The thermodynamical deprotonation of methylammonium chloride (MACl) has several detrimental influences on the quality of formamidinium (FA+)-based perovskite, which limits both efficiency and stability of inverted perovskite solar cells (IPSCs). Herein, a new additive strategy was developed by introducing methyl carbamimidothioate hydroiodide (MCH) into perovskite precursor, where guanylation reaction occurred between MCH and MACl to form a new intermediate of methyl-substituted guanidine (MSG). MSG could then bond with undercoordinated Pb2+ to in-situ form a two-dimensional (2D) perovskite, which would promote the growth and crystallization of three-dimensional (3D) perovskite with higher crystallinity, lower defect-states density and superior stability. Finally, the MCH-treated IPSC with a small area (0.09 cm2) achieved an impressive power conversation efficiency (PCE) of 26.81% (certified as 26.02%), which is one of the highest PCEs reported to date. The large area MCH-treated device (1.00 cm2) also obtained a high PCE of 24.36%. Moreover, the unencapsulated and MCH-treated device exhibited excellent operational stability, maintaining 91.95% and 97.06% of their initial efficiencies after aging in air and a nitrogen-filled atmosphere at 85 oC for 1200 h. The encapsulated MCH-treated devices retained 94.25% of its initial efficiency after continuously tracking at the maximum power-point for 1200 h in air.

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http://dx.doi.org/10.1002/anie.202419070DOI Listing

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