Despite inorganic CsPbI3−xBrx perovskite solar cells (PSCs) being promising in thermal stability, the perovskite degradation and severe nonradiative recombination at the interface hamper their further development. Herein, the typical MXene material, that is, Ti3C2Tx, is employed to be the buried interface prior to the perovskite absorber layer in the device, which multi‐functionalizes the as‐prepared electron‐transfer layers by means of both fascinating preferential crystallization of perovskite and/or accelerating the charge extraction with respect to an ideal energy‐level alignment and suppressed trap states. Accordingly, the power conversion efficiency of the modified PSC device is substantially enhanced by as high as 19.56% in comparison to their counterparts with only the pristine CsPbI3−xBrx active layer. More importantly, MXene modification is favorable to improve the wettability of perovskite precursor solution with enhanced grain size and crystallinity, thereby increasing the UV long‐term stability of solar cells. This work provides a new paradigm toward alleviating the severe nonradiative recombination at the interface in the device whilst enhancing the long‐term stability via the preferential crystallization process.
The fast‐track development in all‐inorganic perovskite photovoltaics for high efficiency are still facing the defect issues including vacancy, undercoordinated ions, and dislocation at the surface/interface of perovskite materials. Herein, three kinds of small‐molecules difluorobenzylamine (DFBA) are found to act as the interfacial modification materials to stabilize and enhance the efficiency of all‐inorganic carbon perovskite CsPbI3–xBrx solar cell. The fluorine atoms with different positions in the benzene ring are demonstrated by the density‐functional theory simulations and experiments to passivate the defect at the surface/interface of perovskites, boosting the photocarrier transfer. Accordingly, the most suitable 2,6‐DFBA is used to modify the perovskite to prepare hole‐transporting materials‐free carbon‐based CsPbI3–xBrx (X = 0.3) perovskite solar cells, and the interface‐modified device yields a power conversion efficiency (PCE) of 14.6%, the open‐circuit voltage is increased to 1.14 V, and the PCE of the unpackaged device remained at 92% of the initial PCE after 1680 h of storage at 20–30% air humidity.
Low‐dimensional organic–inorganic hybrid perovskites (OIHPs) with broadband emission attract immense scientific interest due to their potential application for the next generation of solid‐state lighting. However, due to low exciton utilization, organic cations generally adjust structure rather than contribute the band edge to affect optical properties. Based on this, OIHPs are usually allowed to obtain a low photoluminescence quantum yield (PLQY). Herein, a good charge transfer carrier (p‐phenylenediamine, PPDA) as organic cation is rationally employed and a novel indium‐based perovskite is synthesized. By coupling with H2O molecules, a strong interaction between organic and inorganic components is realized by hydrogen bonding, which has good transportability and greatly improves the exciton utilization. The regions of hydrogen bonding show high electron mobility, combined with the induced recombination center, improving the progress of charge relaxation. As a result, the regulation of hydrogen bond strength based on the microstructure optimization directly determines the optical emission intensity, realizing nearly 100% PLQY. Further, the polyhydrogen bond structure makes each component a stronger interaction, showing high stability in polar, organic, and acidic solvent, as well as long‐term storing, which represents one of the highest overall performances for lighting in OIHPs.
The stability of perovskite solar cells has been identified as the bottleneck for their industrialization. With an aim at tackling this challenge, we self-synthesize a thus-far unreported linearly rotatable structure perovskite, i.e., TrMAPbX 3 (X = Br, I). The as-prepared hybrid perovskite is observed to demonstrate extremely high stability during device operation with high electric field strength and high temperature, which is associated with the good lattice-matching heterojunction structure between the linearly rotatable TrMAPbX 3 structure and 3D inorganic perovskite domain within a wide temperature range. The tight-fitting interface structure is devoted to inhibiting the accumulation of vacancy defects during device operation, which further avoids the δ-phase transition and charge transport resistance. Accordingly, we realize a CsPbI 3−x Br x inorganic perovskite-based solar cell with power conversion efficiency (PCE) of 20.59%, extending the remarkably high thermal stability to 192 h (85 °C and relative humidity of 25%) and 3055 h (25 °C and relative humidity of 25%).
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