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Methylammonium chloride (MACl) additive is almost irreplaceable in high‐performance formamidine perovskite photovoltaics. Nevertheless, Some of the problems that can arise from adding MACl are rarely mentioned. Herein, it is proposed for the first time that the addition of MACl would cause the non‐stoichiometric ratio in the perovskite film, resulting in the halogen vacancy. It is demonstrated that the non‐synchronous volatilization of methylamine cations and chloride ions leads to the formation of halogen vacancy defects. To solve this problem, the NH4HCOO is introduced into the perovskite precursor solution to passivate the halogen vacancy. The HCOO− ions have a strong force with lead ions and can fill the halogen vacancy defects. Consequently, the champion devices' power conversion efficiency (PCE) can be improved from 21.23% to 23.72% with negligible hysteresis. And the unencapsulated device can still retain >90% of the initial PCE even operating in N2 atmosphere for over 1200 h. This work illustrates another halogen defect source in the MACl‐assisted formamidine perovskite photovoltaics and provides a new route to obtain high‐performance perovskite solar cells. [ABSTRACT FROM AUTHOR]

The perovskite photovoltaic field has developed rapidly within a decade. In particular, formamidinium (FA)‐rich perovskite allows a broad absorption spectrum, and is considered to be one of the most promising perovskite materials. Great progress has been achieved, and most recorded high‐efficient perovskite solar cells (PSCs) used the FA‐rich perovskite light absorption layer. However, the black α‐phase formamidinium lead iodide (FAPbI3) perovskite easily transforms into an undesirable δ‐phase at a low temperature. Thus, researchers have put a lot of effort into deeply understanding the phase transformation and stabilization mechanism of FA‐rich perovskite. Herein, the fundamental physical properties of FAPbI3 materials, including crystal structure, phase‐transition temperature, charge‐carrier dynamics, etc. are summarized, and establish a complete phase evolution with temperature by reviewing previous reports. The intrinsic and external factors are subsequently discussed for influencing the stability of FAPbI3 perovskite and the remarkable breakthroughs of FA‐rich PSCs in recent years are reviewed. Moreover, a series of strategies to stabilize FA‐rich perovskite is summarized, including but not limited to compositional engineering, passivating engineering, processing engineering, and strain engineering. Finally, several new viewpoints are provided for improving the efficiency and stability of PSCs. This review may be regarded as a reference project for preparing high‐efficient and stable perovskite photovoltaic devices. [ABSTRACT FROM AUTHOR]

α-Formamidinium lead iodide (α-FAPbI 3) has become one of the most promising candidate materials for stable perovskite solar cells (PSCs) owing to their outstanding optoelectronic properties and high thermal stability. The crystallinity of the active layer of perovskite is essential to the performance of perovskite solar cells. In this paper, we added lead acetate Pb(Ac) 2 as a grain growth agent into the perovskite precursor solution to prepare high-efficiency and stable perovskite solar cells. It was revealed that the crystals of Pb(Ac) 2 -modified film grew selectively along the [200] direction and that the FAPbI 3 active layer grains were arranged neatly and densely, due to the significant influence of a moderate amount of weakly acidic Ac- on the crystal growth of FAPbI 3. The relative reduction in its grain boundaries led to the decrease in the grain boundary impedance, and it was easier for electrons to perform long-range migration in the perovskite active layer. The beneficial effects of Pb(Ac) 2 were further expiored by femtosecond Fs-TA measurements and density of states (tDOS) analysis, where the carrier lifetimes τ 2 was increased from 482.4 ps to 1340 ps, and the trap density of film states was significantly reduced. The filling factor (FF) and power conversion efficiency (PCE) were increased from 76.5% and 19.7–81.1% and 21.8%, respectively, the Pb(Ac) 2 devices were placed in air for 800 h for the light aging test, and the test results still maintained 90% of the original efficiency, which improved the stability of FAPbI 3 crystals. • Pb(Ac) 2 as an additive to modulate the crystalline quality of perovskite active layer films. • Perovskite solar cell defect reduction and carrier lifetime increase by Pb(Ac) 2 modification. • The Pb(Ac) 2 -modified active layer grains have preferential orientation and orderly arrangement. • 81.1% filling factor and 21.8% efficiency are achieved for a single PSC cell with excellent stability. [ABSTRACT FROM AUTHOR]

The development of perovskite solar cells has improved rapidly. However, PSCs generally suffer from instability, due to the detrimental defects. Additive engineering is a favorable method for defect passivation. In this work, the linear pseudo-halogen salt, KSCN, is introduced into the MAPbI 3 perovskite film to improve the performance of PSC. The trap density of cells with SCN− is decreased significantly. The SCN− not only can fill halogen vacancies to reduce the halide-related defects, but also can interact with the uncoordinated Pb2+ via coordinate bond to stabilize perovskite lattice structure. Moreover, the performance of devices with other linear pseudo-halogen anions (OCN−, SeCN−) are also investigated. Due to the improved short circuit current density, the power conversion efficiency of devices increases from 18.02% (PVK) to 20.41% (PVK–SCN-), 19.53% (PVK–OCN-) and 19.23% (PVK–SeCN-), respectively. After introducing pseudo-halide anions, the devices showed robust stability under the ambient environment. [ABSTRACT FROM AUTHOR]

Organic-inorganic hybrid perovskite materials with distinctive optoelectronic properties have attracted much interest in the field of solar cells. As the light absorber, the quality of perovskite films is crucial to the performances of perovskite solar cells. Anti-solvent engineering seems to be an efficient method in preparing high-quality perovskite films, but mostly used anti-solvents are toxic, such as chlorobenzene (CB)， which is harmful to the environmental protection. In the present work, we used the green anti-solvent diethyl carbonate (DEC) instead of CB, demonstrated that the DEC engineered CH 3 NH 3 PbI 3 film exhibits improved morphology and crystallinity as well as reducing defects, which can be attributed to the interaction between DEC and the solvent dimethyl sulfoxide (DMSO). The DEC anti-solvent assisting yields efficient CH 3 NH 3 PbI 3 perovskite solar cells with a champion power conversion efficiency of 20.20% and a steady state efficiency of 86% over a period of 20 days of storage under ambient conditions. The present study provides a viable path way to design green and effective perovskite solar cells in the future. [Display omitted] • Developed a green solvent-assisted perovskite crystallization method. • Formed uniform and compact perovskite films with large grains. • High-quality perovskite films prepared by green anti-solvent diethyl carbonate. [ABSTRACT FROM AUTHOR]