To achieve high-quality perovskite solar cells (PSCs), the morphology and carrier transportation of perovskite films need to be optimized. Herein, C60 is employed as nucleation sites in PbI2 precursor solution to optimize the morphology of perovskite films via vapor-assisted deposition process. Accompanying the homogeneous nucleation of PbI2, the incorporation of C60 as heterogeneous nucleation sites can lower the nucleation free energy of PbI2, which facilitates the diffusion and reaction between PbI2 and organic source. Meanwhile, C60 could enhance carrier transportation and reduce charge recombination in the perovskite layer due to its high electron mobility and conductivity. In addition, the grain sizes of perovskite get larger with C60 optimizing, which can reduce the grain boundaries and voids in perovskite and prevent the corrosion because of moisture. As a result, we obtain PSCs with a power conversion efficiency (PCE) of 18.33% and excellent stability. The PCEs of unsealed devices drop less than 10% in a dehumidification cabinet after 100 days and remain at 75% of the initial PCE during exposure to ambient air (humidity > 60% RH, temperature > 30 °C) for 30 days.
The synthesis and growth of CH3NH3PbI3 films with controlled nucleation is a key issue for the high efficiency and stability of solar cells. Here, 4-tert-butylpyridine (tBP) was introduced into a CH3NH3PbI3 antisolvent to obtain high quality perovskite layers. In situ optical microscopy and X-ray diffraction patterns were used to prove that tBP significantly suppressed perovskite nucleation by forming an intermediate phase. In addition, a gradient perovskite structure was obtained by this method, which greatly improved the efficiency and stability of perovskites. An effective power conversion efficiency (PCE) of 17.41% was achieved via the tBP treatment, and the high-efficiency device could maintain over 89% of the initial PCE after 30 days at room temperature.
Two-dimensional/three-dimensional (2D/3D) Ruddlesden-Popper perovskite materials have shown the enormous potential to achieve both efficient and stable photovoltaic devices for commercial applications. Unfortunately, the single function of spacer cations limits their further improvements in efficiency to reach values as high as those of 3D perovskites. Herein, we developed a new-type multifunctional heterocyclic-based spacer cation of 2-(methylthio)-4,5-dihydro-1H-imidazole (MTIm+) to achieve a synchronous improvement of efficiency and stability for 2D/3D perovskite solar cells (PSCs). Owing to the presence of special chemical groups (imidazole and methylthio), strong interactions have been found between MTIm+ and the 3D perovskite component, leading to an excellent passivation effect. More important, at the initial stage of crystallization, uniform nucleation distribution would be generated around the spacer cation, which is helpful for improved crystallinity and reduced growth defects. The smaller layer space compared to that of cations based on aromatic hydrocarbons caused effective carrier transfer between inorganic layers in 2D/3D perovskites. As a result, the 2D/3D (n = 30) PSCs based on MTIm exhibit a champion PCE up to 21.25% with a high Voc of 1.14 V. Besides, the 2D/3D perovskite devices have realized dramatically enhanced humidity and thermal stability, maintaining 94% of the starting PCE enduring aging at about 50% RH for 2880 h and at 85 °C for 360 h, respectively. We believe that it would provide a significant strategy to further promote the photovoltaic performances and the long-term stability of 2D/3D perovskite devices toward future practical applications.
The preparation of a high‐quality CuSCN thin film is very important to guarantee its efficient performance in an electronic device. Herein, a coordination strategy is reported for the formation of a highly compact CuSCN hole‐transporting layer by retarding fast crystallization via constructing intermediate adducts, and investigated its application for perovskite solar cells (PSCs). Specifically, the strong coordination bond between CuSCN and pyridine derivate ligands results in the formation of a stable intermediate phase, which is further converted to compact CuSCN layers under thermal annealing. The configuration of the intermediate phase is demonstrated to be crucial for the subsequent assembly of high‐quality CuSCN layers and results in an improved performance of the devices. CuSCN thin films crystallized from an intermediate adduct, CuSCN‐(Cl‐Py), with a rippled sheet configuration show an exceptional surface uniformity and high hole mobility, which facilitates efficient hole extraction and suppresses charge recombination in PSCs, resulting in an enhanced device efficiency of 19.19%. That is the highest value of the inverted planar PSCs using CuSCN as a hole‐transporting layer to the best of the authors’ knowledge. This novel coordination strategy can be expected to be used in the preparation of other inorganic charge transporting materials for electronic devices.
'/%3e%3cuse xlink:href='%23a' transform='rotate(23.036 .093 25.536)'/%3e%3cuse xlink:href='%23a' transform='rotate(45.87 1.273 16.18)'/%3e%3cuse xlink:href='%23a' transform='rotate(69.945 .996 12.078)'/%3e%3cuse xlink:href='%23a' transform='rotate(20.66 -19.689 31.932)'/%3e%3c/svg%3e)