Pure-halide reduced-dimensional perovskites, featuring large exciton binding energy and tunable bandgap, show great potential for high-efficiency deep-blue perovskite light-emitting diodes (PeLEDs). However, their efficiency, particularly in the low n-value phase domain ("n" represents the number of octahedral sheets), lags behind analogous perovskite emitters. Herein, it is demonstrated that the vibration of edge-dangling octahedra in the low n-value phase activates notorious exciton-phonon (EP) coupling, thereby deteriorating efficiency.
View Article and Find Full Text PDFWide-bandgap (WBG) perovskite solar cells (PSCs) are employed as top cells of tandem cells to break through the theoretical limits of single-junction photovoltaic devices. However, WBG PSCs exhibit severe open-circuit voltage (V) loss with increasing bromine content. Herein, inhomogeneous halogen-phase distribution is pointed out to be the reason, which hinders efficient extraction of carriers.
View Article and Find Full Text PDFα-FACsPbI is a promising absorbent material for efficient and stable perovskite solar cells (PSCs). However, the most efficient α-FACsPbI PSCs require the inclusion of the additive methylammonium chloride, which generates volatile organic residues (methylammonium) that limit device stability at elevated temperatures. Previously, the highest certified power-conversion efficiency of α-FACsPbI PSCs without methylammonium chloride was only approximately 24% (refs.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Metal halide perovskites are promising candidates for gamma-ray (γ-ray) spectrum detectors. However, achieving high-resolution energy spectra in single-photon pulse-height analysis mode remains challenging, due to the inevitable leakage currents degrade the recognizable fingerprint energies which is critical for resolving γ-ray spectroscopy. We demonstrate under high bias voltage, a deficient contact barrier can lead to excessive surface charge injection, thereby increasing leakage current from electrodes to perovskites.
View Article and Find Full Text PDFFull-Stokes polarization detection, with high integration and portability, offers an efficient path toward next-gen multi-information optoelectronic systems. Nevertheless, current techniques relying on optical filters create rigid and bulky configurations, limiting practicality. Here, a flexible, filter-less full-Stokes polarimeter featuring a uniaxial-oriented chiral perovskite film is first reported.
View Article and Find Full Text PDFHybrid organic-inorganic perovskites with diverse lattice structures and chemical composition provide an ideal material platform for novel functionalization, including chirality transfer. Chiral perovskites combine organic and inorganic sublattices, therefore encoding the structural asymmetry into the electronic structures and giving rise to the spin-splitting effect. From a structural chemistry perspective, the magnitude of the spin-splitting effect crucially depends on the noncovalent and electrostatic interaction within the chiral perovskite, which induces the local site and long-range bulk inversion symmetry breaking.
View Article and Find Full Text PDFWhile significant efforts in surface engineering have been devoted to the conversion process of lead iodide (PbI) into perovskite and top surface engineering of perovskite layer with remarkable progress, the exploration of residual PbI clusters and the hidden bottom surface on perovskite layer have been limited. In this work, a new strategy involving 1-butyl-3-methylimidazolium acetate (BMIMAc) ionic liquid (IL) additives is developed and it is found that both the cations and the anions in ILs can interact with the perovskite components, thereby regulating the crystallization process and diminishing the residue PbI clusters as well as filling vacancies. The introduction of BMIMAc ILs induces the formation of a uniform porous PbI film, facilitating better penetration of the second-step organic salt and fostering a more extensive interaction between PbI and the organic salt.
View Article and Find Full Text PDFFörster resonance energy transfer (FRET) has demonstrated its potential to enhance the light energy utilization ratio of perovskite solar cells by interacting with metal-organic frameworks (MOFs) and perovskite layers. However, comprehensive investigations into how MOF design and synthesis impact FRET in perovskite systems are scarce. In this work, nanoscale HIAM-type Zr-MOF (HIAM-4023, HIAM-4024, and HIAM-4025) is meticulously tailored to evaluate FRET's existence and its influence on the perovskite photoactive layer.
View Article and Find Full Text PDFWide-bandgap mixed-halogen perovskite materials are widely used as top cells in tandem solar cells. However, serious open-circuit voltage (V) loss restricts the power conversion efficiency (PCE) of wide-bandgap perovskite solar cells (PSCs). Herein, it is shown that the resulting methylammonium vacancies induce lattice distortion in methylammonium chloride-assisted perovskite film, resulting in an inhomogeneous halogen distribution and low V.
View Article and Find Full Text PDFTailoring bandgap by mixed-halide strategy in perovskites has attracted extraordinary attention due to the flexibility of halide ion combinations and has emerged as the most direct and effective approach to precisely tune the emission wavelength throughout the entire visible light spectrum. Mixed-halide perovskites, yet, still suffered from several problems, particularly phase segregation under external stimuli because of ions migration. Understanding the essential cause and finding sound strategies, thus, remains a challenge for stable and efficient mixed-halide perovskite light-emitting diodes (PeLEDs).
View Article and Find Full Text PDFMethylammonium 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.
View Article and Find Full Text PDFThe electrochemical CO reduction reaction (CORR) gives an ideal approach for producing valuable chemicals, offering dual benefits in terms of environmental preservation and carbon recycling. In this work, a strong synergistic effect is constructed by adopting electron-rich graphdiyne (GDY) as the supporting matrix, which significantly stabilizes the Au active sites and boosts the CORR process. The as-prepared GDY-supported Au nanoparticles (Au/GDY) exhibit excellent CORR performance, with an extremely high faradaic efficiency of 94.
View Article and Find Full Text PDFLead halide perovskite nanocrystals (LHP NCs) have rapidly emerged as one of the most promising materials for optical sources, photovoltaics, and sensor fields. The controlled synthesis of LHP NCs with high monodispersity and precise size tunability has been a subject of intensive research in recent years. However, due to their ionic nature, LHP NCs are usually formed instantaneously, and the corresponding nucleation and growth are difficult to monitor and regulated.
View Article and Find Full Text PDFDihalogenation of alkenes to the high-added value vicinal dihalides is a prominent process in modern synthetic chemistry. However, their effective conversion still requires the use of expensive and hazardous agents, sacrificial half-reaction coupling or primary energy input. Here, we show a photocatalytically assisted shuttle (p-shuttle) strategy for redox-neutral and reversible vicinal dihalogenation using low-cost and stable 1,2-dihaloethane under visible light illumination.
View Article and Find Full Text PDFMixed-halide perovskites enable precise spectral tuning across the entire spectral range through composition engineering. However, mixed halide perovskites are susceptible to ion migration under continuous illumination or electric field, which significantly impedes the actual application of perovskite light-emitting diodes (PeLEDs). Here, we demonstrate a novel approach to introduce strong and homogeneous halogen bonds within the quasi-two-dimensional perovskite lattices by means of an interlayer locking structure, which effectively suppresses ion migration by increasing the corresponding activation energy.
View Article and Find Full Text PDFOver the past few decades, organic-inorganic halide perovskites (OIHPs) as novel photocatalyst materials have attracted intensive attention for an impressive variety of photocatalytic applications due to their excellent photophysical (chemical) properties. Regarding practical application and future commercialization, the air-water stability and photocatalytic performance of OIHPs need to be further improved. Accordingly, studying modification strategies and interfacial interaction mechanisms is crucial.
View Article and Find Full Text PDFMixed-halide perovskites show tunable emission wavelength across the visible-light range, with optimum control of the light color. However, color stability remains limited due to the notorious halide segregation under illumination or an electric field. Here, a versatile path toward high-quality mixed-halide perovskites with high emission properties and resistance to halide segregation is presented.
View Article and Find Full Text PDFFormamidinium lead iodide (FAPbI ) perovskite possesses an ideal optical bandgap and is a potential material for fabricating the most efficient single-junction perovskite solar cells (PSCs). Nevertheless, large formamidinium (FA) cations result in residual lattice strain, which reduces the power conversion efficiency (PCE) and operational stability of PSCs. Herein, the modulation of lattice strain in FAPbI crystals via a π-conjugated organic amine, i.
View Article and Find Full Text PDFLead-free halide perovskite materials possess low toxicity, broadband luminescence and robust stability compared with conventional lead-based perovskites, thus holding great promise for eyes-friendly white light LEDs. However, the traditionally used preparation methods with a long period and limited product yield have curtailed the commercialization of these materials. Here we introduce a universal hydrochloric acid-assistant powder-to-powder strategy which can accomplish the goals of thermal-, pressure-free, eco-friendliness, short time, low cost and high product yield, simultaneously.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2023
As a special carbon material, graphdiyne (GDY) features the superiorities of incomplete charge transfer effect on the atomic level, tunable electronic structure and anchoring metal atoms directly with organometallic coordination bonds M (metal)-C (alkynyl carbon in GDY), providing it an ideal platform to construct single-atom catalysts (ACs). The coordination environment of single atoms anchored on GDY plays a key role in their catalytic performance. The mini-review highlights state-of-the-art progress in the rational design of GDY-based ACs and their applications, and mainly reveals the relationship between the coordination engineering of the GDY-based ACs and corresponding catalytic performance.
View Article and Find Full Text PDFPerovskite quantum dots are a competitive candidate for next-generation solar cells owing to their superior phase stability and multiple exciton generation effects. However, given the voltage loss in perovskite quantum dot solar cells (PQDSCs) is mainly caused by various surface and interfacial defects and the energy band mismatch in the devices, tremendous achievements have been made to mitigate the loss of PQDSCs. Herein, we elucidate the potential threats that hinder the high of PQDSCs.
View Article and Find Full Text PDFDespite the rapid progress in perovskite light-emitting diodes (PeLEDs), the electroluminescence performance of large-area perovskite devices lags far behind that of laboratory-size ones. Here, we report a 3.5 cm × 3.
View Article and Find Full Text PDFPerovskite light-emitting diodes (PeLEDs) with an external quantum efficiency exceeding 20% have been achieved in both green and red wavelengths; however, the performance of blue-emitting PeLEDs lags behind. Ultrasmall CsPbBr quantum dots are promising candidates with which to realize efficient and stable blue PeLEDs, although it has proven challenging to synthesize a monodispersed population of ultrasmall CsPbBr quantum dots, and difficult to retain their solution-phase properties when casting into solid films. Here we report the direct synthesis-on-substrate of films of suitably coupled, monodispersed, ultrasmall perovskite QDs.
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