Geng Shaoyu, Zhang Song, Shen Nan, Qu Geping, Shen Haojiang, Hu Jiayu, Yang Jie, Jin Yeming, Li Ya, Cao Ruirui, Li Huayang, Shen Zhitao, Xu Zong-Xiang, Chen Shi, Jen Alex K-Y
Henan Key Laboratory of Quantum Materials and Quantum Energy, School of Future Technology, Henan University, Zhengzhou, 450046, China.
Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, Hong Kong, 999077, China.
Angew Chem Int Ed Engl. 2025 May 26;64(22):e202424910. doi: 10.1002/anie.202424910. Epub 2025 Mar 30.
Fabricating high-quality perovskite layers is essential for achieving high-performance solar cells. Considering the significant advancements made in additive engineering for optimizing perovskite crystallization using single additive, exploring the collaborative effect of dual additives on precursor for perovskite crystallization may be an effective way for further advancing device performance. Herein, a binary additives strategy is proposed, where phenylmethylammonium iodide (PMAI) and [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) are introduced into the precursor. Compared with the precursor with no additives or a single additive (PMAI or 2PACz), the use of dual additives more effectively cleaves edge-shared Pb-I octahedra to expedite the transformation from PbI to PbI complexes as prenucleation clusters and produces much larger colloidal particles with accelerated nucleation. Concurrently, the crystallization in both spin-coating and annealing processes is significantly retarded due to the stronger interaction between perovskite and binary additives. Benefiting from such rapid nucleation and slow crystallization, high-quality perovskite layer with larger-sized crystals and fewer defects is formed, resulting in mitigated microstrain, enhanced charge extraction, and suppressed nonradiative recombination. Consequently, the device derived from the use of dual additives could achieve an impressive efficiency of 26.05% (certified 25.49%) and retained 90% of its initial efficiency after 1200 h of maximum power point tracking.
制造高质量的钙钛矿层对于实现高性能太阳能电池至关重要。考虑到在使用单一添加剂优化钙钛矿结晶的添加剂工程方面取得的重大进展，探索双添加剂对钙钛矿结晶前驱体的协同作用可能是进一步提高器件性能的有效途径。在此，提出了一种二元添加剂策略，即将苯基甲基碘化铵（PMAI）和[2-(9H-咔唑-9-基)乙基]膦酸（2PACz）引入前驱体中。与不含添加剂或单一添加剂（PMAI或2PACz）的前驱体相比，使用双添加剂能更有效地裂解边共享的Pb-I八面体，以加速从PbI到作为预成核簇的PbI 络合物的转变，并产生更大的胶体颗粒且成核加速。同时，由于钙钛矿与二元添加剂之间更强的相互作用，旋涂和退火过程中的结晶都显著延迟。受益于这种快速成核和缓慢结晶，形成了具有更大尺寸晶体和更少缺陷的高质量钙钛矿层，从而减轻了微应变，增强了电荷提取，并抑制了非辐射复合。因此，使用双添加剂制备的器件可实现令人印象深刻的26.05%的效率（认证效率为25.49%），并且在最大功率点跟踪1200小时后仍保留其初始效率的90%。
