ABSTRACT Phase‐pure two‐dimensional (2D) interfacial passivation has emerged as an effective strategy for addressing the intrinsic instability and interfacial defects of three‐dimensional (3D) perovskite absorbers. However, conventionally formed 2D layers often suffer from mixed‐n phases, heterogeneous quantum‐well distributions, and disordered orientation, which impede charge transport, distort energy‐level alignment, and accelerate structural degradation. In this review, we elucidate the thermodynamic and kinetic origins of mixed‐phase formation and discuss how dimensional heterogeneity adversely impacts carrier dynamics and device stability. We then summarize recent advances in achieving phase‐pure 2D perovskite interlayers that enable precise n‐value control, favorable crystal orientation, and optimized interfacial energetics. These strategies yield highly ordered 2D/3D heterostructures that effectively suppress ion migration, mitigate non‐radiative recombination, and significantly enhance long‐term operational stability. Finally, we outline the remaining challenges and emerging opportunities for scalable, phase‐pure engineering toward high‐efficiency and stable perovskite photovoltaic technologies. Overall, this review provides a unified framework linking phase purity, interfacial ordering, and device stability, offering guidance for the development of next‐generation robust perovskite photovoltaics.
Inverted inorganic CsPbI3 perovskite solar cells (PSCs) hold great promise for stable and efficient tandem photovoltaics, yet their performance lags behind normal (n-i-p) counterparts due to limited film quality, inefficient carrier extraction, and severe defect-mediated recombination. Here, we demonstrate a triple-functional self-assembled molecule (SAM) engineering strategy to tackle these issues simultaneously. By directly incorporating the SAM into the CsPbI3 precursor solution, the SAM spontaneously enriches at the buried interface to form an efficient hole-selective contact. Meanwhile, its strong interaction with perovskite accelerates crystallization kinetics and enables comprehensive passivation of defects at both grain boundaries and interfaces. As a result, inverted CsPbI3 PSCs achieve an efficiency of 21.10% (certified 20.62%). By leveraging the "three-in-one" functionality of the SAM, this strategy endows PSCs with ideal operational stability (retaining 90% of initial efficiency after 680 h of continuous operating at similar to 50 degrees C) and enables 1 cm(2) devices to deliver a record-high efficiency of 19.69%.
Exploring nonprecious metal-based catalysts for cathodic hydrogen evolution reaction (HER) has facilitated the realization of hydrogen economy toward water electrolysis in alkaline media. However, the difficult water dissociation process for the Volmer step (H2O → H* + OH*) and the subsequent unsuitable OH* adsorption energy on nonprecious metal-based catalysts severely reduce the kinetics of HER. Herein, the universal synthesis for a series of transition metal (Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, and W)-based boride@sulfide heterostructured catalysts is realized by using the molten-salt method to conduct the in situ boronization of commercial sulfides. Significantly, WB2@WS2 heterostructured catalyst exhibits excellent catalytic activity and stability for HER. Balancing interfacial atom orbit hybridization between W(d)-B(s,p) and W(d)-S(s,p) at WB2@WS2 heterostructured interface enhances the built-in electric field. In situ Raman spectroscopy and density functional theory calculation results reveal that the strong built-in electric field in WB2@WS2 optimizes the adsorption and desorption of OH* intermediate, reducing the energy barrier of the rate-determining step (OH* desorption step), and thus favoring the enhancement of catalytic performance toward HER.
Introduction Lithium iron phosphate-graphite (LFP-C) batteries are widely used in various fields due to their high energy density, low cost, high safety, good rate performance, long cycle life, and environmental friendliness. However, prolonged calendar aging leads to increased internal resistance and capacity decay, thereby shortening their service life. In this work, the impacts of storage temperature and SOC on the calendar aging performance of LFP-C batteries were investigated. The results show that the capacity decay is more severe under high temperature and high SOC conditions. The structural evolution of the anode and cathode materials, as well as the cathodeu2013electrolyte interphase (CEI) and solid electrolyte interphase (SEI) layers were analyzed. It is indicated that the structure of LiFePO4 cathode remains stable, while the degree of disorder in the graphite anode increases. The decomposition of the liquid electrolyte leads to an increase of LiF content in the CEI and SEI layers with decreasing Li2CO3 content in the SEI layer at 50 u2103. Methods In an inert atmosphere glove box, several LFP-C CR2025 coin cells were assembled. The cells were charged to the targeted SOC, and then divided into six groups and stored under different conditions (i.e., at 0u2103-50%SOC, 0 u2103-100%SOC, 25 u2103 -50%SOC, 25 u2103-100%SOC, 50 u2103-50%SOC, and 50 u2103-100%SOC) for one month. After storage, each group of cells was cycled at 1C to assess the impact of different storage conditions on the electrochemical performance of the cells. Other cells were disassembled, and then cleaned to obtain the positive and negative electrodes. The capacity degradation mechanisms of batteries during calendar aging were characterized by X-ray diffraction (XRD), Raman spectroscopy, Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy coupled with energy dispersive X-Ray spectroscopy (SEM-EDX), and X-ray photoelectron spectroscopy (XPS). Results and discussion After 1-month storage, the LFP - graphite coin cells are charged and discharged at 1 C for 300 cycles. The results show that the cells stored at 50 u2103 cannot deliver any capacity. The cells stored at 0 u2103 exhibit a significantly higher discharge capacity, compared to the cells stored at 25 u2103. The cycling performance results of the cells after storage at different states of charge (SOC) indicate that the discharge capacity of coin cells stored at 50% SOC is higher than that of cells stored at 100% SOC. It is revealed that there is a slight difference in the XRD patterns of LFP electrodes stored under various temperatures and SOC conditions, indicating that the structure of LFP maintains a high stability under various storage conditions. The XRD patterns of the graphite anodes also remain unchanged, and only the peaks attributed to the graphite and current collector Cu foil appear. The results by Raman spectroscopy indicate that the LFP material remains stable after storage, while the degree of disorder in the graphite anode increases significantly and becomes more pronounced with the increase of storage temperatures and SOC. The results by FTIR reveal the side reaction products on the surfaces of both the cathode and anode materials (i.e., Li2CO3, (CH2OCOOLi)2, and ROCO2Li). The results by SEM-EDX indicate that there is a slight change in the elemental ratio on the surface of the cathode electrodes after storage under different conditions, further validating the stability of the LFP material. The surface of graphite particles becomes rough after storage, and the content of fluorine and phosphorus elements on the surface of graphite anodes increases under high-temperature and high-SOC conditions. The results by XPS show that the content of LiF in the CEI layers increases with increasing the temperature and SOC. The storage temperature shows a more pronounced effect on the composition of the CEI rather than the SOC. The relative content of LiF and Pu2014F in the SEI layers significantly increases, while the relative content of Li2CO3 decreases due to decomposition as the storage temperature increases. Conclusions LiFePO4-graphite coin cells with different SOC (i.e., 50% and 100%) were stored at various temperatures (i.e., 0, 25 u2103 and 50 u2103) and for one month and then charged and discharged for 300 cycles. The results showed that cells stored at 50u2103 were completely inoperative. The battery capacity retention followed an order of 0 u2103-50%SOC u0026gt; 0 u2103-100%SOC u0026gt; 25 u2103 -50%SOC u0026gt; 2 u2103-100%SOC. It was revealed that the LFP cathode exhibited a structural stability as the storage temperature and SOC increased. Conversely, the degree of disorder of graphite anode increased, having a detrimental effect on the lithium ion migration. It was evident that the temperature could have a dominant influence on the composition of the CEI rather than SOC. The relative content of Li2CO3 decreased, while the relative content of LiF decreased within the CEI layers as the storage temperatures and SOC increased. In addition, the relative content of LiF and Pu2014F increased in the SEI layers with temperature, and the temperature had a more significant effect rather than SOC on the SEI layer.
Treating skin injuries remains challenging due to issues like wound infections. In this study, polyvinylidene fluoride (PVDF)/polyethylene oxide (PEO)/azithromycin (AZ) composite nanofibers were prepared using electrospinning to reduce bacterial infections in skin wounds. The surface morphology, chemical structure, and hydrophilicity of the nanofibers were characterized using scanning electron microscopy, Fourier transform infrared spectroscopy, and contact angle measurements, respectively. Antibacterial performance tests revealed that increasing the AZ dosage expanded the antibacterial zone, indicating improved effectiveness. Furthermore, experiments on rat skin infections showed that the PVDF/PEO/AZ membrane inhibited suppuration at S. aureus-infected wound sites. These findings demonstrate the potential of AZ-loaded PVDF/PEO nanofiber membranes as effective antibacterial dressing.
Lithium iron phosphate-graphite (LFP-C) batteries are widely used in energy storage and electric vehicles due to their high safety and good cycling stability. However, there is still a lack of in-depth research to investigate the impact of depth of discharge (DOD) on LFP-C pouch cells. In this work, we systematically investigate the influence of DOD (2.5 V and 1.5 V) on the cycling performance of LFP-C pouch cells, and the evolution of the cathode-electrolyte interphase (CEI) and solid electrolyte interphase (SEI) layers. In comparison to a DOD of 2.5 V, the cell with a DOD of 1.5 V exhibits a rapid capacity degradation after 50 cycles. Combined with comprehensive characterizations, the mechanism of battery decay has been revealed. A deeper discharge to 1.5 V results in an increase in the disorder of graphite. Additionally, the organic components in the SEI layer decreases, while the Li2CO3, LiF, and Li3PO4 inorganic products enrich due to the continued decomposition of electrolyte. Meanwhile, the pouch cells generate a considerable quantity of H2 and minor CH4 gases. This study will pave the way to understand the effects of overdischarge on the electrochemical performance of commercial pouch cells and the evolution mechanism of CEI/SEI layers.
With the increasing awareness of environmental protection, polysaccharide packaging materials have received widespread attention. In this work, a kind of novel polysaccharide composite membrane was prepared by hollow glass microspheres (HGM) into agar (AG) and sodium alginate (SA) matrix and then cross-linking by glycerol (abbreviated as AG-SA-HGM). The addition of hollow glass microspheres significantly improved the thermal stability and flame retardancy of the polysaccharide membrane, with a peak heat release rate of only 72.05 kW m- 2. Besides, the prepared flame retardant packaging membrane not only has excellent flexibility, no cracks after folding, and can restore its original state, but also exhibits special properties of front hydrophobicity (contact angle of 123.82 degrees) and back hydrophilicity (contact angle of 35.33 degrees). Therefore, AG-SA-HGM composite membrane has great potential in flame retardant applications.
With the rising concerns of electromagnetic pollution, the development of lightweight and broadband microwave absorbing materials has become crucial. In this study, the reduced graphene oxide (rGO) aerogels were synthesized using graphene oxides as the precursor. The aerogel exhibited an ultralow density of 0.016 g/cm3, featuring a porous and wrinkled 3D structure that effectively prolonged the propagation path of electromagnetic waves and enhanced energy dissipation. Electromagnetic absorption tests showed that the aerogel achieved a minimum reflection loss (RL) of -30.51 dB with the absorption band ranging from 7.17 to 9.19 GHz at a thickness of 3.5 mm. When the thickness decreased to 2.5 mm, the effective absorption bandwidth (EAB) reached 7.21 GHz. These results demonstrated that the as-prepared rGO aerogels offered twofold advantages of ultralightweight and broadband absorption, making them promising candidates for microwave absorption applications.
Black phosphorus (P(black)) shows impressive physicochemical features for electrocatalysis including adjustable bandgap and high charge carrier mobility. However, the existence of solitary electron pairs in exfoliated P(black) nanosheets (EP(black)) leads to rapid surface degradation, resulting in unfavorable durability. Herein, a P–O bridge was created in the heterostructure EP(black)/vanadium-doped cobalt hydroxide with oxygen vacancy (EP(black)/V–CoO2-xH2) to stabilize and expedite oxygen evolution reaction (OER) activity. By bonding the solitary electron pairs of EP(black) and oxygen species (OH*) of V–CoO2-xH2, the distinctive P–O bridge resulted in important ligand effects that improved not merely the stability of EP(black) but effectively regulated the electron configuration of V–CoO2-xH2. DFT simulations revealed that directional interfacial electron migration from V–CoO2-xH2 to EP(black) facilitated the formation of pivotal OER intermediates and hence boosted OER activities. This study proposes a novel strategy to enhance the electrochemical properties of EP(black), which could be extended to a wide range of high-performance electrocatalyst systems.
Developing catalysts with excellent CO2 capture capability and electrochemical CO2 reduction reaction (CO2RR) at a wide potential range simultaneously is significant but remains a formidable challenge. Here, two novel InMg defective trinuclear cluster-based MOFs (SNNU-41 and SNNU-42) with abundant p-block unsaturated coordinated sites were reported and exhibited good CO2 capture and CO2RR performance simultaneously. Due to the suitable micropores, SNNU-41 showed higher CO2 capture ability at different adsorption pressure conditions. On account of the rigid framework and the closer p band center to Fermi level, SNNU-42 accelerated the conversion of CO2 molecule to C1 efficiency. Notably, via adjusting the ratio of p-block metal (In) in the SNNU-42 framework, the performance of the CO2RR was promoted drastically. SNNU-42 with the InMg (1:1.8) mixed cluster delivered an excellent Faradaic efficiency of 91.3% for C1 products and high selectivity of 72.0% for HCOOH at -2.5 V (vs Ag/Ag+) with a total current density of 77.2 mA cm-2. This work provides a possibility for efficient CO2 capture and CO2RR electrocatalysts through the modulation of electronic structures and composition in MOFs.
Dopant-free poly(3-hexylthiophene) (P3HT) hole transport materials (HTMs) have been acknowledged for their significant potential in enhancing the stability of perovskite solar cells (PSCs). However, the severe recombination loss occurring at perovskite/P3HT interfaces exhibits a tremendous impediment to their photovoltaic efficiency. Herein, we develop a general molecular engineering strategy using tailorable phosphine ligands to modulate the perovskite/P3HT interface for effectively alleviating the recombination loss and maximizing the device voltage. Theoretical and experimental results reveal that the phosphine ligand with balanced electronic and steric properties could establish a strong binding interaction with perovskite, which not only passivates deep-level antisite defects for suppressing energy loss but also optimizes the energy level alignment to facilitate carrier transfer. This approach is applicable to the perovskites with various bandgaps, such as 1.53 eV (CsFAPbI3), 1.7 eV (CsPbI3), and 1.9 eV (CsPbI2Br), delivering top-tier efficiencies of 25.08% (certified 24.54%), 21.42%, and 18.39%, respectively. Benefiting from the improved interface and dopant-free HTMs, these PSCs exhibit outstanding stability under accelerated aging conditions. An effective molecular engineering strategy using tailorable phosphine ligands was developed to modulate the perovskite/P3HT interface to alleviate the recombination loss and maximize the device voltage for perovskites with various bandgaps.
The thermally stable inorganic cesium-based perovskites promise efficient and stable photovoltaics. Unfortunately, the strong ionic bonds lead to uncontrollable rapid crystallization, making it difficult in fabricating large-area black-phase film for photovoltaics. Herein, we developed a facile hydrogen-bonding assisted strategy for modulating the crystallization of CsPbI2 Br to achieve uniform large-area phase-pure films with much-reduced defects. The simple addition of methylamine acetate in precursors not only promotes the formation of intermediate phase via hydrogen bonding to circumvent the direct crystallization of CsPbI2 Br from ionic precursors but also widens the film processing window, thus enabling to fabricate large-area high-quality phase-pure CsPbI2 Br film under benign conditions. Combining with stable dopant-free poly(3-hexylthiophene), the CsPbI2 Br solar cells achieve the record-high efficiencies of 18.14 % and 16.46 % for 0.1 cm2 and 1 cm2 active area, respectively. The obtained high efficiency of 38.24 % under 1000 lux illumination suggests its potential in indoor photovoltaics for powering the Internet of Things, etc.
As the world's first solid-state solar cells, selenium (Se) cells initiated contemporary photovoltaic research. However, the highest efficiency of Se photovoltaics has stagnated at 6.5% since 2017. Here, we report Se solar cells with a certified record efficiency of 7.2% through a critical melting -annealing strategy. This strategy provides enough energy to overcome the high activation energy of disordered Se chains and incorporate them into the lattice, arising from the unique one-dimensional crystal structure of photoactive trigonal Se. The resulting Se films exhibit a 2.3 -fold reduction in trap density compared with conventional Se films. Such high-performance Se cells also achieve an efficiency of 18.0% under 1,000lux indoor illumination, owing to their suitable wide band gap ( , - , 1.9 eV) for indoor photovoltaics (IPVs). This efficiency surpasses those of market -dominant amorphous silicon and all currently available lead-free perovskite IPVs. We further construct Se IPV modules capable of generating a power of 559.8 mW, achieving self -powered wireless electronic shelf labels.
Perovskite solar cells (PSCs) are recognized as one of the most promising next-generation photovoltaics, primarily due to their exceptional power conversion efficiency, ease of processing, and cost-effectiveness. Despite these advantages, challenges remain in achieving high-quality films and ensuring the long-term stability of PSCs, which hinder their widespread commercialization. Polymers, characterized by multifunctional groups, superior thermal stability, flexible long chains, and cross-linking capabilities, offer significant potential to enhance the performance and reliability of PSCs. This review comprehensively presents the multifaceted roles that polymers play in PSCs. Through carefully controlling interactions between polymers and perovskites, crucial aspects such as film crystallization kinetics, carrier transport process, ion migration issues, and mechanical properties under bending can be effectively regulated to maximize the device performance. Furthermore, the hydrophobic properties and strong chelated cross-linking networks of polymers significantly enhance the stability of PSCs under various environmental conditions while effectively mitigating lead leakage, thereby addressing environmental concerns and long-term durability. Moreover, this Perspective identifies potential pathways for further advancing polymer-based strategies in PSC applications.
All solid–state battery (ASSB) is widely recognized as one of the most promising high‐energy‐density systems/technologies. However, thermal safety issues induced by highly reactive materials still exist for solid electrolytes (SEs). Insights on thermal behaviors at elevated temperatures and the underlying mechanism for thermal stability of SE‐based systems are still missing. Herein, thermal stability performance of typical sulfide SEs is systematically investigated with metal Li, whose order of interfacial thermal stability is concluded to be Li 6 PS 5 Cl > Li 3 PS 4 > Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 > Li 4 SnS 4 > Li 7 P 3 S 11 after a comprehensive evaluation. Interestingly, Li 4 SnS 4 , which achieves good air stability, has poor thermal stability with Li metal. This is possibly caused by Li─Sn alloy products generated during thermal decomposition, and their great thermodynamic driving force towards SE for accelerated thermal runaway. Moreover, electrolytes with poor material‐level thermal stability (e.g., Li 7 P 3 S 11 ) may form a dense passivation layer by self‐decomposition with Li metal to retard thermal runaway. Conclusively, the material structure affects the thermodynamic stability of the system, but the reaction products (interphase) affects the kinetic process of the thermal reaction within a certain temperature range. Therefore, thermal stability with both metallic lithium and decomposition products is a necessary condition for interfacial thermal stability of sulfide SEs.
Perovskite solar cells (PSCs) are promising next-generation photovoltaics due to their unique optoelectronic properties and rapid rise in power conversion efficiency. However, the instability of perovskite materials and devices is a serious obstacle hindering technology commercialization. The quality of perovskite films, which is an important prerequisite for long-term stable PSCs, is determined by the quality of the precursor solution and the post-deposition treatment performed after perovskite formation. Herein, we review the origin of instability of solution-processed PSCs from the perspectives of the precursor solutions and the perovskite films. In addition, we summarize the recent strategies for improving the stability of the perovskite films. Finally, we pinpoint possible approaches to further advance their long-term stability.
Inorganic cesium lead triiodide perovskite has shown great potential in photovoltaic applications. Currently, the preparation of high-quality b- or g-phase CsPbI3 films largely relies on the DMAPbI3 (dimethylammonium [DMA]) or "HPbI3"-assisted crystallization method, which unfortunately causes DMAPbI3 residue and deteriorates photovoltaic performance and stability. Herein, a universal hydrogen-bonding-facilitated DMA extraction method is developed to fabricate high-quality g-CsPbI3 films. Theoretical and experimental evidence manifests that the hydrogen bonds formed between polyacrylic acid (PAA) and DMAPbI3 decrease the DMA escape energy barrier, and this not only brings ahead the decomposition process of DMAPbI3 but also accelerates the crystallization kinetics of CsPbI3, resulting in pinhole-free CsPbI3 films without any trace of DMAPbI3 residue and an extended fabrication humidity (up to 80% relative humidity [RH]) and temperature window. Thanks to the environmentally benign crystallization, the CsPbI3 solar cells with dopant-free poly(3-hexylthiophene) (P3HT) yield a high efficiency of 20.25% and superior moisture and operational stability.
All-solid-state batteries (ASSBs) have been widely acknowledged as the key next-generation energy storage technology/device, due to their high safety and energy density. Among all solid electrolytes (SEs) that have been studied for ASSBs, sulfide SEs represent the most promising technical route due to their ultra-high ionic conductivity and desirable mechanical property. However, few results have been reported to study the thermal stability/safety issue of sulfide SEs and ASSBs. Herein, we develop the first-of-its-kind theoretical paradigm and a new conceptual parameter 7th to quantitatively calculate/predict the essential thermal stability of sulfide SEs. This theoretical paradigm takes all types of parameters (e.g. crystal structure, localized polyhedra configuration, bond energy, bond type, bond number, normalization factor, and the energy correction factor) into consideration, and more importantly, can be simplified into one straightforward equation for its convenient application in any crystalline systems. To prove its functionality, the typical experimental strategies (stoichiometric ratio control and elemental doping) are adopted for typical sulfide SEs (Li7P3S11, Li3PS4) to improve their thermal stabilities, based on the predictions obtained from the derived theory and equation. Moreover, the potential doping elements to improve thermal stability of sulfide SEs are screened throughout the whole periodic table, and the theoretically predicted trends correspond well with experimental evidence. This work may represent the most critical breakthroughs in the research field of thermal stability for sulfide SEs, not only because it fills the gap of this field, but also due to its precise and quantitative prediction based on a complete consideration of all parameters that determine their thermal stabilities. The handy model developed herein can also be applied to any crystalline materials.
We propose a phase transition growth strategy for the deposition of CsPbI2Br films that allows relaxation of the tensile strain by 62 ± 4% and reduction of defect densities at the film surface and in bulk. PSCs achieve an efficiency of 16.5%.
Inorganic cesium lead halide (i.e., CsPbI3−xBrx) perovskite solar cells have made great breakthroughs in the last years with power conversion efficiency beyond 20%, thermal and photo stability reaching hundreds of hours. Hole transporting materials, as important building blocks in perovskite solar cells, present significant influences on both performance and stability. Understanding the energy loss mechanisms and failure pathways of inorganic perovskite solar cells that are originated from the hole transporting layer and the adjacent interfaces paves the way to enhance the efficiency towards Shockley-Queisser limit and to approach the long-term stability requirement. In this review, we first briefly overview the fundamentals of inorganic perovskites and solar cells, particularly on the criteria for designing and engineering efficient hole transporting materials. Second, we give a comprehensive review of recent advances on inorganic, small molecular and polymeric hole transporting materials. Finally, we discuss the challenges of state-of-the-art inorganic perovskite solar cells in view of the hole transporting materials and conclude this review by providing perspective on development of advanced hole transporting materials towards next-generation efficient and stable inorganic PSCs.