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• The oxidative I 2 /I 3 − in Sn-Pb perovskite is effectively eliminated to stabilize Sn2+. • The movable I− is successfully neutralized, protecting the Ag counter electrode from corrosion. • The solar cell device shows promoted photovoltage and efficiency with enhanced stability. In recent hotly researched tin–lead (Sn-Pb) mix perovskite solar cells (PSCs), the oxidation of Sn2+ is not an isolated process but accompanied by the oxidation of I− to I 2 , which are both responsible for the severe p-doping and complex defect situation. Diffusion of interstitial I further severely corrodes the metal electrode to fail the PSC. Thereby, managing the I− oxidation and meanwhile neutralizing the movable I− together with suppressing Sn2+ oxidation is quite a challenge for efficient and stable Sn-Pb PSCs. In this work, a natural reductive amino acid (DOPA) is introduced into perovskite layer to successfully inhibit the oxidation of both Sn2+ and I−, at the same time, neutralize the diffusive I− to protect the Ag electrode from corrosion. Benefiting from the improved chemistry situation, the DOPA doped PSC shows significantly promoted photovoltage and efficiency at AM1.5, with enhanced light and shelf stability. This work highlights the importance of I defects management to achieve efficient and stable Sn-Pb PSCs. [ABSTRACT FROM AUTHOR]

• Formation of (TMA) x FA 1-x Pb(PF 6) x I 3-x /FAPbI 3 heterojunction through interface ion exchange. • Strong hydrogen bonding and ion size effect stabilize the phase structure. • A champion efficiency of 21.43% was obtained with greatly enhanced device stability. Though formamidinium lead triiodide FAPbI 3 is hotly researched, it still suffers from chemical and phase instabilities, arising from inherent weak chemical bonding and easily transformed crystal configures respectively. This induces depraved opto-electronic properties and device instability, which is imperative to be solved. Here, chemical interaction enhancement in heterostructure of (TMA) x FA 1-x Pb(PF 6) x I 3-x /FAPbI 3 simultaneously improves the chemical and phase stability with preserving its inherent bandgap. Strong hydrogen bonding between PF 6 - and FA+ drastically reduces the α phase formation energy and diminishes the interface trap states. The resulting perovskite solar cells achieve improved efficiency of 21.43% compared with 19.32% of the control device. Meanwhile, ∼90% and 80% of the initial efficiency are maintained for unpacked devices after 1200 h storage (25 °C, 30% relative humidity) and 300 h maximum power point tracking (1 sun, 25 °C, N 2), outperforming the control one. This work highlights a robust interface construction method to overcome the inherent problem of FAPbI 3. [ABSTRACT FROM AUTHOR]