficiency (PCE) of 20.35% (certified 19.72%) with an open-circuit voltage of 1.35 volts for a ~0.07-square centimeter aperture area, while 1.02-square centimeter devices delivered a PCE of 19.00%. Furthermore, the corresponding blade-coated two- and four-terminal all-perovskite TSCs demonstrated high PCEs of 27.34 and 28.46%, respectively. This study reveals the origins of phase segregation during blade coating and provides a viable strategy to mitigate it, paving the way for scalable and high-efficiency TSCs.

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Figures

Fig. 1.
Fig. 1.. Crystallization process and halide distribution of blade-coated WBG films.
In situ PL measurements of (A) a control film and (B) an ABP-treated film. (C) TOF-SIMS depth profiling of a control and an ABP-treated films. Buried interface GIXRD patterns of (D) a control film and (E) an ABP-treated film. PL mapping of (F) a control film and (G) an ABP-treated film. a.u., arbitrary units.
Fig. 2.
Fig. 2.. Phase segregation mechanism of blade-coated WBG films.
(A) XRD measurements of blade-coated films before air knife treatment. (B) Calculated formation energy (ΔH) for FAPbI3 and FAPbBr3 in different phases. f.u., (per) formula unit. (C) COHP analysis of the Pb-Pb interaction in FAPbI3 and FAPbBr3 with 2H phases. (D) Br mixing energy (EBr mixing) in different perovskite matrices. (E) ESP distribution of an ABP molecule. (F) ABP adsorption energy (Ead) on FAPbI3 and FAPbBr3 surfaces. (G) Schematic diagram of phase segregation generation and inhibition mechanism.
Fig. 3.
Fig. 3.. Carrier transport dynamics and defect passivation of blade-coated WBG perovskite films.
In situ PL measurements under continuous light illumination for (A) a control film and (B) an ABP-treated film. (C) XPS spectra of Pb 4f in perovskite films with and without ABP treatment. (D) PL and (E) TRPL spectra of a control film and a target film. (F) Energy band diagram of a control film and a target film. (G) Mott-Schottky plots for reference and ABP-treated PSCs. (H) Trap state densities (NT) of a control device and a target device measured at 300 K. (I) Light intensity–dependent VOC comparison of devices with and without ABP treatment.
Fig. 4.
Fig. 4.. Performance of blade-coated single-junction WBG PSCs.
(A) J-V scans of a control and an ABP-treated single-junction WBG PSCs. (B) VOC of the reported WBG blade-coated PSCs. (C) Steady-state power outputs and (D) EQE spectra of a control and an ABP-treated devices. (E) Maximum power point (MPP) tracking of the devices with and without ABP treatment in N2 under 100–mW cm−2 white light illumination at 55°C. (F) J-V scans, (G) steady-state power output, and (H) EQE spectrum of a representative 1.02-cm2 aperture area blade-coated WBG cell.
Fig. 5.
Fig. 5.. Performance of blade-coated all-perovskite two-terminal and four-terminal TSCs.
(A) Device architecture and (B) cross-sectional SEM image of two-terminal TSCs. (C) J-V scans, (D) steady-state power output, and (E) EQE spectra of a two-terminal blade-coated all-perovskite TSC. (F) Device architecture, (G) J-V scans, (H) steady-state power outputs, and (I) EQE spectra of a four-terminal blade-coated all-perovskite TSC. PEDOT:PSS, poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate).
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