Buried Interface Regulation with a Supramolecular Assembled Template Enables High‐Performance Perovskite Solar Cells for Minimizing the <i>V</i><sub>OC</sub> Deficit

Despite the rapid development of perovskite solar cells (PSCs) in the past decade, the open-circuit voltage (V<sub>OC</sub>) of PSCs still lags behind the theoretical Shockley-Queisser limit. Energy-level mismatch and unwanted nonradiative recombination at key interfaces are the main factors detrimental to V<sub>OC</sub>. Herein, a perovskite crystallization-driven template is constructed at the SnO<sub>2</sub>/perovskite buried interface through a self-assembled amphiphilic phosphonate derivative. The highly oriented supramolecular template grows from an evolutionary selection growth via solid-solid phase transition. This strategy induces perovskite crystallization into a highly preferred (100) orientation toward out-of-plane direction and facilitated carrier extraction and transfer due to the elimination of energy barrier. This self-assembly process positively passivates the intrinsic surface defects at the SnO<sub>2</sub>/perovskite interface through the functionalized moieties, a marked contrast to the passive effect achieved via incidental contacts in conventional passivation methods. As a result, PSCs with buried interface modification exhibit a promising PCE of 25.34%, with a maximum V<sub>OC</sub> of 1.23 V, corresponding to a mere 0.306 V deficit (for perovskite bandgap of 1.536 eV), reaching 97.2% of the theoretical V<sub>OC</sub> limit. This strategy spontaneously improves the long-term operational stability of PSCs under thermal and moisture stress (ISOS-L-3: MPP, 65 °C, 50% RH, T<sub>92</sub> lifetime exceeding 1200 h).

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Publication Details

Journal
Advanced Materials
Published
2025-04-09
DOI
https://doi.org/10.1002/adma.202418011
Citations
16
Primary Topic
Perovskite Materials and Applications
Type
article
Field-Weighted Citation Impact
11.69

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article

Buried Interface Regulation with a Supramolecular Assembled Template Enables High‐Performance Perovskite Solar Cells for Minimizing the VOC Deficit

Ruijie Ma, Bingcheng Yu, Shiang Li, Zhiwei Ren et al.
16 citations
Advanced Materials
Perovskite Materials and Applications
11.69
article

Buried Interface Regulation with a Supramolecular Assembled Template Enables High‐Performance Perovskite Solar Cells for Minimizing the VOC Deficit

Ruijie Ma, Bingcheng Yu, Shiang Li, Zhiwei Ren, Jinyao Tang, Chang Sheng Yan, Zhenrong Wang, Dongyang Li, Xinhui Lu, Liren Zhang, Jiyao Zhang, Randi Azmi, Gang Li, Han Yu, Shuyan Chen, Kuan Liu, Tao Zhu, Mingliang Li, Guohao Sun, Hao Xia, Lei Cheng, Qiong Liang, Thachoth Chandran Hrisheekesh
article en
16 citations

Abstract

Despite the rapid development of perovskite solar cells (PSCs) in the past decade, the open-circuit voltage (V<sub>OC</sub>) of PSCs still lags behind the theoretical Shockley-Queisser limit. Energy-level mismatch and unwanted nonradiative recombination at key interfaces are the main factors detrimental to V<sub>OC</sub>. Herein, a perovskite crystallization-driven template is constructed at the SnO<sub>2</sub>/perovskite buried interface through a self-assembled amphiphilic phosphonate derivative. The highly oriented supramolecular template grows from an evolutionary selection growth via solid-solid phase transition. This strategy induces perovskite crystallization into a highly preferred (100) orientation toward out-of-plane direction and facilitated carrier extraction and transfer due to the elimination of energy barrier. This self-assembly process positively passivates the intrinsic surface defects at the SnO<sub>2</sub>/perovskite interface through the functionalized moieties, a marked contrast to the passive effect achieved via incidental contacts in conventional passivation methods. As a result, PSCs with buried interface modification exhibit a promising PCE of 25.34%, with a maximum V<sub>OC</sub> of 1.23 V, corresponding to a mere 0.306 V deficit (for perovskite bandgap of 1.536 eV), reaching 97.2% of the theoretical V<sub>OC</sub> limit. This strategy spontaneously improves the long-term operational stability of PSCs under thermal and moisture stress (ISOS-L-3: MPP, 65 °C, 50% RH, T<sub>92</sub> lifetime exceeding 1200 h).

Advanced MaterialsVol. 37(24)
Hong Kong Polytechnic University (HK), Chinese University of Hong Kong (HK), Hong Kong University of Science and Technology (HK), Chinese University of Hong Kong, Shenzhen (CN), State Key Laboratory of Synthetic Chemistry (CN), University of Hong Kong (HK)
Croucher Foundation, National Natural Science Foundation of China, Guangdong Science and Technology Department, Centers for Disease Control and Prevention
Affordable and clean energy
Openalex Percentile: Top 1%
Perovskite Materials and Applications
11.69
DOIOpen Access PDFOpenAlex
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