To advance sustainable hydrogen production, we developed an acid-etching strategy to enhance perovskite oxides for oxygen evolution reaction (OER). This method preferentially removes A-site cations (La, Sr), accompanied by slight Ni loss, inducing A-site deficiency and oxygen vacancy while exposing B-site centers. The etched perovskite oxide (H-LBO) achieves superior OER activity with a low overpotential of 213 mV at 10 mA cm-2 in 1 M KOH, outperforming pristine perovskite oxide (LBO, 285 mV) and commercial RuO2 (389 mV). This work offers a simple approach to modulate surface defects and electronic structures for cost-effective, highperformance OER electrocatalysts.
Sodium-ion batteries (SIBs) represent a compelling alternative to lithium-ion batteries (LIBs) for large-scale industrialization, primarily due to their cost-effectiveness, enhanced safety profiles, and superior performance in cold climates. Within the spectrum of cathode materials, sodium-based layered transition-metal oxides (NaxTMO2) stand out for their high energy density and manufacturing scalability. Nevertheless, practical deployment is severely impeded by surface and interfacial instabilities triggered by environmental exposure and electrolyte interactions. This paper offers a comprehensive review of the interfacial instability mechanisms in NaxTMO2, encompassing their origins, evolutionary pathways, mitigation strategies, and cutting-edge characterization techniques. We begin by elucidating the fundamental thermodynamics and kinetics governing surface and interfacial behaviors, demonstrating how the coupling of bulk and interface evolution induces structural degradation and capacity decay. Subsequently, we systematically classify stabilization strategies—including bulk-phase engineering, interfacial architecture design, and electrolyte optimization—evaluating their efficacy in addressing specific failure modes. The critical roles of in situ and operando characterization in decoding interfacial evolution under coupled electrochemical, mechanical, and chemical stresses are also analyzed. Finally, we propose future research directions for interface stabilization, highlighting the imperative to translate fundamental insights into actionable design principles for SIBs and next-generation energy storage systems.
The active site of MoS2, predominantly located at the crystalline edge, limits selectivity for the CO2 reduction reaction (CO2RR). Single-Atom Catalysts (SACs), have emerged as a promising avenue to enhance the catalytic performance of MoS2, owing to their high catalytic selectivity on the basal plane and tunable activity in various chemical reactions. In this regard, transition metals from the 8B and 1B groups (Cr, Cu, Sc, Ti, V, and Ni) were investigated as dopants on the basal plane for the first time, employing first-principles calculations based on a 4 × 4 × 1 supercell of the MoS2 monolayer. The Ti/MoS2 catalyst was identified as the most stable among the SACs, attributed to its optimal formation energy. Various Ti-doped models were analyzed, encompassing energy band structure, density of states, charge differential density, Bader charge, and Gibbs free energy. Our findings indicate that Ti induces diminished electron binding, thereby weakening C[double bond, length as m-dash]O with lower energy, consequently enhancing the availability of surface sites and facilitating catalytic reactions. In our investigation of possible reaction pathways, the preferred CO2RR pathway was identified as the reverse water gas conversion (RWGS), with the rate-limiting step being CO2 hydrogenation into carboxyl (*COOH). The Ti modification model on the MoS2 basal surface demonstrated exceptional catalytic performance, reducing the rate-limiting step to 0.177 eV, which is 17 times lower than that of pure MoS2. These calculational results provide valuable theoretical insights for designing highly efficient SACs on MoS2-based functional materials.
Amorphous metal-selenium (M-Se) alloys hold promise for applications such as catalysis, electronics, and surface-enhanced Raman spectroscopy (SERS) sensing due to their surface reactivity, isotropic properties, and tunable bandgap. However, controlling the synthesis of nanostructured noble-metal-based M-Se materials is difficult, as the strong metallic bonding and low chemical reactivity of noble metals hinder homogeneous selenization. Here we show a one-step micellar self-assembly reduction method to produce amorphous semiconducting Rh-Se mesoporous nanospheres (a-Rh-Se MNs). We systematically investigate how composition, surface curvature, and crystallinity affect SERS performance. a-Rh-Se MNs with low curvature and high amorphization achieve enhanced sensitivity toward typically non-adsorbing, low-polarizability analytes, including hexachlorobenzene, anthracene, and polytetrafluoroethylene microplastics (even in wastewater). Combined experimental and theoretical analyses reveal that co-modulating curvature and amorphization tunes key electronic descriptors (e.g., d-band center and work function), thereby promoting resonant charge transfer. This finding overturns the conventional paradigm that prioritizes high-surface-area substrates. Our work establishes mesostructured a-Rh-Se for SERS applications and provides insights into M-Se surface chemistry for designing advanced SERS materials.
Inverted perovskite solar cells (PSCs) garner extensive attention for improved operating stability but the power conversion efficiency (PCE) still lags behind its theoretical limit. The energetic losses responsible for this PCE deficit primarily stem from non-radiative recombination induced by crystalline defect states in the perovskite bulk and at interfaces, coupled with inefficient carrier extraction caused by energy level mismatches across adjacent interfaces. Here, a tailored additive engineering strategy is proposed by designing a planar molecule 4-Cyanobenzamide (4-CBA) that features multifunctional active sites for the perovskite precursor. The dual electron-rich moieties C & boxH;O and C equivalent to N can strongly anchor uncoordinated Pb2+, thereby stabilizing the [PbI6]4- framework and alleviating internal residual strain. The enhanced & horbar;NH2 group, acting as both a hydrogen bond acceptor and donor, compensates for vacancy defects through interactions with FA+/I-, regulating the preferential growth of crystal planes, and reducing non-radiative recombination. Notably, 4-CBA with a planar structural orientation can also tune energy level matching, minimize interfacial steric hindrance, and optimize carrier transport balance. The champion PSC device based on 4-CBA achieves a PCE of 26.25% and an exceptional fill factor (FF) of 85.97%.
Herein, a novel 3D flower-like ZnCo MOF-modified Bi2WO6 is first fabricated via a simple solvothermal approach and applied for complete rhodamine B (RhB) photocatalytic degradation. First, granular flower-shaped BWO and cubic MOF are synthesized. The crystal structure, microscopic morphology, and surface element distribution of these materials are characterized, and their photocatalytic degradation performance toward RhB is evaluated. To clarify the feasibility of modifying the optical catalytic performance of BWO by MOF, a synergistic BWO-MOF composite photocatalyst was prepared, and an extremely high efficiency of 99.1% in the degradation of Rhodamine B within 1 h is achieved. Photoelectrochemical measurements are performed to verify the enhanced separation and transfer of photogenerated charges. Meanwhile, a plausible visible-light-driven photocatalytic degradation mechanism for the BWO/MOF system is proposed, which provides a theoretical basis for regulating photogenerated charge separation and achieving efficient photocatalytic degradation.
Integrated energy systems (IESs) coupled with renewable energy and power-to-gas technologies provide an effective pathway for renewable-energy accommodation and carbon reduction. However, conventional power-to-gas systems generally rely on fixed syngas compositions and predetermined product routes, limiting flexibility under time-varying market conditions. This paper proposes a flexible multi-product low-carbon dispatch strategy for a solid oxide electrolysis cell (SOEC)-based IES through syngas composition regulation. Unlike previous thermoneutral SOEC studies focused on steady-state steam electrolysis for hydrogen production, the established polarization-based formulation is extended to H₂O/CO₂ co-electrolysis by coupling reverse water-gas shift equilibrium with a variable feed ratio. The resulting model links the inlet H₂O/CO₂ ratio, outlet H₂/CO ratio, cell voltage, thermoneutral state, and stack power. A multi-product coordination mechanism jointly optimizes the SOEC feed ratio and methanol–synthetic-natural-gas pathway under time-varying electricity and product prices. A bi-level Stackelberg framework further coordinates production and carbon-trading decisions with electricity, heat, gas, and CO₂ dispatch while enforcing thermoneutral operating and power-ramping constraints. Six comparison cases quantify the effects of feed-ratio regulation and product switching. The proposed strategy achieves a daily net profit of 4,414.38 CNY, an ROI of 88.15%, and an energy efficiency of 83.86%, while daily net emissions reach −136.91 kg under the defined accounting boundary. The corresponding unit profit of carbon abatement reaches 6.80 CNY/kg, confirming the value of composition-aware multi-product dispatch.
Achieving selective CO2 methanation under photothermal conditions requires catalysts capable of maintaining non-equilibrium interfacial states that balance reduction and oxidation processes-an ability rarely attainable through conventional thermal synthesis. Here, we propose a rapid Joule-heating strategy that injects energy in a kinetically non-equilibrium, current-induced manner, triggering rapid exsolution of nanoparticles and electronic reconstruction within seconds. This approach creates LaNiO3-La2NiO4 heterostructures embedded with socketed alloying Ni-Fe nanoparticles, where the coupled oxygen migration and charge redistribution give rise to electronically modulated metal/oxide interfaces. The kinetically confined process produces finely dispersed, electronically asymmetric active sites while avoiding the structural degradation typical of slow thermal treatments. The optimized catalyst (LNF-JH1100) achieves a CH4 production rate of 166.5 mmol g(-1) h(-1) with >97% selectivity at 350 degrees C, showing a remarkable activity, selectivity, and stability. Combined spectroscopic and theoretical analyses reveal that this non-equilibrium interface modulates the local electron density and intermediate binding sequence, and is associated with a shift in the dominant reaction pathway from a single HCOOH-mediated surface hydrogenation pathway prone to CO release to a cooperative HCOO/HCOOH cycle that promotes direct CH4 formation. This work demonstrates the potential of rapid Joule heating as an effective route to couple structural exsolution with electronic reconfiguration, offering new opportunities for the rational design of adaptive, high-performance photothermal catalysts.
Developing efficient electrocatalysts for the oxygen evolution reaction (OER) is imperative for electrochemical energy conversion devices such as water electrolyzers and metal-air batteries. Rationally modulating the charge localization by constructing a built-in electric field (BEF) is a compelling strategy to boost OER performance, but it remains highly challenging. Here, this work successfully integrates the Ru/Ni co-mixed oxide (RNO) and the acid-etched perovskite oxide LaCo0.9Fe0.1O3 (H-LCFO) to construct a RNO/H-LCFO heterojunction catalyst. Experimental characterization confirms that H-LCFO increases the interfacial work function difference and reverses the direction of the built-in electric field (BEF), driving electron transfer from the H-LCFO to RNO and facilitating the lattice oxygen mechanism (LOM) for OER. Consequently, the RNO/H-LCFO achieves an overpotential of 260 mV at a current density of 10 mA cm-2 in alkaline solution. When employed as an air cathode in a Zinc-air battery, it delivers a higher peak power density of 124.2 mW cm-2 than that of Pt/C+RuO2 and exhibits stable cycling over 180 h. This work demonstrates that defect engineering of perovskite oxides can effectively manipulate the interfacial BEF direction, offering a promising design strategy for high-performance, cost-effective OER electrocatalysts.
Surface flashover is an important factor in the design of the oil-paper insulation of converter transformers, but its underlying mechanism remains unclear yet. In this paper, the relationship between flashover overvoltage and the increase in electrode distance under uniform field distribution is investigated. The flashover strength ratio λ, defined as the flashover field strength at the oil-solid interface divided by that of pure oil, shows a “U-shaped” curve for oil-paper samples. However, for oil-PTFE interfaces, this λ value changes slightly when the electrode distance is large. These phenomena are attributed to the effect of the electric double layer (EDL), which leads to the variation of charge distributions in the diffusion layers at the oil-solid interface. Furthermore, in order to study the EDL, an experiment is designed to measure the interface conductivity, and the surface potential distribution at the interface is measured by Kelvin Probe Force Microscopy (KPFM). Both experimental results confirm that the charge density in the EDL of the oil-paper interface is much larger than that of the oil-PTFE sample, and the “U-shaped” curve of the λ value in the oil-paper sample is explained in terms of field distortion due to the non-uniform charge distributions in the EDL.
Abstract Maximizing atomic utilization of noble metals is essential for high-efficiency electrocatalysis. However, small-sized noble metal nanoparticles (NPs) often struggle to achieve both high activity and structural stability. Here, we demonstrate that ultrafine Pd NPs (sub-3 nm) can be stabilized at a carbon-supported, short-range-ordered FeCoNiB mesoporous matrix. Through precise control of the Ni/Co ratio of FeCoNiB and Pd loading, the resulting material features a well-defined mesoporous architecture with abundant crystalline–amorphous interfaces. The optimized Pd4.4-FeCoNiB electrode with 4.4 at. % Pd loading shows a high mass activity (3.41 A mgPd–1), a Faradaic efficiency up to 98.81%, and durability toward electrocatalytic conversion of waste polyethylene terephthalate-derived ethylene glycol (EG) into value-added glycolic acid (GA). These improvements stem from strong electronic and interfacial coupling between FeCoNiB and Pd, which is further stabilized by short-range ordering in the amorphous alloy. Such interactions not only enhance the structural integrity of Pd active sites but also facilitate EG activation and GA desorption. This work highlights a promising interfacial design route for developing cost-effective and durable low Pd-loading electrocatalysts for plastic upcycling.
Passivating both bulk and surface defects in perovskite films represents an effective strategy to suppress nonradiative recombination losses and enhance the photovoltaic performance of perovskite solar cells. Herein, we propose a symmetry-breaking strategy for synergistically passivate grain boundary and bulk defects by employing Piperazine dihydrochloride (PDCl) and its derivative 1-(4-Chlorophenyl)piperazine dihydrochloride (4CPPDCl) as interfacial modifiers. Compared to PDCl, the introduction of a chlorophenyl side chain onto the piperazinium cation in 4CPPDCl provides a stronger molecular dipole moment and more passivation sites, enabling efficient passivation of perovskite surface defects. Meanwhile, 4CPPDCl treatment induces surface reconstruction and secondary grain growth, further improving film quality, while also optimizing the perovskite/ ETL energy-level alignment to reduce non-radiative recombination. Consequently, the champion 4CPPDClpassivated device achieves a power conversion efficiency (PCE) of 26.62 %, with an open-circuit voltage (Voc) of 1.192 eV and a fill factor (FF) of 86.34 %. The scalability of this approach is demonstrated by perovskite solar modules reaching 22.61 % efficiency. Moreover, the device exhibits outstanding operational stability, retaining 92.3 % of its initial PCE after 1000 h of continuous maximum power point tracking.
Protonic ceramic fuel cells (PCFCs) are one of the most promising energy conversion technologies because of the high efficiency and environmental friendliness. However, the lower operating temperature causes sluggish reaction kinetics and degradation, especially for the cathode side. In this work, Ruddlesden-Popper (R-P) perovskite Sr3Fe2O7-s is optimized by doping Pr at A-site, leading to an enhancement of electrical conductivity and polarization resistance. Higher oxygen vacancy concentration and larger active area facilitate the ion conduction and oxygen reduction reaction, increasing the electrochemical performance by 14%. These results demonstrate the potential of Sr3-xPrxFe2O7-s as active cathode for PCFCs.
The co-electrolysis of H2O and CO2 in solid oxide electrolysis cells (SOEC) enables the simultaneous production of H2 and CO, which is a critical pathway for power-to-gas (P2G) technologies. The reaction mechanisms of SOEC co-electrolysis are more complex than those of conventional SOECs operating on water electrolysis. Additionally, multiphysics coupling processes such as heat and mass transfer are highly intricate, which poses greater challenges for modeling and analyzing syngas production. In this study, a 3D multiphysics SOEC model is established and validated, enabling a novel application of 3D modeling to the detailed parametric analysis of syngas production. The key design and operational parameters were examined to identify factors affecting syngas production. The results show that moderately extending the channel length (<= 1.5 times the original length) enhances H2 yield with favorable efficiency. A moderate inlet flow rate can better balance the gas production rate and reactant utilization, while a higher flow rate helps alleviate reactant starvation and reduce thermal losses. Pressurization enhances CO production significantly, even surpassing the expected increase. Higher temperature favors RWGS, thus enhancing CO formation under H2-rich conditions and enabling efficient coproduction under unbalanced feed conditions. For CO-rich feeds, higher temperatures combined with extended reaction time further increase CO yield while maintaining stable H2 output. For example, raising the temperature from 1023 K to 1123 K increases CO concentration nearly fourfold (1.82 mol/m3 -> 7.08 mol/m3). This work provides theoretical guidance for high-efficiency syngas production in large-scale SOEC systems.
The development of efficient and cost-effective electrocatalysts for the oxygen evolution reaction (OER) is crucial for advancing green hydrogen production via water electrolysis. While perovskite oxides represent promising non-noble metal catalysts, their OER performance is often limited by poor conductivity and insufficient active site exposure. In this work, we report a rapid and versatile plasma engineering strategy to significantly enhance the OER activity of perovskite oxides LaMO3 (M = Fe, Co, Ni). The modified catalyst (V-LaFeO3) exhibits increased specific surface area, abundant oxygen vacancies, and improved charge transfer capability. As a result, V-LaFeO3 achieves a low overpotential of 332 mV at a current density of 10 mA cm- 2, outperforming both pristine LaFeO3 and commercial RuO2. The universality of this approach is further demonstrated with LaCoO3 and LaNiO3 oxides, which also show enhanced OER performance after plasma treatment. This study highlights plasma engineering as a general and efficient strategy for designing high-performance perovskite-based electrocatalysts for sustainable energy applications.
Polypropylene (PP)/polyolefin elastomer (POE) blends are promising cable insulation materials due to their excellent electrical and mechanical properties. However, their flammability, melt-dripping behavior, and significant smoke emission pose serious safety hazards, limiting their applications in high-safety-demand fields. In this work, a synergistic flameretardant system composed of piperazine pyrophosphate (PAPP) and melamine polyphosphate (MPP) was introduced into the PP/POE blend via melt blending. At a PAPP: MPP mass ratio of 3:1, the composite achieved a UL-94 V-0 rating and a limiting oxygen index (LOI) of 37.5%. Cone calorimetry test (CCT) results revealed that compared with neat PP/POE, the peak heat release rate (pHRR) and total heat release (THR) were significantly reduced by 91.5% and 84.9%, respectively, and the total smoke release (TSR) decreased by approximately 96%, indicating effective suppression of heat and smoke release. The designed flame-retardant PP/POE composite achieves an optimal balance among flame retardancy, mechanical properties, and electrical performance, providing fundamental insights for the rational design of highly efficient halogen-free flame-retardant PP cable insulation materials.
Dynamic charge transport in polymer materials is fundamental to improve insulation performance. However, it is challenging to understand migration mechanisms at the nanoscale in polymer composites under high temperatures. Herein, polypropylene (PP) films by solution crystallization are fabricated. We use Kelvin probe force microscopy to explore the charge migration of PP polycrystalline microregions. The accumulation and dissipation rate obey the exponential law. Charge injection barrier ofα-PP is lower than that ofβ-PP under normal conditions, which is mainly influenced by the surface conductivity. The charge transport rate enhances with the field strength. By constructing the heating system, the migration rate is found to increase with temperature. Furthermore, the irregular structure ofβphase introduces more shallow traps, promoting charge transport at high temperatures. Charge migration states of two phases tend to be consistent above 100 °C. Anin-situmicro-region dielectric constant testing method is proposed. The dielectric constant ofβphase is slightly higher. Specifically, its reverse increase beyond 100 °C is primarily attributed to interface polarization and the enhancement of dipole orientation. The observation aligns well with bulk experiments. This study provides crucial insights into the microregion charge behavior of polymer dielectrics at high temperatures.
Solid Oxide Electrolysis Cell (SOEC) technology, recognized for its high energy conversion efficiency, offers a promising pathway for converting CO2 electrochemically into valuable chemicals, thereby contributing to carbon neutrality goals. However, the widespread adoption of SOEC is hindered by the limited catalytic performance of conventional fuel electrodes based on Ni-YSZ. To address this challenge, this work develops the novel fuel electrodes composed of layered perovskite oxides, (La4Sr4)0.9Ti7.2 & times;0.4Cu0.4O26 (LSTXCu, where X = Ni, Co, Fe), decorated with exsolved Cu-X alloy nanoparticles via a Cu-induced process at low temperature. The in-situ formed X-Cu alloy nanoparticles, creating heterogeneous interfaces with the perovskite substrate, significantly enhance the electrocatalytic activity towards the CO2 reduction reaction (CO2RR). Electrochemical analysis exhibits that the full cells with the LSTXCu-r fuel electrode exhibited outstanding CO2 electrolysis performance, delivering maximum current densities of 1.98 A cm-2 at 2.0 V and 850 degrees C in pure CO2 atmosphere. The values represent a substantial performance improvement of 152.3 %, compared to cells using LSTX-r electrodes with sole exsolved X metal nanoparticles.
Solid oxide fuel cells (SOFCs) are a promising energy conversion technology with high efficiency and environmental compatibility. Applied as anode materials, perovskite oxides govern the electrochemical performance, with an exsolution strategy for enhancing catalytic activity. In this work, Sr2Fe1.5Mo0.5O6-delta exhibits an A-site deficient surface enriched with Sr and O vacancies via the acid etching method, thereby exposing B-site cations and facilitating the nucleation process during exsolution. The optimized Fe nanoparticles distribution enhances the H2 adsorption and H2O desorption, resulting in a 25 % increase of the peak power density to 1.04 W cm-2 from 0.83 W cm- 2 at 800 degrees C. The ingenious design of surface reconstruction demonstrates significant potential in advancing perovskite-based electrocatalysts for SOFCs.
Lattice strain engineering induced by heteroatom doping serves as an effective approach to precisely regulate the electronic structure and enhance the intrinsic activity of catalysts. However, the synergistic role of bimetallic co-doping in steering the strain effect and its impact on the catalytic performance remains to be explored. Herein, we introduced Ni and Ru co-doping in barium titanate (Ba0.9Ti0.8Ni0.1Ru0.1O3-delta, BTNR22) with the lattice expansion strain, where Ni serves to induce lattice strain, and Ru stabilizes the crystal structure and modulates the electronic structure of active sites. The porous BTNR22 catalyst exhibits enhanced performance for photothermal CO2 methanation, with a CH4 evolution rate of 126.93 mmol & centerdot;g-1 & centerdot;h-1 at 400 degrees C, 373 times higher than that of Ba0.9TiO3-delta. In addition, the in situ diffuse reflectance infrared Fourier-transform spectroscopy (in situ DRIFTS) and density functional theory (DFT) calculations reveal that the lattice expansion strain narrowed the bandgap of the catalyst, and the Ru-VO active sites facilitated the thermodynamically favorable pathway, synergistically enhancing the adsorption and activation of CO2 and the photogenerated carrier dynamics. This study offers a promising avenue for constructing highly active catalysts via strain engineering and mechanistic insight into the correlation between photothermal catalysis and the strain effect.