Phenylethylammonium Bis(trifluoromethylsulfonyl)imide as a Spontaneous Perovskite Passivator Effectively Combined with PTAA Hole Transport Material in Perovskite Solar Cells
Naoyuki Nishimura a, Hiroyuki Kanda a, Ryuzi Katoh b, Atsushi Kogo a, Takurou N. Murakami a
a National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Japan, 日本、〒305-0046 茨城県つくば市東1丁目1−1, つくば市, Japan
b Nihon University, College of Engineering, 1 Nakagawara, Tokusada, Tamura, Koriyama, Japan
Proceedings of Asia-Pacific Conference on Perovskite, Organic Photovoltaics&Optoelectronics (IPEROP25)
Kyoto, Japan, 2025 January 19th - 21st
Organizers: Atsushi Wakamiya and Hideo Ohkita
Poster, Naoyuki Nishimura, 057
Publication date: 4th October 2024

Perovskite passivation has become instrumental for obtaining highly efficient and durable perovskite solar cells (PSCs). Phenylethylammonium (PEA)-based passivator is one of the most major categories as it is effective in improving PSC performances taking advantages of its large adsorption energy over perovskite surface. Thus, combining PEA-based passivators with thermally stable poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) hole transport material (HTM) is promising strategy to contracting highly efficient and durable PSCs, in principle. However, the conventional PEA-based passivation suffers from thermal stability issues; under thermal stress even at moderate temperatures for a short duration (e.g., 50 °C for several minutes), the overlayer of the perovskite passivated with PEA iodide transforms to a two-dimensional (2D) perovskite of (PEA)2PbI4 (n = 1), which hampers carrier transfer, thus negating the passivation effects and/or degrading the photovoltaic (PV) performances. [1, 2]

Herein, we propose a novel and simple strategy to address the thermal stability issues using a newly synthesized PEA bis(trifluoromethylsulfonyl)imide (PEA-TFSI) additive for PTAA HTM.[3] During the HTM deposition with the PEA-TFSI additive over perovskite layers, the PEA cations spontaneously passivated the perovskite presumably exploiting the large adsorption energy, forming a monolayer-like passivation overlayer. The resulting PEA-based passivation did not exhibit crystallization to the detrimental 2D perovskite at 85°C; hence, it did not cause PV performance drop due to the thermal stress. The PSCs with optimal PEA-TFSI addition resulted in effectively enhanced PV performances, achieving a 22.1% power conversion efficiency. The PV performance enhancement can be attributed to both the improved affinity at the PTAA/perovskite interface, which is crucial in combining PTAA HTMs yet hardly attainable by aliphatic-ammonium-based passivators, and the PEA passivation effects. This study provides novel insights into widely used PEA-based passivators and paves the way for perovskite passivation effectively combined with thermally stable PTAA HTMs.

This study was supported by the project JPNP21016, commissioned by the New Energy and Industrial Technology Development Organization (NEDO).

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