All-inorganic halide perovskites have attracted significant attention for photodetection applications owing to their excellent optical and electrical properties, together with superior stability against chemical and radiation-induced degradation. Here, we report a facile solution-processing strategy for synthesizing large-area (up to 8.5 × 8 cm2) single-crystal-like CsPbBr3 films. Compared with bulk single crystals, these films offer advantages including large-area scalability, controllable thickness, and improved device integration while maintaining comparable optoelectronic properties. The as-prepared films exhibit a low trap density of 9.4 × 1010 cm−3, enabling a high carrier mobility of 66 cm2 V−1 s−1 and an outstanding mobility–lifetime product of up to 1.02 × 10−3 cm2 V−1. Photodiodes based on these films demonstrate excellent performance, including a high responsivity of 432 mA W−1, a detectivity of 2.4 × 1011 Jones, and a fast response time of 44 ms. Importantly, the large-area devices exhibit excellent uniformity in responsivity and detectivity across different regions. Moreover, the devices retain over 90% of their initial responsivity after one month of storage under N2 conditions and remain operational after 5 days in air. Stable photocurrent responses under varying laser intensities for up to 20 min further confirm their excellent operational stability.
In this study, we synthesized a layered double hydroxide (LDH) with bimetallic centers of copper and iron (CuFe-LDH) and employed it as a multifunctional flame retardant and smoke suppressant to enhance the flame retardancy and smoke suppression properties of polyvinyl chloride (PVC). The results indicate that during the combustion of the CuFe-LDH/PVC composite, a dense carbon layer with tortuous pathways forms in the condensed phase through Lewis acid-catalyzed and reduction-coupling mechanisms. Coupled with the dilution effects of H2O and CO2 during combustion, the CuFe-LDH/PVC composite exhibits remarkable flame retardant and smoke suppressant properties, achieving a limiting oxygen index value of 34.8% and achieving a UL-94 V-0 rating. Compared to pristine PVC, the peak heat release rate of the CuFe-LDH/PVC composite was reduced by 20.55%, and the maximum average rate of heat emission decreased by 27.9%. Furthermore, the maximum smoke density and maximum average rate of smoke emission were reduced by 36.5% and 67.8%, respectively. This research proposes a novel method for designing and synthesizing additives that enhance the flame retardancy and smoke suppression performance of PVC from a catalytic perspective while avoiding the formation of multi-phase interfaces, thereby alleviating the adverse effects of traditional co-addition methods on polymers.
Halide perovskites have demonstrated great potential for next-generation X-ray detectors owing to their strong X-ray absorption, excellent charge-transport properties, tunable band structures, and low-cost processability. These advantages enable high-sensitivity, low-dose, and fast-response X-ray detection for medical imaging, security screening, and industrial inspection. Recently, heterostructure engineering has become an effective strategy for improving detector performance and stability by regulating band alignment, interfacial coupling, and carrier transport. In this review, we highlight recent advances in heterostructure-engineered halide perovskite X-ray detectors, including perovskite/perovskite and perovskite/functional-material heterostructures. Particular emphasis is placed on how heterointerfaces improve charge separation and transport, suppress recombination losses, inhibit ion migration, and enhance device stability and imaging performance. Finally, we discuss the remaining challenges and future opportunities for developing high-performance, stable, and scalable perovskite X-ray detection technologies.
Bioethanol upgrading to higher alcohols (C4-10-OH) involves several sequential reaction steps occurring at multiple different active sites. Therefore, precisely engineering heterogeneous catalysts with appropriate local chemical structures of active sites and spatial environments is highly desired for efficient ethanol tandem conversion. Herein, we constructed a novel Cu-based catalyst featuring atomically dispersed Cu sites confined in a hierarchical silicalite-1@La2O3@silicalite-1 architecture, where single Cu atoms were confined in the micropores of surface silicalite-1 (S-1) zeolite nanoislands dispersed on the outer La2O3 layer encapsulating a hollow S-1 zeolite core. By modulating the content of Cu and La species, such a constructed multihierarchical Cu@S-1@La2O3@S-1 catalyst exhibited excellent performance in ethanol conversion to higher alcohols, along with an impressively high ethanol conversion of 74.9% and C4-10-OH selectivity of 85.0%, as well as an unprecedentedly high production rate of higher alcohols (10.575 mol·gCu-1·h-1) at 275 °C, far exceeding those over state-of-the-art Cu-based catalysts. It was elucidated that surface single-atom Cu sites first notably promoted the adsorption and activation of ethanol and thus initiated its dehydrogenation to produce acetaldehyde, and subsequently, acetaldehyde intermediates migrated to the outer La2O3 layer featuring abundant medium-strength basic and acidic sites, thereby facilitating the condensation of acetaldehydes and their further dehydration. This work provides an innovative approach for rationally designing high-performance supported Cu catalysts with a spatiotemporal decoupling structure applied in advanced heterogeneous tandem catalytic processes through the design of site-specific confinement within hierarchical structures.
The glycerol hydrogenolysis reaction is a critical connection between the biodiesel industry and the production of high‐value‐added chemicals, underscoring its significant development potential and substantial social value. In this study, we synthesized a series of Cu‐ZrO 2 ‐Al 2 O 3 catalysts and investigated the influence of Al 2 O 3 on the dispersion and chemical states of Cu species, the surface acid–base properties of the ZrO 2 ‐Al 2 O 3 support, and the overall catalytic performance for the selective hydrogenolysis of glycerol to 1,2‐propanediol (1,2‐PDO). The results indicate that the addition of appropriate amounts of Al 2 O 3 enhances the dispersion of copper active sites within the catalyst, reduces both the quantity and strength of basic sites, and increases the proportion of medium‐strength acid sites on the surface. The improved dispersion of Cu active species, an optimal balance between acidity and alkalinity, along with a synergistic interaction between Cu active species and surface acid–base sites collectively facilitates the smooth progression of the dehydration–hydrogenation pathway involving acidic sites. Consequently, the optimal Cu/ZrO 2 ‐10%Al 2 O 3 catalyst exhibits excellent catalytic capability and cyclic stability under mild conditions, achieving a glycerol conversion rate of 94.1% and a selectivity toward 1,2‐PDO of 96.0%. Furthermore, these copper‐based catalysts may have potential applications in the efficient exploitation and utilization of biomass resource.
Phase change materials (PCMs) absorb and release energy from the environment effectively during the phase change process, leading to their widespread use in the field of thermal energy storage. However, the development of PCMs has been limited by issues such as poor thermal conductivity and light absorption. We therefore designed a silver-plated melamine foam (MF) framework and synthesized a phenolamine aggregate coating on the MF through a redox reaction, enhancing the bonding with silver nanoparticles and resulting in fully silver-plated MF. Meanwhile, hydroxylated carbon nanotubes (HCNTs) were added to the framework as a filler. This modification improved the conductivity of the corresponding polyethylene glycol (PEG)-based composite PCMs from 0.33 (pure PEG) to 0.82 W m⁻¹ K⁻¹ due to the construction of a multilevel thermal conduction channel. Additionally, a high photothermal conversion efficiency of 92.4% was achieved through the combined effect of the local resonance absorption of the silver and the molecular thermal vibration of the HCNTs. These advances provide a new strategy for optimizing the performance of PCMs, with potential applications in energy storage and thermal management.
Currently, the application of copper-based catalysts in methanol steam reforming (MSR) to produce hydrogen is fundamentally hindered by the sintering of copper nanoparticles and the ambiguous nature of the active sites that govern the coupling reaction between methanol and water. Here, we present a rationally designed supported Cu catalyst on the amorphous Al2O3 decorated samarium oxide nanorod. It was shown that the partial embedding of Cu nanoparticles by the Sm2O3 triggered robust metal-support interactions, leading to the formation of abundant well-defined Cu+-OV-Sm2+ interfacial ensembles (OV: oxygen vacancy). The optimized Cu/ Al2O3/Sm2O3-NR catalyst achieved complete methanol conversion and exhibited a high H2 production rate of 472.6 mmol gcat-1 h-1 at 300 degrees C. Importantly, the Cu/Al2O3/Sm2O3-NR catalyst exhibited outstanding long-term stability for about 200 h under the reaction condition. Through comprehensive characterizations coupled with density functional theory calculations, it was unveiled that Cu+ sites at Cu+-OV-Sm2+ interfacial ensembles preferentially facilitated the activation and dehydrogenation of CH3OH to form Cu-HCO structures and meanwhile the adjacent OV-Sm2+ sites efficiently promoted the dissociation of H2O to generate Sm-OH species, significantly accelerating the MSR reaction via a formate pathway. Moreover, the pronounced electronic coupling between defective Cu+-OV-Sm2+ interfacial ensembles and reaction intermediates weaken C-H bonds within the intermediates, thereby accelerating dehydrogenation processes. This study not only devises an effective approach for creating robust interfacial dual active sites for MSR reaction but only offers broad guidance for the design of high-performance Cu-based catalysts in heterogeneous catalysis.
Regulating the reaction pathway to overcome the activity-stability trade-off of catalysts is significant but remains highly challenging in acidic oxygen evolution reactions (OERs). Herein, we incorporated atomically dispersed Ru into an oxygen vacancy-rich (Ovc) MnO2-x host through a combination of hydrothermal reaction, argon-plasma bombardment, and isomorphic substitution, resulting in a distinctive catalyst (Ru-AP-MnO2-x) featuring Ovc-mediated heteroasymmetric dual-active-site Mn-Ovc-Ru units. Impressively, the Ru-AP-MnO2-x catalyst achieved a low overpotential of 233 mV at 100 mA cm-2 and demonstrated an exceptional stability for >5000 h at 10 mA cm-2 in 0.5 M H2SO4. When used in a proton exchange membrane water electrolyzer (PEMWE), it required a potential of only 1.76 V to reach 3 A cm-2 (surpassing the DOE 2026 target: 1.8 V at 3 A cm-2) and operated stably at 1 A cm-2 for up to 2200 h with an extremely low potential decay rate of only 22.3 μV h-1, positioning it among the top-ranked Ru/Ir-based catalysts. Operando characterizations and theoretical calculations demonstrated that enhanced Ru-O covalency and reduced Ru-Mn distance in the unique Mn-Ovc-Ru unit enabled a heteroasymmetrical-dual-active-site-assisted lattice oxygen mechanism (HADAS-LOM) for OER, where the *O intermediates transferred from Ru to Mn sites coupled lattice O (Olat) for rapid O2 release. Moreover, the bridged Ovc increased the electron density at Ru sites to mitigate overoxidation, while synergistic Ru-Mn dual sites allowed Olat around Mn instead of Ru sites to form an *OO intermediate, effectively protecting Ru from dissolution. This work offers a blueprint for engineering Ovc and multiple active-site synergy in the design of acid-stable, high-efficiency OER electrocatalysts.
Photocatalytic CO2 reduction to produce high value-added hydrocarbons has attracted significant attention, yet its overall efficiency remains unsatisfactory. In this work, a micro-liquid film reactor featuring enhanced mixing efficiency was utilized to realize the doping of single Fe atoms into the lattice of TiO2, enabling the generation of abundant atomically dispersed Fe delta+-Ov-Ti structures (Ov: oxygen vacancy). The results showed that compared to pristine TiO2, the optimized Fe-TiO2 photocatalyst bearing a 4 wt% Fe content exhibited 15.2 times higher activity, with a significant shift in the predominant product from CO to CH4, as well as an impressively high CH4 formation rate of 29.2 & micro;mol g-1 h-1, surpassing those over most of the state-of-the-art TiO2-based photocatalysts previously reported. It was revealed that the incorporation of single-atom Fe could reduce the bandgap of the TiO2 matrix, and atomically dispersed Fe delta+-Ov structures could improve the separation efficiency of photogenerated charge carriers and facilitated the adsorption and activation of CO2 and the formation and stabilization of the key *CO reaction intermediate, thereby accelerating photocatalytic CO2 reduction to produce CH4. The present work affords a simple and efficient strategy for designing single-atom Fe-regulated TiO2-based photocatalysts for a synergistic enhancement of CO2 photoreduction activity and CH4 selectivity.
Micro–mesoporous Beta zeolites could be rapidly synthesized using a micro-liquid film reactor via a non-classical crystallization process.
ABSTRACT In methanol‐to‐olefins (MTO) reactions, extending the catalyst lifetime remains a critical challenge for industrial applications. Herein, we develop a synergistic synthetic strategy integrating a micro‐liquid film (MLF) reactor, crystal seed assistance, and ligand protection to efficiently incorporate cerium species into SSZ‐13 zeolite, thereby yielding highly dispersed CeO x nanocluster‐modified SSZ‐13 zeolites (Ce‐SSZ‐13). The CeO x loading effectively modulated the acid properties by weakening Brønsted acid strength while generating additional weak Lewis acid sites. The Ce‐SSZ‐13 zeolite featuring a 1 wt% Ce loading showed excellent catalytic performance at a weight hourly space velocity of 1 h −1 and 400°C, with a long catalyst lifetime of 10.4 h and a 91.3% selectivity of light olefins. Notably, the catalyst lifetime was enhanced by 41.1% compared with the unmodified SSZ‐13 zeolite, accompanied by a significantly reduced coke formation rate of 0.081 mg·min −1 . It was revealed that the appropriate acidity of Ce‐SSZ‐13 zeolites efficiently suppressed hydrogen transfer and aromatization processes in MTO reactions and stabilized key hydrocarbon pool intermediates, thereby shifting the reaction pathway toward the olefin cycle. These findings provide an effective strategy for rationally designing high‐performance SSZ‐13 catalysts for MTO reactions and highlight the critical role of acid modulation of SSZ‐13 zeolites.
Regenerable cathodes that integrate efficient charge transfer with abundant binding sites are essential for electrochemical U(VI) capture in hybrid capacitive deionization (HCDI) systems. Herein, Ti3C2Tx MXene (MXene), a two-dimensional transition metal carbide, a high-entropy Prussian blue analogue (HEPBA), and their composite, MXene-HEPBA, were evaluated as cathode materials for electro-assisted U(VI) removal. MXene mainly exhibited electric double-layer capacitive behavior, whereas HEPBA and MXene-HEPBA showed pronounced Faradaic redox characteristics. By coupling the conductive MXene scaffold with the multimetal coordination-active HEPBA framework, MXene-HEPBA delivered specific capacitances of 87 F/g at 1.25 A/g and 67 F/g at 6.25 A/g. In synthetic U(VI)-containing solutions, MXene-HEPBA achieved a U(VI) uptake capacity of 56 mg/g under optimized HCDI conditions and exhibited efficient regeneration, with a desorption efficiency of 92% using 0.5 mol/L HNO3 under a reverse voltage of 0.8 V. In actual uranium-bearing groundwater, MXene-HEPBA achieved approximately 59% U(VI) removal, corresponding to an uptake capacity of 47.612 mg/g after pH and flow-rate optimization. Mechanistic analyses revealed that U(VI) was mainly immobilized as coordinated uranyl-like species through coupled electrosorption, surface complexation, and multisite coordination involving MXene surface terminations and HEPBA coordination sites. These results demonstrate its potential as a regenerable HCDI cathode for electrochemical purification of uranium-contaminated groundwater.
Ball-in-ball structures assembled of core(s) and shell(s) with void interior space has aroused great research interests for efficient energy storage and conversion applications owing to their unique morphology effect and consequently remarkable performance. This review systematically summarizes the recent advances in synthesizing well-defined ball-in-ball structured materials and their structure-property-performance relationship in energy storage and conversion fields. Initially, this review outlines of recently reported synthetic methods of ball-in-ball structured materials and fabrication mechanisms, including hard template method, soft template method, template free method and emerging method. Then, the important applications, including photocatalysis, electrocatalysis, lithium-ion batteries, dye-sensitized solar cells (DSSC) and supercapacitor, as well as the great advantages induced by morphology effects were elaborately discussed. Finally, key prospects and challenges for future development are highlighted to inspire further advancements and application of ball-in-ball structured materials across various fields.
Recently, cobalt-based heterogeneous catalysts have become a promising avenue in the propane dehydrogenation (PDH) process, due to their remarkable hydrocarbon activation ability and economic viability. However, achieving highly efficient and stable catalytically active Co species for the PDH reaction continues to pose a significant challenge. Herein, we constructed a hollow silicalite-1 (S-1) zeolite architecture stabilized by a highly dispersed, uniform, and nanosized CoO catalyst (CoO@S-1) derived from the uniform S-1 zeolite precursor prepared by a microliquid-film reactor-assisted hydrothermal method. The results showed that the ultrafine CoO nanoparticles were homogeneously immobilized on the outer shell matrix and inner walls of the hollow S-1 zeolite. As-constructed CoO@S-1 catalyst achieved an impressively high propylene production rate of 1596 mmolC3H6gCo -1h-1 in PDH at a 1.6 h-1 propane space velocity and 600 degrees C. Additionally, the catalyst delivered an unprecedentedly high propylene production rate of 44.5 mmolC3H6gcat -1h-1 at a higher space velocity of 6.0 h-1, far surpassing those of state-of-the-art cobalt-based PDH catalysts. It was unveiled that the superior catalytic PDH efficacy of the catalyst was mainly ascribed to the formation of highly dispersed and ultrafine active CoO species stabilized on the hollow S-1 zeolite through Co-O-Si structures formed by consuming abundant skeletal silanol groups of the zeolite precursor, thereby leading to enhanced activity, propylene selectivity, and structural stability. The present study affords a promising way to construct high-performance S-1 zeolite-immobilized metal-oxide catalysts for advanced alkane dehydrogenation applications.
Nickel oxide (NiOx), an efficient inorganic hole transport layer (HTL), has emerged as a key material driving the industrialization of inverted perovskite solar cells (PSCs). Its success stems from favorable energy-level alignment, excellent charge transport features, high stability, and low cost. Among various preparation methods, solution-based syntheses are particularly attractive for NiOx-based PSCs, due to their simplicity, compatibility, and scalability. This review systematically summarizes four mainstream solution-based techniques for synthesizing NiOx HTLs, including pre-synthesized nanoparticles, sol-gel, solution combustion, and chemical bath depositions. For each method, we discuss the reaction mechanisms and processing features, the resulting film properties, and strategies for performance optimization in PSCs. We then outline challenges associated with each route and highlight recent advances in material modification, process engineering, and structural design aimed at overcoming these bottlenecks and enhancing device efficiency. Further research should address critical issues such as uniformity control in large-area, rapid synthesis processes and reliable preparation of high-crystallinity, low-defect films at low temperatures. A deeper understanding of the relationships among solution processes, microstructure, and device performance will be essential for fully realizing the potential of solution-based NiOx HTLs in high-performance, high-stability, and low-cost perovskite photovoltaic technologies.
The performance of zeolites can be strongly influenced by their morphologies and internal porous structure. Due to the low premixing efficiency of precursor mixture solutions during conventional zeolite synthesis, it is difficult to synthesize a uniform ZSM-5 zeolite. In this study, we report a rapid and highly efficient method for synthesizing uniform nanosized ZSM-5 zeolite using a hydrothermal approach facilitated by a microliquid-film reactor (MLFR), without the addition of crystal seeds. The results demonstrated that the MLFR significantly improved the micromixing of high-viscosity zeolite precursor mixture solutions in a short duration, thereby substantially accelerating the subsequent silicon source hydrolysis, polycondensation, nucleation, and crystal growth processes during ZSM-5 zeolite synthesis. Compared to ZSM-5 zeolite synthesized by the traditional hydrothermal method using a mechanical stirring tank, the MLFR-derived ZSM-5 zeolite exhibited smaller particle size, improved crystallinity, higher specific surface area, excellent hydrothermal stability, and a more developed pore structure. Notably, the MLFR-derived ZSM-5 zeolite achieved a high propylene selectivity of approximately 55.08%, an unprecedentedly high selectivity of light olefins (89.92%), and a long catalytic life of 126 h in the methanol-to-propylene (MTP) reaction, mainly attributable to the increased accessibility of acid sites and the reduced diffusion pathways in smaller ZSM-5 zeolite particles. This study offers a promising strategy for the high-efficiency synthesis of uniform nanosized ZSM-5 zeolite and provides a deeper understanding of the enhanced catalytic performance of ZSM-5 zeolites in the MTP reaction.
The widespread deployment of rechargeable batteries is central to the global transition towards clean energy, yet their long-term stability remains a challenge. Electrode degradation, manifested through interfacial reactions, structural disorder and gas evolution, elevates internal resistance, accelerates capacity loss and complicates recycling. Surface coatings can stabilize electrode–electrolyte interfaces, suppress parasitic reactions and enhance structural resilience. In this Review, we survey coating technologies for high-energy battery active materials, including nickel-rich (nickel content ≥60%) cathodes, graphite and silicon anodes, and lithium metal. Wet-chemical approaches offer strong compositional tunability and compatibility with scalable manufacturing; gas-phase methods enable nanometre-scale, ultrathin and highly conformal interfacial control; solid-state strategies provide solvent-free processing pathways; and emerging methods enable rapid and multifunctional coating routes across a broader range of material and process conditions. The industrial adoption of these coating technologies depends on balancing electrochemical gains with process scalability, cost and recycling compatibility. Future progress will rely on multifunctional and adaptive coatings, in situ process monitoring and green chemistries to support durable and circular battery systems. Surface coatings for active materials stabilize the electrode–electrolyte interface and mitigate battery degradation, but their effectiveness and scalability vary across materials and deposition methods. This Review discusses the trade-offs of wet-chemical, gas-phase, solid-state and emerging coating technologies.
The anti-wear performance of spherical plain bearings directly affects the equipment's service life and operational reliability. Constructing a porous surface combining oil storage capacity and high hardness is an important approach to enhancing oil-lubricated wear resistance. However, bearing steel is a non-valve metal, making it difficult to achieve stable arc initiation and high-quality coating growth during conventional MAO. To address this issue, this study designed a phosphate–silicate composite electrolyte system, which enabled direct MAO on 42CrMo spherical plain bearing steel without any pretreatment, and induced hydrogen-dominated sustained deflagration behavior. The discharge characteristics, growth mechanism, microstructure, mechanical properties, and oil-lubricated tribological performance of the coating were systematically investigated.The results indicate that the direct arc initiation without pretreatment originates from an equivalent passivation layer formed synergistically by an anodic gas film and a SiO2 deposition layer. The sustained deflagration continuously inputs high-density energy into localized regions, promoting coating growth and forming a hard oil storage structure. As the sustained deflagration proceeds, the coating hardness increases from 182.12 HV to 341.37 HV, representing an enhancement of 87.44%. Meanwhile, the minimum wear rate under contact friction conditions reaches 2.71×10-4 mm3/(N·m), and further decreases to 4.28×10-5 mm3/(N·m) under oil-lubricated conditions. This study demonstrates that the hard oil storage structure can continuously store and release lubricating oil, forming a stable lubricating film at the friction interface, thereby significantly improving the wear resistance and service life of the coating. This work provides a new approach for MAO strengthening of non-valve metal spherical plain bearing surfaces.
Currently, the rapid synthesis of SSZ-13 zeolite featuring uniform morphology and small size by the conventional hydrothermal method is highly challenging due to the formation of highly viscous and inhomogeneous precursor gel formed under mechanical stirring. Herein, we report a rapid synthesis of SSZ-13 zeolite using a micro-liquid-film (MLF) reactor-mediated approach. It was demonstrated that the MLF reactor greatly intensified the micro-mixing of zeolite mixture precursor suspensions within a short time of only 10 min, thereby ensuring the formation of more uniform starting precursor gel and sufficient contact between the silica source and the template, thereby facilitating the creation of more building units of the CHA-type framework during hydrothermal treatment, greatly accelerating the subsequent nucleation and crystal-growth processes of SSZ-13 zeolite. Through regulating the premixing of precursor solutions by precisely tuning the operating parameters of the MLF reactor, the SSZ-13 zeolite with high crystallinity was completely synthesized with a short hydrothermal time of 12 h, and the morphology, pore structure, and acidity of SSZ-13 zeolites could be effectively controlled. The synthesized SSZ-13 zeolite possesses a high surface area and uniform cubic morphology. Moreover, with the aid of both the MLF reactor and commercial SSZ-13 zeolite crystal seeds, uniform submicron-sized SSZ-13 zeolite could be achieved with a significantly shortened hydrothermal time of 3 h. Notably, the as-synthesized SSZ-13 zeolite exhibited excellent catalytic methanol-to-olefins performance, with a catalytic lifetime more than two times longer than that of SSZ-13 zeolite synthesized without the aid of the MLF reactor.