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Tin‐lead (Sn‐Pb) mixed perovskite with a narrow bandgap is an ideal candidate for single‐junction solar cells approaching the Shockley‐Queisser limit. However, due to the easy oxidation of Sn2+, the efficiency and stability of Sn‐Pb mixed perovskite solar cells (PSCs) still lag far behind that of Pb‐based solar cells. Herein, highly efficient and stable FA0.5MA0.5Pb0.5Sn0.5I0.47Br0.03 compositional PSCs are achieved by introducing an appropriate amount of multifunctional Tin (II) oxalate (SnC2O4). SnC2O4 with compensative Sn2+ and reductive oxalate group C2O42− effectively passivates the cation and anion defects simultaneously, thereby leading to more n‐type perovskite films. Benefitting from the energy level alignment and the suppression of bulk nonradiative recombination, the Sn‐Pb mixed perovskite solar cell treated with SnC2O4 achieves a power conversion efficiency of 21.43%. More importantly, chemically reductive C2O42− effectively suppresses the notorious oxidation of Sn2+, leading to significant enhancement in stability. Particularly, it dramatically improves light stability. [ABSTRACT FROM AUTHOR]

The poor film stability of Sn-Pb mixed perovskite film and the mismatched interface energy levels pose significant challenges in enhancing the efficiency of tin–lead (Sn-Pb) mixed perovskite solar cells. In this study, polyvinylpyrrolidone (PVP) is introduced into the PVK perovskite precursor solution, effectively enhancing the overall stability of the film. This improvement is achieved through the formation of robust coordination bonds between the carbonyl (C=O) in the pyrrole ring and the undercoordinated SnII and PbII, thereby facilitating the passivation of defects. Furthermore, the introduction of PVP inhibits the oxidation of tin (Sn), thereby enhancing the n-type characteristics of the perovskite film. This adjustment in the energy level of the PVK perovskite film proves instrumental in reducing interface energy loss, subsequently improving interface charge transfer and mitigating device recombination. Consequently, perovskite solar cells incorporating PVP achieve an outstanding champion power conversion efficiency (PCE) of 21.31%. [ABSTRACT FROM AUTHOR]

Electron transport layer (ETL)‐free perovskite solar cells (PSCs) have witnessed great progress via material and interface engineering. Enlighten by the wisdom from an old story of efficient silicon solar cells design, highly efficient MINP (metal/insulator/n‐type perovskite/p‐type spiro‐MeOTAD) PSC with polar insulating inter‐layer (PIIL) modified fluorine‐doped tin oxide (FTO) is reported as electron selective contact. The PIIL forms metal‐insulator‐semiconductor (MIS) junction with FTO and perovskite layer, while the n‐type perovskite forms P‐N junction with p‐type spiro‐MeOTAD. Unlike the classic MINP silicon solar cells where the I‐layer is usually neutral tunneling layer, the PIIL here optimizes the energy level alignment at the FTO/perovskite interface with its intrinsic electronic polarity while acting as an effective tunneling layer. Also, the functional group of the PIIL passivates the FTO/perovskite interface defects thus suppressing carrier recombination thereof and enhancing all device performance parameters simultaneously. Accordingly, the power conversion efficiency is greatly improved from 12.82% to 19.75%. With the enhanced electron collection and decreased carrier recombination of the MIS junction, this collaborative effect of interface engineering and defect passivation contribute to more stable ETL‐free PSC with less hysteresis. This work highlights the potential of novel device and interface design for simple‐structured, efficient and cost‐effective PSCs. [ABSTRACT FROM AUTHOR]

Efficient electron transport layer–free perovskite solar cells (ETL‐free PSCs) with cost‐effective and simplified design can greatly promote the large area flexible application of PSCs. However, the absence of ETL usually leads to the mismatched indium tin oxide (ITO)/perovskite interface energy levels, which limits charge transfer and collection, and results in severe energy loss and poor device performance. To address this, a polar nonconjugated small‐molecule modifier is introduced to lower the work function of ITO and optimize interface energy level alignment by virtue of an inherent dipole, as verified by photoemission spectroscopy and Kelvin probe force microscopy measurements. The resultant barrier‐free ITO/perovskite contact favors efficient charge transfer and suppresses nonradiative recombination, endowing the device with enhanced open circuit voltage, short circuit current density, and fill factor, simultaneously. Accordingly, power conversion efficiency increases greatly from 12.81% to a record breaking 20.55%, comparable to state‐of‐the‐art PSCs with a sophisticated ETL. Also, the stability is enhanced with decreased hysteresis effect due to interface defect passivation and inhibited interface charge accumulation. This work facilitates the further development of highly efficient, flexible, and recyclable ETL‐free PSCs with simplified design and low cost by interface electronic structure engineering through facile electrode modification. [ABSTRACT FROM AUTHOR]

To realize high-performance perovskite solar cells (PSCs) ensuring low-cost flexible application with low energy consumption, efficient electron transport layers (ETL) that can be processed at low temperatures are desired. In this contribution, low temperature (about 70 °C) UV/ozone irradiation was applied to synthesis crystallized TiO 2 films as ETL. The UV exposure induces photo-catalytic removal of the organic ligands and spontaneous coalescence of the TiO 2 framework, resulting in excellent TiO 2 films with considerable crystallinity. UV irradiation induces both complete removal of organic media and more efficient charge collection. Accordingly, planar heterojunction (PH) PSCs with such ETL exhibited outstanding photovoltaic performance up to 17.03%, which is even higher than the value (12.98%) of counterpart device with high temperature thermal sintered TiO 2 ETL (without TiCl 4 treatment). These low temperature solution-processed TiO 2 films by facile UV irradiation are suitable for the low-cost, large yield solution process on a flexible substrate for photoelectric devices. [ABSTRACT FROM AUTHOR]

Silver nanowire (Ag NW)-based transparent back electrodes prepared via all solution-process are promising for bifacial and semitransparent perovskite solar cells (PSCs). However, the inadequate electrical contact between the silver nanowires themselves and the contact with substrate leads to reduced overall solar cell performance; meanwhile, serious corrosion of Ag NW in ambient environment restricting the further applications. In this work, polyvinylpyrrolidone (PVP) as a binder in Ag NW electrode significantly enhances the conductivity and transparency at the same time improving the interface electric contact. The PSC with PVP modified Ag NW electrode demonstrated frontside and backside efficiency approaching 18 % and 14.1 % (AM1.5, 1 Sun), respectively, which achieves 82 % efficiency with normal Ag device and bifacial factor of 79 %. The long-term storage stability of PSC is also improved by PVP protection. The final device structure is ITO/Ni O x /MeO/(FA0.92MA0.08)0.95Cs0.05Pb(I0.9Br0.1)3/PEAI/PC61BM/BCP/ Ag NW. This work highlights the method to fabricate robust transparent Ag NW electrode for bifacial perovskite solar cells. • Polyvinylpyrrolidone (PVP) in Ag nanowire (Ag NW) electrode significantly enhances the conductivity and transparency. • PVP modified Ag NW electrode improves the interface electric contact and charge transport of the solar cell. • The Perovskite solar cell (PSC) with PVP modified Ag NW electrode demonstrated high efficiency and bifacial factor. • The long-term storage stability of PSC is also improved by PVP protection. [ABSTRACT FROM AUTHOR]

• 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]

Inorganic nickel oxide (NiO x)-based inverted perovskite solar cells (PSCs) are reported to be more stable compared to those using organic hole transport layer materials. However, the Fermi level of NiO x is relatively away from the valence band of perovskite (PVK) layer, causing a large energy level shift at the NiO x /PVK interface and a weak built-in electric field strength. These increase the possibility of recombination, reduce the effective charge collection, seriously affect the efficiency of the device. In this work, an interface dipole with -CF 3 end group is anchored to the NiO x /PVK interface, leading to a more matched energy level structure and greatly reducing the energy barrier at the NiO x /PVK interface. Moreover, the addition of Si-CF 3 significantly improves the conductivity of NiO x and blunts the defects to large extent. The dipole interlayer significantly improves the built-in electric field and thus increases the photovoltage. Ultimately, the modified device achieves a score of 19.58% efficiency, much better than 17.98% of the control device. [Display omitted] [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]

• The fluorine atom has induced electrostatic potential and dipole moment change. • Cl- doping can enhance crystallization and prevent phase change. • The champion device achieves a PCE of 16.29% and the humidity stability is improved. [Display omitted] All-inorganic CsPbI 2 Br material has attracted considerable attention due to its good balance between phase stability and absorption capacity. However, the power conversion efficiency (PCE) and device stability of CsPbI 2 Br-based perovskite solar cells (PSCs) still lag far behind those of their counterparts, mainly deriving from the notoriously poor moisture stability under humid environment and large serious charge recombination. Herein, a typical phenethylammonium chlorine (PEACl) and its fluorinated derivative 4-fluoro-phenethylammonium chlorine (F-PEACl) are individually incorporated to modify the surface of CsPbI 2 Br film to ameliorate the above issues. Benefiting from the comprehensive passivation effect of ammonium halogen, the trap states of treated CsPbI 2 Br are vastly suppressed. In particular, fluorination significantly increased the dipole moment and hydrophobic property of F-PEACl. Thus, the present CsPbI 2 Br PSC achieves a champion PCE of 16.29% with high open-circuit voltage of 1.272 V, while the reference device and PEACl-treated device yield PCEs of 14.30% and 15.64%, respectively. More importantly, the PSC with F-PEACl capping layer retains 87.2% of its initial PCE after 1000 h storage under 20% RH ambient without encapsulation. Our results reveal the underlying mechanism of performance improvement by surface passivation strategy and provide an effective approach to further boost the CsPbI 2 Br PSC efficiency and stability. [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]