Chen Hui, Cao Qi, Pu Xingyu, Zhao Qingyuan, He Xilai, Zhou Zihao, Wang Tong, Feng Guangpeng, Yin Ranhao, Chen Zhongwei, Tajibaev Ilkhom, Boynazarov Ilkhom, Bai Yijun, Jia Shiyao, Li Xuanhua
State Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an, 710072, China.
Key Laboratory of Physics and Technology for Advanced Batteries (Ministry of Education), College of Physics, Jilin University, Changchun, 130012, China.
Adv Mater. 2025 Aug 11:e10553. doi: 10.1002/adma.202510553.
Self-assembled molecules (SAMs) deposited on nickel oxide (NiO) are the basis for achieving high-performance inverted perovskite solar cells (PSCs). Unfortunately, the dissolution and redeposition of SAMs caused by the perovskite precursors leads to leaky monolayers, resulting in perovskite degradation and reduced stability. Here, a novel method is reported to realize strong coupling between NiO and SAMs via inserted reductant [9tris(2-carboxyethyl)phosphine hydrochloride (TCEP)] for an integrated NiO-SAMs hole transport layer (HTL). TCEP reduces NiO and in situ forms C═O···Ni coordinated bond and O─H···O─Ni hydrogen bond, while its -COOH is connected with SAM's -PO(OH) by phosphonate and hydrogen bond, which improve the compactness of SAMs, thereby strengthening hole extraction and lowering interfacial non-radiative recombination. Simulation calculations demonstrate that the HTL strongly coupled by TCEP has a stronger adsorption energy, significantly improving device long-term stability. Therefore, the device based on integrated NiO-SAMs HTL obtains a substantial efficiency of 26.34%. The devices maintain an impressive 97.5% of their original efficiency after 1000 h of operation under 1-sun illumination and 90.1% after 1000 h of thermal treatment at 85 °C in nitrogen atmosphere. This work offers new horizons for designing NiO-based HTLs with high SAMs coverage for high-performance PSCs.
