The photovoltaic performance of perovskite solar cells (PSCs) is immensely related to the perovskite film quality, defect states density, and interfacial energy‐level alignment. Herein, a self‐polymeric monomer of N‐(hydroxymethyl) acrylamide (HAM) with CC, CO, and –NH multifunctional groups is introduced in the preparation of a CsPbBr3 film by a two‐step method to regulate the crystallization process and band structure and simultaneously passivate the dual‐ionic defects. The results show that the HAM monomer first undergoes a pre‐polymerization in the CsBr precursor aqueous solution after preheating to retard the crystallization of CsPbBr3, and subsequently a further polymerization occurs during the annealing of the perovskite film to load at grain boundaries and form the CO⋯Pb (Cs) Lewis acid–base coordination and N–H⋯Br hydrogen bonding. Consequently, a large‐grained CsPbBr3 film with low defect density and optimized band structure is fabricated to effectively suppress nonradiative recombination and accelerate carrier extraction and transport, delivering a champion power conversion efficiency of 9.05% for the HAM‐incorporated CsPbBr3 PSCs, which is much higher than 6.50% efficiency for the reference one. Furthermore, the unencapsulated device maintains over 92% of the initial efficiency after 30 days storage in air with 85% relative humidity or at 85 °C, exhibiting superior moisture and thermal durability.
The incorporation of an inorganic hole transport material (HTM) with high hole mobility and matched energetics at the back interface of perovskite/carbon plays a major role in improving the power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs). Here, M3+ (M = Sc, Y, and La)-doped CuAlO2, CuAl(M)O2, with superior p-type conductivity and suitable energy band is inserted between the CsPbBr3 perovskite layer and carbon electrode as an efficient HTM to enhance hole extraction and reduce energy loss within carbon-based CsPbBr3 PSCs. The balance between the increased interstitial oxygen concentration and the carrier scattering caused by the lattice distortion of CuAl(M)O2 endows a higher hole mobility of CuAl(Sc)O2, giving a substantially increased PCE of 10.13% of the CuAl(Sc)O2 tailored CsPbBr3 PSCs, compared with the 6.5% efficiency of the device without HTMs. Moreover, the CuAl(Sc)O2-based CsPbBr3 PSCs without packaging still have 90% of the original efficiency after being stored for 720 h in an air environment with a relative humidity of 85% at 85 °C, exhibiting an outstanding long-term humidity-thermal tolerance.
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