Constructing robust heterointerfaces for carrier viaduct via interfacial molecular bridges enables efficient and stable inverted perovskite solar cells

Xu, Huifen1,2; Liang, Zheng1,2; Ye, Jiajiu1,3; Zhang, Yong6,7; Wang, Zihan1,2; Zhang, Hui1; Wan, Changmao1,2; Xu, Guangkun10; Zeng, Jie6,7; Xu, Baomin6,7; Xiao, Zhengguo2,8,9; Kirchartz, Thomas3,4,5; Pan, Xu1

2023-10-01

10.1039/d3ee02591h

ENERGY & ENVIRONMENTAL SCIENCE   Impact Factor & Quartile

1754-5692

1754-5706

A robust perovskite-substrate interface is critical to realize state-of-the-art inverted (p-i-n) perovskite solar cells (PSCs), as it enables charge carrier selectivity by means of suitable electrostatics, energy level alignment, and low interfacial recombination. To achieve this goal of carrier selectivity in p-i-n type PSCs, we propose a strategy of carrier viaduct via an interfacial molecular bridge comprised of Ph-CH2N+H3-n(CH3)(n) ammonium cations (where n is the degree of substitution). Through a joint theoretical-experimental study, we demonstrate that the most stable heterointerface is established by quaternary ammonium (QA, n = 3), where the -N+(CH3)(3) groups preferentially insert into the perovskite frameworks, with a vertical downward orientation of the phenyl groups towards the perovskite-substrates. This interfacial molecular bridge configuration as a carrier viaduct enables directional carrier management and redistributes a homogeneous environment at the heterointerface. Therefore, the carrier viaduct strategy enhances charge carrier extraction and transport in both in-plane or out-of-plane directions. Meanwhile, the bottom interfacial molecule acts as a double-sided molecular binder, maintaining the contact stack and strengthening the weak interface. The fabricated lab-scale inverted PSCs exhibit a champion efficiency of 25.45% (certified at 24.9%), with the fill factor exceeding 85.66%, corresponding to 95% of their thermodynamic limit at its bandgap (E-g = 1.54 eV). The corresponding perovskite solar modules for an active area of 23.25 cm(2) deliver an efficiency of 20.91%. Notably, even unencapsulated target PSCs retain nearly their initial efficiency after 3000 hours under light soaking at maximum power point tracking.

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This work was financially supposed by the National Natural Science Foundation of China (Grant U22A20142, No. 52302324 and No. 52272252), the National Key Ramp;D Program of China (No. 2021YFB3800102), HFIPS Directorapos;s Fund (Grant YZJJ-GGZX-2022-01) an["U22A20142","52302324","52272252"] ; National Natural Science Foundation of China[2021YFB3800102] ; National Key Ramp;D Program of China[YZJJ-GGZX-2022-01] ; HFIPS Directorapos;s Fund[554 2108085J34]

Chemistry ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology

Chemistry, Multidisciplinary ; Energy & Fuels ; Engineering, Chemical ; Environmental Sciences

WOS:001085652600001

ROYAL SOC CHEMISTRY

Web of Science

1.Chinese Acad Sci, Inst Solid State Phys, Hefei Inst Phys Sci HIPS, Key Lab Photovolta & Energy Conservat Mat, Hefei 230031, Peoples R China
2.Univ Sci & Technol China USTC, Hefei 230026, Peoples R China
3.Forschungszentrum Julich, IEK5 Photovolta, D-52425 Julich, Germany
4.Univ Duisburg Essen, Fac Engn, D-47057 Duisburg, Germany
5.Univ Duisburg Essen, CENIDE, D-47057 Duisburg, Germany
6.Southern Univ Sci & Technol SUSTech, Shenzhen Engn Res & Dev Ctr Flexible Solar Cells, Shenzhen 518055, Peoples R China
7.Southern Univ Sci & Technol SUSTech, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
8.Univ Sci & Technol China USTC, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
9.Univ Sci & Technol China USTC, Dept Phys, Hefei 230026, Peoples R China
10.Hainan Univ, State Key Lab Marine Resources Utilizat South Chin, Haikou 570228, Peoples R China

Xu, Huifen,Liang, Zheng,Ye, Jiajiu,et al. Constructing robust heterointerfaces for carrier viaduct via interfacial molecular bridges enables efficient and stable inverted perovskite solar cells[J]. ENERGY & ENVIRONMENTAL SCIENCE,2023.

Xu, Huifen.,Liang, Zheng.,Ye, Jiajiu.,Zhang, Yong.,Wang, Zihan.,...&Pan, Xu.(2023).Constructing robust heterointerfaces for carrier viaduct via interfacial molecular bridges enables efficient and stable inverted perovskite solar cells.ENERGY & ENVIRONMENTAL SCIENCE.

Xu, Huifen,et al."Constructing robust heterointerfaces for carrier viaduct via interfacial molecular bridges enables efficient and stable inverted perovskite solar cells".ENERGY & ENVIRONMENTAL SCIENCE (2023).