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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]

[Display omitted] • A facile surface modification method using alkylamines to treat the CsPbI 3 surface is proposed. • HDA treatment can ameliorate defect passivation and energy level alignment to reduce voltage loss. • A champion PCE of 18.21% is achieved for the HDA-treated inverted CsPbI 3 PSCs. • HDA treatment promotes the humidity stability both of CsPbI 3 films and solar cells. Inorganic CsPbI 3 perovskite has been regarded as a kind of promising light-harvesting material due to its outstanding photoelectrical characteristics especially in perovskite solar cells (PSCs). However, there are still some problems hindering its further development, among which non-radiative recombination induced by traps and voltage loss are very pivotal. Here, the passivation of surface defects and energy level alignment of perovskite films are greatly ameliorated by facile surface modification with alkylamines. It is found that the undercoordinated Pb2+ are effectively passivated by the terminal amino group, leading to significantly reduced surface trap density, while the charge lifetime of treated perovskite films is prolonged. Besides, the bilateral amino groups from hexanediamine (HDA) can provide additional hydrogen bond to coherently connect the PbI 6 4− octahedra. Moreover, gradient energy levels are created after surface treatment, which promote the carriers transfer and reduce the voltage deficit. Consequently, a champion power conversion efficiency (PCE) of inverted CsPbI 3 PSCs over 18 % with higher fill factor (FF) of 81.21 % and open circuit voltage (V OC) of 1.10 V is obtained compared to the pristine device with a lower PCE of 12.69 % (V OC of 1.01 V, and FF of 62.49 %). Besides, the unencapsulated device with HDA treatment exhibits good stability with keeping 80 % of its initial efficiency after being aged for 1000 h at 35 % relative humidity. Our work can offer a facile but effective approach for the development of highly efficient and stable inverted CsPbI 3 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]

[Display omitted] • HEMA additive was added to the CsPbI 2 Br precursor solution to improve crystallization. • HEMA molecules could passivate defects and suppress charge recombination. • A champion efficiency of 16.13% was obtained with greatly enhanced device stability. CsPbI 2 Br all-inorganic perovskite has attracted considerable attention due to its high thermal stability and suitable bandgap, while the unsatisfactory crystallization quality and moisture instability significantly hinder its further application. Herein, a novel multifunctional liquid additive, 2-hydroxyethyl methacrylate (HEMA), is introduced into the CsPbI 2 Br precursor to ameliorate the above issues. Our results demonstrate that the functional groups of HEMA can interact with perovskite precursor, thus improving crystallization and passivating defects at the same time, and leading to a champion power conversion efficiency of up to 16.13%. Importantly, HEMA molecule in perovskite films will polymerize to a hydrophobic polymer at grain boundaries through breaking C = C bonds during the high temperature annealing process (160 °C). Moreover, this multifunctional liquid additive strategy endows perovskite films with promoted moisture tolerance by crosslinking perovskite grains and blocking moisture penetration, thus the unencapsulated device maintains 78% of its initial efficiency after aging at 30% relative humidity for 1000 h. These results demonstrate that the additive engineering with multifunctional molecule is applicable strategy for developing CsPbI 2 Br all-inorganic perovskite solar cells with both high efficiency and stability. [ABSTRACT FROM AUTHOR]