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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]

Electron transport layers (ETLs) are crucial for achieving efficient and stable planar perovskite solar cells (PSCs). Reports on versatile inorganic ETLs using a simple film fabrication method and applicability for both low‐cost planar regular and inverted PSCs with excellent efficiencies (>22%) and high stability are very limited. Herein, we employ a novel inorganic ZnSe as ETL for both regular and inverted PSCs to improve the efficiency and stability using a simple thermal evaporation method. The TiO2‐ZnSe‐FAPbI3 heterojunction could be formed, resulting in an improved charge collection and a decreased carrier recombination further proved through theoretical calculations. The optimized regular PSCs based on TiO2/ZnSe have achieved 23.25% efficiency with negligible hysteresis. In addition, the ZnSe ETL can also effectively replace the unstable bathocuproine (BCP) in inverted PSCs. Consequently, the ZnSe‐based inverted device realizes a champion efficiency of 22.54%. Moreover, the regular device comprising the TiO2/ZnSe layers retains 92% of its initial PCE after 10:00 h under 1 Sun continuous illumination and the inverted device comprising the C60/ZnSe layers maintains over 85% of its initial PCE at 85 °C for 10:00 h. This highlights one of the best results among universal ETLs in both regular and inverted perovskite photovoltaics. [ABSTRACT FROM AUTHOR]

Understanding the function of moisture on perovskite is challenging since the random environmental moisture strongly disturbs the perovskite structure. Here, we develop various N2-protected characterization techniques to comprehensively study the effect of moisture on the efficient cesium, methylammonium, and formamidinium triple-cation perovskite (Cs0.05FA0.75MA0.20)Pb(I0.96Br0.04)3. In contrast to the secondary measurements, the established air-exposure-free techniques allow us directly monitor the influence of moisture during perovskite crystallization. We find a controllable moisture treatment for the intermediate perovskite can promote the mass transportation of organic salts, and help them enter the buried bottom of the films. This process accelerates the quasi-solid-solid reaction between organic salts and PbI2, enables a spatially homogeneous intermediate phase, and translates to high-quality perovskites with much-suppressed defects. Consequently, we obtain a champion device efficiency of approaching 24% with negligible hysteresis. The devices exhibit an average T80-lifetime of 852 h (maximum 1210 h) working at the maximum power point. Perovskite structure is disturbed by environmental moisture, limiting the device performance. Here, Wei et al. monitor the effect of moisture during the growth by N2-protected characterization techniques, and obtain an operationally stable perovskite solar cell with efficiency approaching 24%. [ABSTRACT FROM AUTHOR]

A novel biphenyl fumaronitrile as an acceptor and triphenylamine as donor conjugated building blocks are used for the first time to successfully synthesize donor–acceptor–donor molecule (D‐A‐D) 2,3‐bis(4′‐(bis(4‐methoxyphenyl)amino)‐[1,1′‐biphenyl]‐4‐yl)fumaronitrile (TPA‐BPFN‐TPA). The new TPA‐BPFN‐TPA with low‐lying HOMO is used as a dopant‐free hole‐transporting material (HTM) in mesoporous perovskite solar cells. The performance of the solar cells using this new HTM is compared with the traditional 2,2′,7,7′‐tetrakis(N,N′‐di‐p‐methoxyphenylamino)‐ 9,9′‐spirobifluorene (Spiro‐OMeTAD) HTM based devices for outdoor and indoor performance evaluation. Under 1 sun illumination, dopant‐free TPA‐BPFN‐TPA HTM based devices exhibit a power conversion efficiency (PCE) of 18.4%, which is the record efficiency to date among D‐A‐D molecular design based dopant‐free HTMs. Moreover, the stability of unencapsulated TPA‐BPFN‐TPA‐based devices shows improvement over Spiro‐OMeTAD‐based devices in harsh relative humidity condition of 70%. Another exciting feature of the newly developed HTM is that the TPA‐BPFN‐TPA‐based devices exhibit improved PCE of 30% and 20.1% at 1000 lux and 200 lux illuminations, respectively. This new finding provides a solution to fabricate low indoor (low light) and outdoor (1 sun) perovskite solar cell devices with high efficiency for cutting‐edge energy harvesting technology. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PSCs) employing organic-inorganic halide perovskite as active layers have attracted the interesting of many scientists since 2009. The power conversion efficiency (PCE) have pushed certified 25.2% in 2019 from initial 3.81% in 2009, which is much faster than that of any type of solar cell. In the process of optimization, many innovative approaches to improve the morphology of perovskite films were developed, aiming at elevate the power conversion efficiency of perovskite solar cells (PSCs) as well as long-term stability. In the context of PSCs research, the perovskite precursor solutions modified with different additives have been extensively studied, with remarkable progress in improving the whole performance. In this comprehensive review, we focus on the forces induced by additives between the cations and anions of perovskite precursor, such as hydrogen bonds, coordination or some by-product (e.g., mesophase), which will lead to form intermediate adduct phases and then can be converted into high quality films. A compact uniform perovskite films can not only upgrade the power conversion efficiency (PCE) of devices but also improve the stability of PSCs under ambient conditions. Therefore, strategies for the implementation of additives engineering in perovskites precursor solution will be critical for the future development of PSCs. How to manipulate the weak forces in the fabrication of perovskite film could help to further develop high-efficiency solar cells with long-term stability and enable the potential of future practical applications. [ABSTRACT FROM AUTHOR]

Abstract Zinc oxide (ZnO) as an electron transport material has been used in regular planar perovskite solar cells (PSCs). Herein, ZnO nanoparticles serve as an additive directly in perovskite active layer in order to fabricate a bulk-heterojunction inverted planar PSC. The CH 3 NH 3 PbI 3-x Cl x :ZnO bulk heterojunction is prepared by mixing ZnO nanoparticles into CH 3 NH 3 PbI 3-x Cl x precursor solution. ZnO nanoparticles act as catalytic centers and induce the growth of perovskite grains leading to the formation of large-size perovskite crystals. Remarkably, hysterysis-free power conversion efficiency of 17.26% is achieved when precisely control the concentration of ZnO nanoparticles in CH 3 NH 3 PbI x Cl 3-x :ZnO bulk heterojunction active layer. The presence of ZnO nanoparticles in the perovskite films enhances the conductivity and electron mobility. Efficient charge injection of CH 3 NH 3 PbI x Cl 3-x :ZnO film can improve charge extraction in the PSCs. Moreover, the PSCs with CH 3 NH 3 PbI x Cl 3-x :ZnO bulk heterojunction exhibit high fill factor of 77.3% and short current density of 22.71 mA cm−2, which is attributed to improved perovskite quality. The bulk heterojunction structure is fabricated by combining perovskite and metal oxides, which is of great importance to the development and commercialization of PSCs in the future. Graphical abstract Image 1 Highlights • A CH 3 NH 3 PbI 3-x Cl x :ZnO bulk heterojunction exits in the perovskite solar cell. • ZnO nanoparticles improve light harvesting efficiency of perovskite solar cell. • ZnO nanoparticles lead to the formation of large-size perovskite crystals. • ZnO nanoparticles improve conductivity and electron mobility of perovskite film. [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]