<p>The phase instability of perovskite materials remains a significant obstacle to their practical application in photovoltaics. Herein, we present a high-configurational-entropy strategy based on formamidinium ion (FA<sup>+</sup>) to fabricate the photoactive phase-stable halide perovskites through incorporating 2-amino-1,3,4-thiadiazole (2NTD). 2NTD optimally balances interactions with the [PbI<sub>6</sub>]<sup>4–</sup> octahedral frameworks while enhancing the rotational freedom of FA<sup>+</sup>. This synergistic effect amplifies FA<sup>+</sup> anisotropy and elevates configurational entropy. Moreover, 2NTD effectively inhibits the formation of I<sub>2</sub>/I<sub>3</sub><sup>–</sup> species and passivates the associated trap-state, thereby reducing the self-degradation behavior within perovskite films caused by undesirable iodine species. This improvement significantly enhances the crystallization and phase-stability of the perovskites under I<sub>2</sub>-rich conditions. Consequently, efficiencies of 26.63% (certified 26.40%) for a 0.09-cm<sup>2</sup> inverted PSCs, 25.34% for a 1-cm<sup>2</sup> device, and 23.08% for a 12.96-cm<sup>2</sup> mini-module were obtained. Moreover, the target device exhibits a minimized non-radiative voltage loss of 69 mV and an improved long-term operational stability.</p>

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Entropy-driven strategy stabilizes photoactive halide perovskites for inverted solar cells

  • Xin Chen,
  • Wei Hui,
  • Qi Wang,
  • Ping Xu,
  • Zhilu Xu,
  • Ben Fan,
  • Lin Song,
  • Xiaopeng Xu,
  • Yihui Wu,
  • Qiang Peng

摘要

The phase instability of perovskite materials remains a significant obstacle to their practical application in photovoltaics. Herein, we present a high-configurational-entropy strategy based on formamidinium ion (FA+) to fabricate the photoactive phase-stable halide perovskites through incorporating 2-amino-1,3,4-thiadiazole (2NTD). 2NTD optimally balances interactions with the [PbI6]4– octahedral frameworks while enhancing the rotational freedom of FA+. This synergistic effect amplifies FA+ anisotropy and elevates configurational entropy. Moreover, 2NTD effectively inhibits the formation of I2/I3 species and passivates the associated trap-state, thereby reducing the self-degradation behavior within perovskite films caused by undesirable iodine species. This improvement significantly enhances the crystallization and phase-stability of the perovskites under I2-rich conditions. Consequently, efficiencies of 26.63% (certified 26.40%) for a 0.09-cm2 inverted PSCs, 25.34% for a 1-cm2 device, and 23.08% for a 12.96-cm2 mini-module were obtained. Moreover, the target device exhibits a minimized non-radiative voltage loss of 69 mV and an improved long-term operational stability.