Functional 2D Phases in Mixed Dimensional Perovskite Photovoltaics

Organic-inorganic hybrid perovskite solar cells (PSCs) with unique properties exhibit their powerful competitiveness in the photovoltaic field over the past few years. However, the challenges of stability for perovskite devices limit the commercialization and further development. The 2D/3D hybrid structures combine the superior efficiency of bulk perovskites and the superior stability of layered perovskites and gradually get hotspots of the photovoltaic field. In addition, there remains a lack of comprehensive understanding and systematic summary of the function of 2D perovskite attributed to the complex nature of 2D/3D structures. Here, the latest progress of 2D/3D hybrid structures and focus on the functionality of 2D phases in mixed structures and the underlying mechanism from the perspective of their different distributions in the perovskite layer is summarized. Then, the insight and vital factors for overall improvements in the stability of 2D/3D structures are thoroughly discussed. Finally, it is expected that this review will contribute to the present challenges and future research prospects in the photovoltaic industry.     

Gradient “Single-Crystal” Li-Rich Cathode Materials for High-Stable Lithium-Ion Batteries

As one of the high-energy cathode materials of lithium-ion batteries (LIBs), lithium-rich-layered oxide with “single-crystal” characteristic (SC-LLO) can effectively restrain side reactions and cracks due to the reduced inner boundaries and enhanced mechanical stabilities. However, there are still high challenges for SC-LLO with diverse performance requirements, especially on their cycle stability improvement. Herein, a novel concentration gradient “single-crystal” LLO (GSC-LLO), with gradually decreasing Mn and increasing Ni contents from center to surface, is designed and prepared by combining co-precipitation and molten-salt sintering methods, yielding a capacity retention of 97.6% and an energy density retention of 95.8% within 100 cycles at 0.1 C. The enhanced performance is mostly attributed to the gradient-induced stabilized structure, free of cracks and less spinel-like structure formation after long-term cycling. Furthermore, the gradient design is also beneficial to the safety of LLOs as suggested by the improved thermal stability and reduced gas release. This study provides an effective strategy to prepare high-energy, high-stability, and high-safety LLOs for advanced LIBs.     

19.28% Efficiency and Stable Polymer Solar Cells Enabled by Introducing an NIR-Absorbing Guest Acceptor

Here, a near-infrared (NIR)-absorbing small-molecule acceptor (SMA) Y-SeNF with strong intermolecular interaction and crystallinity is developed by combining selenophene-fused core with naphthalene-containing end-group, and then as a custom-tailor guest acceptor is incorporated into the binary PM6:L8-BO host system. Y-SeNF shows a 65 nm red-shifted absorption compared to L8-BO. Thanks to the strong crystallinity and intermolecular interaction of Y-SeNF, the morphology of PM6:L8-BO:Y-SeNF can be precisely regulated by introducing Y-SeNF, achieving improved charge-transporting and suppressed non-radiative energy loss. Consequently, ternary polymer solar cells (PSCs) offer an impressive device efficiency of 19.28% with both high photovoltage (0.873 V) and photocurrent (27.88 mA cm⁻²), which is one of the highest efficiencies in reported single-junction PSCs. Notably, ternary PSC has excellent stability under maximum-power-point tracking for even over 200 h, which is better than its parental binary devices. The study provides a novel strategy to construct NIR-absorbing SMA for efficient and stable PSCs toward practical applications.     

Efficient Inverted Perovskite Solar Cells with a Fill Factor Over 86% via Surface Modification of the Nickel Oxide Hole Contact

The poor interface quality between nickel oxide (NiO_x) and halide perovskites limits the performance and stability of NiO_x-based perovskite solar cells (PSCs). Here a reactive surface modification approach based on the in situ decomposition of urea on the NiO_x surface is reported. The pyrolysis of urea can reduce the high-valence state of nickel and replace the adsorbed hydroxyl group with isocyanate. Combining theoretical and experimental analyses, the treated NiO_x films present suppressed surface states and improved transport energy level alignment with the halide perovskite absorber. With this strategy, NiO_x-based PSCs achieve a champion power conversion efficiency (PCE) of 23.61% and a fill factor of over 86%. The device's efficiency remains above 90% after 2000 h of thermal aging at 85 °C. Furthermore, perovskite solar modules achieve PCE values of 18.97% and 17.18% for areas of 16 and 196 cm², respectively.     

Multiple Function Synchronous Optimization by PbS Quantum Dots for Highly Stable Planar Perovskite Solar Cells with Efficiency Exceeding 23%

Colloidal lead sulfide (PbS) quantum dots (QDs), which possess quantum confinement effect and processing compatibility with perovskite, are regarded as an excellent material for optimizing perovskite solar cells (PSCs). However, the existing PSCs optimized by PbS QDs are still facing the challenges of poor performance of the charge transport layers, low utilization in the near-infrared (NIR) region, and unsuitable energy level alignment, which limit the improvement of power conversion efficiency (PCE). Herein, a synchronous optimization strategy is realized via simultaneously introducing PbS QDs into SnO₂ electron transport layer and employing rare-earth-doped PbS QDs (Eu:PbS QDs) film with hydrophobic chain ligands as the NIR light-absorping layer and hole transport layer (HTL) of devices. PbS QDs effectively decrease the density of trap states by passivating defects. Eu:PbS QDs film with adjustable bandgap is employed as an absorption layer to broaden the NIR spectral absorption. The well-matched energy level between Eu:PbS QDs layer and perovskite layer implies efficient hole transfer at the interface. The successful synchronous optimization greatly elevates all photovoltaic parameters, reaching a maximum PCE of 23.27%. This PCE is the highest for PSCs utilizing PbS QDs material in recent years. The optimized PSCs retain long-term moisture and light stability.     

Multifunctional Organic Potassium Salt Additives as the Efficient Defect Passivator for High-Efficiency and Stable Perovskite Solar Cells

Despite the rapid developments are achieved for perovskite solar cells (PSCs), the existence of various defects in the devices still limits the further enhancement of the power conversion efficiency (PCE) and the long-term stability of devices. Herein, the efficient organic potassium salt (OPS) of para-halogenated phenyl trifluoroborates is presented as the precursor additives to improve the performance of PSCs. Studies have shown that the 4-chlorophenyltrifluoroborate potassium salt (4-ClPTFBK) exhibits the most effective interaction with the perovskite lattice. Strong coordination between  BF₃⁻/halogen in anion and uncoordinated Pb²⁺/halide vacancies, along with the hydrogen bond between F in  BF₃⁻ and H in FA⁺ are observed. Thus, due to the synergistic contribution of the potassium and anionic groups, the high-quality perovskite film with large grain size and low defect density is achieved. As a result, the optimal devices show an enhanced efficiency of 24.50%, much higher than that of the control device (22.63%). Furthermore, the unencapsulated devices present remarkable thermal and long-term stability, maintaining 86% of the initial PCE after thermal test at 80 °C for 1000 h and 95% after storage in the air for 2460 h.     

Inorganic Filler Enhanced Formation of Stable Inorganic-Rich Solid Electrolyte Interphase for High Performance Lithium Metal Batteries

Lithium metal (LM) is a promising anode material for next generation lithium ion based electrochemical energy storage devices. Critical issues of unstable solid electrolyte interphases (SEIs) and dendrite growth however still impede its practical applications. Herein, a composite gel polymer electrolyte (GPE), formed through in situ polymerization of pentaerythritol tetraacrylate with fumed silica fillers, is developed to achieve high performance lithium metal batteries (LMBs). As evidenced theoretically and experimentally, the presence of SiO₂ not only accelerates Li⁺ transport but also regulates Li⁺ solvation sheath structures, thus facilitating fast kinetics and formation of stable LiF-rich interphase and achieving uniform Li depositions to suppress Li dendrite growth. The composite GPE-based Li||Cu half-cells and Li||Li symmetrical cells display high Coulombic efficiency (CE) of 90.3% after 450 cycles and maintain stability over 960 h at 3 mA cm⁻² and 3 mAh cm⁻², respectively. In addition, Li||LiFePO₄ full-cells with a LM anode of limited Li supply of 4 mAh cm⁻² achieve capacity retention of 68.5% after 700 cycles at 0.5 C (1 C = 170 mA g⁻¹). Especially, when further applied in anode-free LMBs, the carbon cloth||LiFePO₄ full-cell exhibits excellent cycling stability with an average CE of 99.94% and capacity retention of 90.3% at the 160th cycle at 0.5 C.     

Air-Stable Li2S Cathode for Quasi-Solid-State Anode-Free Batteries with High Volumetric Energy

Anode-free batteries can maximize the energy density but their development is hindered by a lack of Li-rich cathodes for compensating the irreversible Li loss. Li₂S cathode is particularly appealing to this desire due to 2.6–4.7 folds more Li content and 4.2–6.8 times higher capacity than conventional intercalation cathodes. But its practical application is hindered by poor stability against moisture attacking in the air. Herein, a facile expendable polymer sheathing strategy toward air-stable Li₂S cathodes with high capacities for developing high-performance quasi-solid-state anode-free batteries without risk of cell leakage is reported. Tight protection by dense polymer barrier dramatically prolongs the lifetime of Li₂S cathode by 2,000 times at least in the air. Such air-stable Li₂S cathode allows for high compatibility of anode-free battery production with commercial schemes. More attractively, the polymer protective layer can in situ transform to multifunctional gel polymer electrolyte for releasing ionic pathways and enhancing cell performance by inhibiting LiPS loss and smoothing Li plating. With air-stable Li₂S cathode, the quasi-solid-state anode-free cells are assembled in ambient environment to deliver superb volumetric energy density of 1093 Wh L⁻¹. This study may shed new light to push the commercialization of high-energy and reliable anode-free batteries forward.     

Mitigating Surface Deficiencies of Perovskite Single Crystals Enables Efficient Solar Cells with Enhanced Moisture and Reverse-Bias Stability

Metal halide perovskite single crystals are promising for diverse optoelectronic applications due to their outstanding properties. In comparison to the bulk, the crystal surface suffers from high defect density and is moisture sensitive; however, surface modification strategies of perovskite single crystals are relatively deficient. Herein, solar cells based on methylammonium lead triiodide (MAPbI₃) thin single crystals are selected as a prototype to improve single-crystal perovskite devices by surface modification. The surface trap passivation and protection against moisture of MAPbI₃ thin single crystals are achieved by one bifunctional molecule 3-mercaptopropyl(dimethoxy)methylsilane (MDMS). The sulfur atom of MDMS can coordinate with bare Pb²⁺ of MAPbI₃ single crystals to reduce surface defect density and nonradiative recombination. As a result, the modified devices show a remarkable efficiency of 22.2%, which is the highest value for single-crystal MAPbI₃ solar cells. Moreover, MDMS modification mitigates surface ion migration, leading to enhanced reverse-bias stability. Finally, the cross-link of silane molecules forms a protective layer on the crystal surface, which results in enhanced moisture stability of both materials and devices. This work provides an effective way for surface modification of perovskite single crystals, which is important for improving the performance of single-crystal perovskite solar cells, photodetectors, X-ray detectors, etc.     

Intrinsically Flexible and Aging Resistant Fluorene-Based Rod-Coil Copolymer for Bendable Deep-Blue PLEDs

In the field of flexible light-emitting display, goal-oriented intelligent molecular design is used to control various behaviors of molecules, which provides potential for the development of flexible light-emitting conjugated polymers (LCPs). The introduction of non-conjugated units into polymer molecules is a key prerequisite for realizing the intrinsic flexibility, but its easy interchain slip will also lead to the formation of interchain excited states, which is detrimental to the efficiency of light-emitting diodes. Herein, two kinds of fluorene-based rod-coil copolymer with stable deep blue emission characteristics is presented and with Commission Internationale de L'Eclairage (CIE) coordinates of (0.18, 0.14) and (0.15, 0.09), respectively. Surprisingly, the copolymer films show efficient blue emission even at 100% tension. Meanwhile, the rod-coil copolymer possesses better aging resistance compared to rigid π-conjugated counterparts. Finally, both rigid and flexible light-emitting diodes based on rod-coil copolymer exhibit stable deep blue emission, and the G2-based PLED with CIE coordinates of (0.16, 0.08), which approach National Television System Committee standard blue specification. These results confirm the validity of rod-coil copolymer design strategy in constructing inherently flexible polymers with deep blue emission, which have great application potential in flexible PLEDs.