Electrochemical CO2 reduction (CO2RR) holds promise for sustainable fuel and chemical production but faces fundamental challenges rooted in limited CO2 availability and high activation reaction barriers. These issues manifest as slow kinetics, low selectivity, and poor stability under industrial operational conditions. While the catalyst/electrolyte interface engineering plays a decisive role in modulating the local microenvironment, which directly influences the kinetics and thermodynamics of CO2RR, current understanding remains fragmented due to the complex interplay of interfacial factors. Herein, in this review, we address this gap by moving beyond conventional categorization by materials or products. We present a unified mechanism-oriented framework that directly links interfacial design strategies for tackling the core challenges of CO2 availability, site accessibility, and reaction affordability. We systematically decouple the interface interactions and survey interfacial engineering strategies for CO2 reduction, including mass-transport control, electrostatic microenvironment tuning, molecular functionalization, and device–interface engineering. By elucidating the mechanistic principles behind these strategies and their interconnections, this review provides actionable guidelines for engineering robust interfaces that break inherent trade-offs among activity, selectivity, and stability. We aim for this perspective to not only advance understanding of microenvironment modulation but also accelerate the development of scalable, carbon-neutral energy conversion technologies.
For decades, the industry has believed that spherical graphite (SG) yield correlates strongly with graphite flake size. To clarify natural graphite (NG) spheroidization mechanisms, a comprehensive evaluation was conducted by extracting intermediate products from an industrial production line and utilizing separated jet mills to simulate continuous processing in the study. Focused ion beam-scanning electron microscope (FIB-SEM) cross-sectional analysis and nanocomputed tomography (Nano-CT) imaging revealed that flakes of different thicknesses underwent distinct morphological changes (folding, bending, or fragmentation) under mechanical force, with only flakes above a critical thickness (∼2 μm) forming SG cores. Statistical correlation between thickness (measured via statistical method under SEM) and yield demonstrated that thickness—not only size—is the dominant factor, redefining “effective SG flakes” to include small but thick flakes. Therefore, prioritizing thickness protection over size preservation in grinding-flotation and spheroidization processes increased SG yield by 7% in industrial validation. The work provides new insights for high-efficiency SG production.
ZnIn2S4 (ZIS) has garnered significant interest in photocatalytic energy conversion and environmental remediation due to its tunable band gap, strong visible-light response, and facile synthesis. However, its practical application is severely hindered by inherent limitations, including low charge carrier separation efficiency and sluggish surface reaction kinetics. Constructing heterojunctions has emerged as an effective strategy to enhance ZIS performance by leveraging precise band alignment and interface engineering to optimize charge separation. While excellent reviews on ZIS-based photocatalysis have been published, comprehensive reviews focusing specifically on the design and evaluation of ZIS-based heterojunctions remain scarce. This review systematically summarizes recent advances in ZIS-based heterojunctions, providing a detailed discussion of heterojunction types and key synthesis strategies. Multi-scale modification strategies for synergistically enhancing photocatalytic activity are also examined. Furthermore, the charge separation mechanisms and surface reaction pathways are elucidated through advanced in situ characterization techniques and density functional theory (DFT) calculations. ZIS-based heterojunctions demonstrate great potential across various photocatalytic applications, including H2 evolution, CO2 reduction, H2O2 production, N2 fixation, pollutant degradation, and emerging fields such as plastic reforming and tumor therapy. Finally, future research directions are outlined, encompassing crystal phase regulation, adaptive heterojunction design, and AI-driven screening, thereby providing theoretical guidance for the development of highly efficient ZIS-based photocatalysts.
SnSe2 is a promising thermoelectric (TE) material with intrinsic n-type characteristics and a high theoretical ZT value of 2.95 along the a-axis. However, its densely packed crystal lattice in the plane perpendicular to the c-axis leads to weak phonon scattering, limiting improvements through conventional defect or nanostructure-based strategies. In this study, the rare-earth element Yb is introduced into tin-rich SnSe2, predominantly segregating at grain boundaries and enhancing phonon scattering, while a small fraction incorporates into the lattice and modifies the electronic structure, simultaneously tuning both electrical and thermal transport behaviors. Yb incorporation enhances multiple phonon scattering mechanisms, significantly reducing lattice thermal conductivity, reaching a minimum of ~0.48 W·m−1·K−1. Meanwhile, it modulates the electronic structure by introducing impurity states, altering band alignment, and enhancing band degeneracy, collectively increasing the density-of-states (DOS) effective mass and Seebeck coefficient, contributing to a maximum power factor of 436.47 μW·m−1·K−2 at 773 K. As a result, the Yb-doped SnSe2 sample with 1.0 wt% achieves a peak ZTmax of ~0.53 at 773 K along the direction parallel to the pressing direction, representing an ~95.3% enhancement over the undoped sample. This study presents a synergistic and effective strategy for optimizing SnSe2-based TE materials via rare-earth doping, paving the way for next-generation high-performance TE devices.
The practical application of solid polymer electrolytes (SPE) is limited due to notorious high crystallinity and low ionic conductivity. Existing research concentrated on reducing crystallinity and increasing Li salt concentration have made certain process. However, the segmentation and isolation effects of large and numerous grains on amorphous region have always been overlooked and the effect of grain size remains largely unexplored. Herein, take polyethylene oxide (PEO) as an example, “grain size refinement” strategy is adopted to improve the related room-temperature ionic conductivity by simply placing PEO based SPE on Li sheets coated with ester monomers and conducting in-situ polymerization. During these processes, in addition to reducing the interaction force between polymer chains and decreasing the driving force for crystallization, ester monomers are conducive to form interface with polymer clusters, which serves as additional nucleation sites and promotes the formation of refined grains. Then instantaneous high-temperature provided by muffle furnace triggers rapid solidification of monomers, leading to the locking of refined grain structure and the formation of more interconnected amorphous regions. Time-of-flight secondary ion mass spectrometry and polarization microscope confirm these processes, while small-angle X-ray scattering results indicate that the grain size reduces to one-third of its original size. Then the room-temperature conductivity increased by at least two orders of magnitude for PEO-based SPE.
As nature's most abundant renewable carbon source, biomass enables a closed–loop carbon-neutral paradigm for producing industrial oxygenates. Biomass electrocatalytic oxidation reaction (BOR) replaces the energy-intensive oxygen evolution reaction (OER), simultaneously achieving green synthesis of value-added oxygenates and enhancing electrolytic energy efficiency, thereby displacing fossil–based production routes. This review systematically elucidates the electrocatalytic conversion of biomass derivatives (e.g., alcohols, furanal, and sugars, etc.) into value-added products coupled with hydrogen production from the perspectives of catalyst design principles and reaction mechanisms. Further focus on integrated anode–cathode systems that synergistically couple biomass oxidation with cathodic carbon dioxide reduction (for fuel synthesis) or nitrate reduction (for ammonia production and pollutant remediation), overcoming limitations of standalone hydrogen generation while enabling coproduction of chemicals and carbon/nitrogen resource cycling. Advanced multi-field coupling strategies are analyzed for their efficacy in enhancing reaction selectivity and efficiency, including photo-electrocatalysis to excite charge carriers, thermo-electrocatalysis to optimize kinetics, and high-pressure electrocatalysis to regulate mass transfer. Future efforts should prioritize non-precious metal active site engineering and scalable reactor design to advance biomass refining from conceptual frameworks toward industrial implementation.
Wide-bandgap (WBG) perovskite solar cells (PSCs) are critical for tandem architectures but suffer from light-induced halide segregation and non-radiative recombination. Although conventional rare-earth doping passivates defects, it concurrently introduces vacancies and lattice strain that exacerbate halogen migration. Herein, we report a thermally induced doping strategy where Pr3+/Sm3+ ions pre-embedded in MeO-4PACz diffuse into the perovskite during annealing. Through combined tolerance factor analysis, structural characterization, and DFT calculations, we identify a dual doping mechanism: predominant interstitial incorporation with minor B-site substitution. This approach reduces defect density, increases iodine migration energy barriers (from 0.85 to 0.94 and 1.12 eV), and minimizes lattice distortion. Consequently, the experimental results show that the open-circuit voltage increases from 1.198 V to 1.230 V (Pr3+) and 1.233 V (Sm3+), and the fill factor increases from 83% to 86%. Finally, the PCE reached 23.04% (Pr3+) and 23.39% (Sm3+) (20.12% for control) with > 90% stability retention after 1500 h. In addition, the optimized semitransparent WBG device PCE was 19.48% (Pr3+) and 19.85% (Sm3+), and the PCE of 4-T perovskite was 27.05% (Pr3+) and 27.56% (Sm3+). This method will be beneficial for the development and application of WBG PSCs and TSCs.
Aqueous electrolytes, while conferring inherent safety advantages, inevitably induce hydrogen-evolution corrosion, resulting in nonuniform Zn deposition and shortened cycle life. Herein, a novel electrolyte with buffering function is designed to modulate ion behavior and stabilize interface pH. The introduced additive acts as a cushion maskant (CM) that spontaneously adsorbs onto the Zn metal surface, displacing interfacial water molecules and thereby suppressing corrosion. Simultaneously, its coordination with Zn2+ homogenizes the Zn2+ flux to promote uniform deposition. Moreover, the protonation/deprotonation equilibria of CM within the electrolyte buffer local pH fluctuations, stabilizing the interfacial microenvironment. Consequently, a beneficial solid electrolyte interphase (SEI) is established, which further shields the Zn anode, enhances interfacial stability, and markedly improves cycling durability. Accordingly, Zn//Zn symmetrical cells in CM-containing electrolyte can realize exceptional lifespan for 2800 h at 2 mA cm−2 and 970 h even at 10 mA cm−2. In addition, CM demonstrates the superior practical applicability in Zn//I2 full cells for long-term and rate tests. Zn//I2 pouch full cell can operate for 150 mAh with CM. This study offers a distinctive and comprehensive strategy for stabilizing the Zn anode.
This study explored thermal and electrodeposition impacts of distinct chaotic current waveforms to enhance current efficiency and reduce heat loss through the regulation of electrode interfacial reaction dynamics, advancing current efficiency, energy conservation, and carbon neutrality. Two universal control methodology was developed to achieve independent amplitude and offset boosting of arbitrary chaotic signals, implemented through a specially designed chaotic circuit. Three distinct waveforms (w-, F-, and G-signals) were systematically investigated for their thermal and electrochemical effects. Experimental and COMSOL simulation results demonstrated that Joule heating was governed by both fluctuation amplitude and frequency characteristics, following the sequence w < F < G. When the current density was about 1500 A/m2, the corresponding optimal voltage fluctuations were identified as 2.8 V (w), 0.51 V (F), and 0.23 V (G), yielding current efficiency improvements of 2.2%, 0.7%, and 5.1%, respectively, based on the electrodeposition experiments. Combining experiments on electrolytes at different temperatures with corresponding SEM characterization revealed that chaotic current suppresses manganese nodules not only through Joule heating-induced temperature rise, but also via effective regulation of the interfacial electrochemical environment, thus allowing effective inhibition even at lower temperatures. These findings provide both theoretical insights and practical methodologies for implementing chaotic currents in industrial electrodeposition processes.
Electrochromic (EC) fabrics exhibiting tunable optical and thermal modulation have attracted extensive attention in both active camouflage and wearable electronic. However, the lack of compatibility among the basic components of an EC device for flexible EC fabrics remains a challenge, hindering its future application. Herein, a highly integrated all-in-one EC fabric (AECF) is developed by assembling all the essential components into a piece of fabric, which is based on the dual-band EC polyaniline (PANI), Au collector, and a gel electrolyte filled into the fabric matrix. Benefiting from such a highly integrated configuration, the AECF possesses an ultrathin thickness of 82.0 μm and high flexibility, which could endow it with good conformity on arbitrarily shaped surfaces, further enhancing the applicability of the intrinsically non-stretchable EC fabrics device. Stemming from the optical modulation of the PANI EC layers, the AECF exhibits a color switch between golden yellow and dark green, with both visible and infrared reflectance modulation. Considering the excellent conformability and active optical-thermal modulation, the AECF is further developed into an environmental adaptive camouflage prototype system by integrating with a model car, which exhibits a fast color blending with dynamic environment background. This study is anticipated to provide new insights into developing high-performance EC fabrics toward the applications in wearable displays and active military camouflage.
Iron-based Prussian blue analogs (PBAs) represent promising, facile-to-prepare, and low-cost positive electrode materials for sodium-ion batteries. However, their practical application is hindered by the markedly irreversible three-phase transitions and severe lattice distortion that occur during sodium ion storage, leading to capacity limitations and diminished cycling stability. Herein, a simple pyrrole-induced phase transition engineering strategy is proposed to successfully transform monoclinic PBAs into cubic polypyrrole-PBAs (PPy-PBAs). In situ X-ray diffraction (XRD) testing and density functional theory (DFT) calculations reveal that the phase transition mechanism transforms from an unfavorable three-phase process to a highly reversible two-phase transition. Compared to complex three-phase transition (PBAs), the efficient two-phase transition (PPy-PBAs) exhibits smaller lattice volume contraction/expansion and less Fe-C/Fe-N bond length stretching/shrinking, demonstrating remarkable structural stability. Moreover, this strategy effectively reduced the energy barrier for sodium-ion (Na+) migration, with the density of states crossing the Fermi level, significantly enhancing electronic conductivity, and thereby facilitating redox reactions and Na+ transport kinetics within the material. The reversible two-phase transition enables sustainable sodium-ion storage through phase-transition engineering. Compared with PBAs that undergo structural distortion and significant lattice strain, the optimized positive electrode material demonstrates a discharge capacity of 136 mAh/g and an ultralong stable cycling lifespan of 1700 cycles, establishing new possibilities for advanced sodium-ion batteries.
Wearable heaters with multifunctional capabilities and high performance are in high demand for future personal thermal management. However, the development of such devices remains challenging due to limitations in flexibility, complex fabrication, inadequate Joule heating efficiency, insufficient electromagnetic interference (EMI) shielding, and poor antibacterial performance. Here, Ag@PEDOT heterostructures were decorated on laser-induced graphene (LIG) through a simple spray-coating process followed by a facile chemical synthetic method to deposit silver nanoparticles (AgNPs) onto the PEDOT layers. The resulting composite retains the intrinsic flexibility and comfort of the original graphene matrices, while demonstrating exceptional Joule heating characteristics—achieving a broad temperature range (30°C–100°C) at low operating voltages (0.8–2.6 V) and a rapid photothermal response (reaching 89.6°C within 180 s at 1.5 sun irradiation). Moreover, the material exhibits superior electromagnetic shielding effectiveness (33 dB in the X-band) and outstanding antibacterial activity, with an inhibition rate exceeding 95% against Escherichia coli and Staphylococcus aureus. This study offers a promising strategy for designing multifunctional wearable heaters suited for personal healthcare and thermal management applications.
Organic semiconductor photocatalysts hold promise for solar-driven hydrogen evolution, yet their efficiency is often constrained by weak intermolecular interactions, limited light-harvesting ability, and inefficient charge transport. Addressing these challenges requires precise structural modulation of donor–acceptor assemblies to establish robust electronic coupling and broaden absorption profiles. In this study, a molecular engineering strategy is introduced that simultaneously tailors the donor side chains and tunes the size of the fullerene acceptor cage, thereby promoting electron transport and enhancing light absorption, which ultimately leads to improve photocatalytic activity. Three fullerene-indacenodithiophene (IDT) derivatives—SA-C60-DTIDTT (SA-C1), SA-C60-IDTT (SA-C2), and SA-C70-IDTT (SA-C3)—are synthesized and assembled into supramolecular architectures through a liquid–liquid interfacial deposition method. Replacing the thiophene ring in the donor side chain with a benzene ring strengthens π–π stacking interactions, resulting in more efficient charge transport pathways. Incorporation of C70, with its extended π-system, further facilitates electron delocalization and broadens visible-light absorption. As a result, the SA-C70-IDTT photocatalyst achieves a hydrogen evolution rate of 17.16 mmol g−1 h−1. This study highlights the effectiveness of donor–acceptor structural modulation for constructing high-performance, solar-driven hydrogen evolution photocatalysts.
The pursuit of highly efficient energy storage technique represents the key drive for the global energy structure transformation towards future renewable society. The state-of-the-art Li/Na-ion secondary battery that relies on the intercalation reaction is now well-established as the primary technology by the virtue of high energy and power density as well as the environmental benign. Despite the advantage, tremendous effects have been made for the improvement of the electrochemical performance of Li/Na-ion battery to mitigate the huddle between existing technology and increasing application demand. One of the major challenges lies in the further improvement of the energy efficiency, which is closely related to the voltage hysteresis behavior. The existence of voltage hysteresis could reduce energy output efficiency and accelerates capacity fading thus hindering the practical applications. Due to the voltage hysteresis between charging and discharging, it may induce the part of the energy lost, which decreases the energy conversion efficiency, increases polarization at high rates, intensifies side reactions at high potentials, and reduces the cycle life. At the same time, it also leads to the dendrite growth, promotes gas generation, and increases the risk of thermal runaway. In this review, we systematical outline the previous research on the topic which would contribute to the fundamental understanding of the origination and mechanism of voltage hysteresis. Critical assessments of battery behavior upon cycling are presented in combination with summaries of multiple modification strategies to mitigate the hysteresis in both Li/Na-ion battery. The remaining problems and future prospectives are also proposed which are expected to facilitate for the rational design of advanced electrode materials. This, in our point of view, could inspire the novel insight into future battery development towards practical application as well.
V-based materials, with the high specific capacity and multi-electron redox reactions, are considered as preferred cathodes for low-cost and high-safety aqueous zinc-ion batteries. Nevertheless, poor electronic conductivity, sluggish kinetics, vanadium dissolution, and unstable structure pose severe challenges for the further practical applications. To address these issues, in this study, transition metal ions Mo6+ and polyaniline were incorporated into V2O5 derived from vanadium acetylacetonate via a one-step hydrothermal method (MPVO). The results reveal that MPVO exhibits a unique three-dimensional (3D) sea urchin-like morphology with a satisfactory specific surface area and high concentration of oxygen vacancies. These characteristics offer more reaction sites for Zn2+ and adjust the electronic conductivity. Moreover, kinetic analysis and density-functional-theory calculations indicate that MPVO performs metallic behavior, with the lowest Zn2+ diffusion barrier and outstanding pseudocapacitive storage capacity. Hence, the MPVO cathode delivers a reversible capacity of approximately 457.5 mAh g−1 at 0.1 A g−1. Moreover, it demonstrates remarkable high-rate capacity and robust long-cycle performance. This study realizes a triple-strategy approach of enlarging the interlayer spacing, evolving from a zero-dimensional (0D) to 3D sea urchin-like morphology, and introducing abundant defects. These synergistic strategies significantly enhance the rapid kinetics and high stability of the MPVO cathode and provide new insights for designing V-based cathodes.
The porous carbon-coated Ni0.5Zn0.5Fe2O4 ferrite embedded within Ti3C2Tx MXene interlayers was successfully synthesized via solvothermal and electrostatic self-assembly, followed by carbonization. The resulting Ni0.5Zn0.5Fe2O4@C/Ti3C2Tx composites exhibit superior electromagnetic wave absorption properties, achieving a minimum reflection loss of −63.25 dB at 17.32 GHz with a coating thickness of only 1.53 mm. Notably, heat treatment at 800°C induces the formation of an open interlayer porous microstructure and abundant heterogeneous interfaces, which effectively suppress nanoparticle agglomeration, enhance interfacial polarization, and optimize impedance matching. This study demonstrates a novel strategy to integrate MOF-derived ferrite with MXene for constructing hierarchical porous structures, offering new insights into the rational design of lightweight, high-performance microwave absorbing materials.
Lithium-ion batteries are widely used in various fields, including electric vehicles and energy storage systems. Accurate battery life prediction is essential for effective safety management. However, acquiring sufficient aging information from limited cycle data for accurate life prediction often results in increased feature dimensionality and model complexity. To solve this problem, this paper proposes a method to achieve lossless information dimensionality reduction through the deep variational autoencoder. Based on the lithium iron phosphate battery dataset, only a limited number of cycles are utilized. A comprehensive feature set with 1519 features is constructed to capture more detailed aging characteristics from limited data. After correlation analysis, 76 high-quality features are preliminarily screened. To balance the preservation of aging information with the complexity of the subsequent network, we propose a dimensionality reduction approach that minimizes feature redundancy while retaining essential information. This method reduces the feature set to 10 key features while preserving the original aging information with minimal loss. The maximum mean square error before and after dimension reduction is 0.02139. The proposed method enables life prediction only with the support of simple machine learning method, with only a few parameters required. The adopted dimensionality reduction method offers useful guidance for high-dimensional feature processing in similar scenarios.
The utilization of coal resources is critically important in the modern era, and advancements in coal chemical technology are key to maximizing their value. Integrating modern coal chemical technology with the promotion of low-carbon products is essential for achieving efficient coal resource utilization while supporting sustainable economic development. However, several challenges remain, including low conversion rates, high pollutant emissions, and insufficient residue reuse. Although researchers have made significant progress in addressing these issues, further in-depth studies are needed to improve conversion efficiency, enhance gas recovery, and optimize secondary utilization of residues to ensure more sustainable development. The study systematically reviews advancements in traditional coal chemical technology and elaborates on the progress and advantages of modern coal chemical processes. Additionally, it highlights the pivotal role of carbon capture, utilization, and storage (CCUS) technologies in reshaping the energy structure. Furthermore, the reuse of coal chemical residues represents a crucial step forward in refining coal chemical technology. By addressing these aspects, this work serves as a reference for promoting cleaner and more efficient coal resource utilization.
High-performance and temperature-resistant lithium metal batteries (LMBs) can operate at extremely high temperatures (i.e., > 150°C), and there is a high demand for them in high-temperature scenarios or in special fields such as military application. However, due to the unstable organic solvents, traditional liquid electrolytes usually undergo severe degradation and pose serious safety risks at elevated temperatures (i.e., > 60°C). Herein, functional Li7La3Zr2Ta0.5O12@methoxy polyethylene glycol (LLZT@mPEG) is synthesized via a novel and effective method known as in situ coupled macromolecular bridge, and corresponding all-solid-state composite polymer electrolyte (LLZT@mPEG-CPE) is further prepared. Rigid LLZT cores and flexible ionic conductive polymer side-chains are closely combined by electrostatic interaction, thus resolving the challenge of interface compatibility between different phases. The introduction of mPEG-COOH can further improve the dispersibility of LLZT@mPEG, enhance the stability of electrolyte/electrode interface, effectively inhibit the continuous decomposition of the polymer, enabling LMBs with high thermal tolerance and fast-cycling ability. As a consequence, our LLZT@mPEG-CPE shows great thermal stability and outstanding electrochemical performance. Remarkably, Li|LLZT@mPEG-CPE|LFP cell delivers superior temperature-resistance with a capacity retention of 94% after 500 cycles at high rate of 5 C and extreme temperature as high as 160°C. This study provides an innovative design principle for advanced all-solid-state CPEs of LMBs capable of extremely high temperature operation.
The practical application of lithium−sulfur (Li−S) batteries is hindered by the shuttle effect of soluble lithium polysulfides and sluggish sulfur redox kinetics, resulting in rapid capacity fading and limited cycle life. Here, we present a rationally engineered yolk–shell nanoreactor architecture that integrates dual confinement and catalytic functionality to address these challenges. The nanoreactor comprises a polar, catalytically active core encapsulated within a conductive nitrogen-doped carbon shell, offering synergistic physical restriction of polysulfides and accelerated multistep sulfur conversion. Density functional theory calculations reveal uniformly low-energy barriers along the Li2S8-to-Li2S pathway, with no evident rate-limiting step. Benefiting from this cooperative design, the sulfur host achieves a ultralow capacity decay (0.028% per cycle over 1000 cycles at 2 C) and enables a high areal capacity (493 mAh g−1 at 4.3 mg cm−2 sulfur loading) with 76.3% retention after 100 cycles at 0.3 C. This work offers a versatile strategy for constructing catalysis-integrated sulfur hosts and highlights the potential of yolk–shell nanoreactors in advancing practical Li−S energy storage systems.
The environmental issues caused by carbon dioxide (CO2), a major greenhouse gas, have garnered increasing attention, driving the widespread application of electrocatalytic CO2 reduction reactions (eCO2RR) in pollutant treatment. Metal-CO2 batteries (MCBs) have emerged as a promising alternative to conventional fuel cells, garnering significant interest due to their capacity to integrate energy storage with eCO2RR. The electrolyte is of pivotal significance in MCBs, given its considerable impact on battery performance, service life, and safety. However, due to the inherent limitations of conventional electrolytes, such as flammability, thermal instability, poor low-temperature performance, side reactions, achieving simultaneous optimization of all required performance parameters remains a formidable scientific challenge. Electrolytes should simultaneously possess high ionic conductivity, substantial CO2 solubility, broad electrochemical stability window, and thermodynamically robust interfaces with the electrode materials to ensure overall system performance and stability. It is fortunate that a range of methodologies have been established for the purpose of modifying electrolytes. In this review, we provide a concise overview of the structural characteristics of conventional MCBs, systematically classify MCBs electrolytes into liquid, solid-state, and semi-solid-state categories, and highlight the unique advantages and challenges. We further explore key optimization strategies like bulk composition tuning and additive engineering to enhance performance and put forward several suggestions for the future development of MCBs electrolytes according to persistent challenges. The findings of this study can provide valuable insights for the development of MCBs.
Chain diamines have gained attention in carbon capture recently for their high CO2 absorption capacity and rate. However, how diamine structure regulates the activation barrier of CO2 absorption remains unclear, and the large number of amine candidates hinders efficient screening of low-energy absorbents. To resolve these issues, this study first used DFT to investigate the regulation mechanism of diamines on CO2 absorption and clarify key reaction pathways and structure-activity relationships. It was confirmed that diamines react with CO2 via a zwitterion mechanism, while diamine/tertiary amine mixtures react with CO2 through single-step proton transfer. Diamines with more primary amine sites have lower barriers; methyl/ethyl substitution, carbon chain extension (on either amine), or hydroxyl substitution (on diamines) increases the proton transfer barrier. To address low screening efficiency from excessive candidates, an efficient framework integrating DFT and active learning was constructed. Using DFT-calculated reaction barriers, a feature mapping with RDKit descriptors was built, and an active learning model was developed via 10 iterative rounds. The model achieved high prediction accuracy (R2 = 0.821) for the rate-determining step's activation barrier. SHAP analysis identified the steric-related first-order molecular connectivity index (T_Chi1v) as the dominant feature. Finally, the optimal amine pair (AEEA + EDMA, activation barrier: 0.8 kcal·mol−1) was identified. This work clarifies the core mechanism via DFT, enables efficient candidate screening via active learning, and explains the optimal combination's performance through mechanistic tracing—providing an interpretable route for developing low-energy, high-efficiency mixed amine absorbents and advancing carbon capture technology.
Understanding and chemically tailoring the interfacial properties is essential for improving both efficiency and stability of perovskite solar cells (PSCs). All-inorganic cesium-based perovskites have emerged as promising candidates for thermally stable PSCs, however, their poor phase stability and high density of surface defects continue to impede device performance. Herein, we introduce functionalized halogenated phenethylammonium iodide (X-PEAI, X = H, F, Cl, Br) as modifiers, and a synergistic optimization of the perovskite bulk and interface is achieved through an integrated regulation strategy. It is found that Cl-PEAI with a strong dipole moment, achieves the optimal regulatory effect. It not only improves the film morphology but also effectively passivates the defect states through strong Lewis acid-base interactions. In addition, it also introduces an additional dipole layer at the interface, which enhances the carrier transport effect. Consequently, Cl-PEAI-treated devices deliver a champion power conversion efficiency (PCE) of 19.53% and retain 92.9% of their initial efficiency after 720 h of ambient storage, thereby underscoring the potential of rational ligand design within this specific ammonium salt category for advancing stable, high-performance all-inorganic PSCs.
Metal-organic frameworks (MOFs) exhibit significant potential for the adsorption of volatile organic compounds (VOCs) due to their tunable pore structures and high specific surface areas. However, identifying high-performing MOFs within the vast structural space remains challenging, primarily due to unclear structure–performance relationships. Moreover, existing studies often overlook realistic adsorption scenarios that involve coexisting atmospheric components such as O2, N2, and water vapor, and rarely address capacity–selectivity trade-offs or conducted systematic comparisons of model performance. Herein, we developed a data-driven machine learning framework integrating multi-model comparisons, stacking ensemble modeling, and interpretability analyses for predicting the adsorption performance of MOFs for airborne toluene with high accuracy. The stacking model, comprising eight complementary base models and a multilayer perceptron (MLP) as the meta-learner, demonstrated an enhanced capability to capture complex nonlinear relationships between descriptors and performance, achieving superior predictive accuracy (R2 = 0.922, RMSE = 0.186) compared to the best-performing individual model, CatBoost (R2 = 0.890, RMSE = 0.326). Furthermore, by incorporating SHAP, PDP, and feature interaction analyses, this study elucidated the synergistic regulatory mechanisms associated with key structural descriptors. Statistical analysis further revealed that the structural parameters of high-performing MOFs exhibited significant convergence, with metal centers such as Cu and their open metal sites (OMS) quantitatively identified as critical performance-enhancing factors. Finally, the stacking model was successfully deployed as an interactive web platform that enables real-time prediction and visual interpretability of MOF performance, serving as a practical tool for the efficient screening of MOF candidates for airborne toluene adsorption.
Electrochemical exfoliation (ECE) and dispersion technologies, as typical top-down electrochemical methods, exhibit outstanding advantages of being green, efficient, controllable, and scalable in the preparation of functional nanomaterials. ECE leverages an “intercalation–exfoliation” mechanism for the efficient and controllable production of few-/single-layer two-dimensional (2D) materials for energy storage. Electrochemical dispersion (ECD) is an efficient one-step method to prepare metal-based electrode nanomaterials, utilizing synergistic anodic oxidation and electric double-layer effects to transform bulk raw materials into functionalized nanomaterials with better dispersibility. This review systematically analyzes the electrochemical formation mechanisms of these two ways for synthesizing electrode materials under both direct current (DC) and alternating current (AC) power supplies. It centers on the mechanistic principles of two key approaches: the use of ECE to control the structure and properties of 2D layered electrodes, and the application of ECD to synthesize and optimize functionalized metal-based materials for energy storage devices. As promising electrochemical strategies for nanomaterial synthesis, ECE and ECD offer considerable promise for constructing and tailoring the properties of advanced energy storage electrodes.
Iron-chromium redox flow batteries (ICRFBs) are promising for large-scale energy storage but suffer from sluggish Cr3+/Cr2+ redox kinetics and severe hydrogen evolution reaction (HER) at the anode. To address these issues, a bougainvillea-like indium-doped BiOCl nanosheet architecture on carbon cloth (C-In/BiOCl-CC) was developed as a high-performance electrode. The unique hierarchical structure was found to significantly increase the specific surface area and active sites, thereby facilitating efficient Cr ion conversion. Simultaneously, indium doping effectively suppresses HER by elevating the hydrogen evolution overpotential, while the synergistic effect between In and BiOCl enhances electronic conductivity and reduces charge transfer resistance. As a result, the electrode demonstrates a low Cr3+ reduction overpotential of 0.35 V at 140 mA cm-2 and a charge transfer resistance of 0.492 Ω. The assembled ICRFB achieves an energy efficiency of 84.7% and a voltage efficiency of 86.5% at 140 mA cm-2, while maintaining stable performance over 800 cycles with coulombic efficiency exceeding 97%. This work offers an effective electrode design strategy for high-performance and long-life ICRFBs.
Lithium-metal anodes offer exceptional theoretical capacity and the lowest electrochemical potential, but their practical use is limited by dendrite growth, unstable SEI formation, and large volume fluctuations. Carbon nanofibers (CNFs), with their low weight, high conductivity, and tunable structures, serve as effective hosts for regulating lithium deposition. Heteroatom doping further enhances lithiophilicity and interfacial stability: nitrogen creates abundant nucleation sites, oxygen and sulfur increase surface polarity and strengthen the SEI, and fluorine facilitates LiF-rich interphases for dendrite-free growth. Multi-element doping can also provide synergistic improvements in Coulombic efficiency and cycling stability. Despite these advances, challenges remain, including electrolyte consumption in high-surface-area structures, nonuniform dopant distribution, and potential degradation of CNF properties at high doping levels. This article summarizes recent progress in heteroatom-doped CNFs for lithium-metal anodes and outlines key limitations and future directions toward scalable, high-performance lithium-metal batteries.
The accumulation of persistent organic pollutants (POPs) in aquatic systems poses severe environmental and health risks, underscoring the need for sustainable, efficient remediation technologies. Biomass-derived carbon materials have emerged as cost-effective photocatalysts owing to their high surface area, tunable electronic structure, and excellent charge transport properties. This review summarizes recent progress in their synthesis, structural design, and surface modification for photocatalytic degradation of organic pollutants. Emphasis is placed on key mechanisms such as reactive oxygen species (ROS) generation, band gap tuning, and interfacial charge separation, as well as performance-enhancing strategies including heteroatom doping, heterojunction formation, and hybrid integration for improved visible-light activity. The dual functionality of these materials in adsorption and photocatalysis is also highlighted, revealing synergistic pollutant removal pathways. Finally, critical challenges related to scalability, stability, and reproducibility are discussed, along with future perspectives for translating biomass-derived carbon photocatalysts from laboratory research to practical environmental applications.
Heterostructures show great potential on highly efficient electrocatalysts for oxygen evolution reaction (OER) owing to optimization of electronic structure, synergies, exposure to multiple active sites. In present work, we establish a spherical nanoflower-structured nickel-iron carbonate hydroxides/silicate hydroxides (denoted as NiFeCH/SH) with crystalline/amorphous heterostructure by a facile hydrothermal synthesis strategy. Characterization analysis confirms the controlled partial phase conversion without structural collapse, which is based on the Ni-Fe bi-metallic effect. The heterostructures under bimetallic effect provides the optimized catalyst with good electrical conductivity and abundant active sites, which makes it achieve exceptional OER performance with an ultralow overpotential of 251 mV at 10 mA cm−2 and a small Tafel slope of 31.8 mV dec−1, alongside outstanding long-term stability. The enhanced stability is originated from the protection of silicate. Density functional theory (DFT) methods reveal that the enhanced activity stems from moderate electronic structure caused by suppressing electron transition to eg orbitals of metal active sites. This work establishes a dual-regulation strategy integrating tetrahedral silicate engineering and bimetallic cooperation to simultaneously enhance OER activity and durability, offering new perspectives for designing robust alkaline water electrolysis catalysts through electronic and defect structure manipulation.
Efficient catalysis of unsaturated hydrocarbon hydrogenation/isomerization reactions is important for realizing sustainable chemical processes and enhancing the whole energy efficiency. However, the development of “one-pot” catalysts with high activity, excellent selectivity and outstanding stability remains a major challenge. This study presents a novel catalyst design that utilizes NU-1000 with open metal sites to enhance metal-molecule interactions and promote selective adsorption. By using a strategic multimetal doping technique Ti/Zr/Hf, homomeric high-density frustrated Lewis pairs (FLPs) architecture with different coordination metals namely M-NU-1000-X (M=Zr, Hf, Ti, X = 1~6 represented various metal combinations) were obtained. The strategic multimetal doping finely tune FLPs’ acidity/basicity and electron structure favorable for improve acid-base synergism effect and steric hindrance effect. DFT calculations reveal a mechanism that generated active hydrogen through cleaving H2 at the FLPs site then attack cycloolefin double bond selectively. The hydrogenation/isomerization mechanism was promoted greatly by catalysis effect induced by metals-based π anti-donation effect. Furthermore, we constructed a robust connection model between the calculated Gibbs free energy values of the transition state and some parameter and obtained activation energy barriers based on the descriptor model, thus significantly decreasing huge computational cost. Dynamic Time Warping (DTW) analysis reveals that the dynamic response of polarizability and LUMO energy levels is a key factor determining catalytic activity. The introduction of Ti significantly enhances these dynamic differences, while dynamic site regulation of the local coordination environment further amplifies the differentiation in catalytic performance. A novel approach has been established that integrates electronic structure properties, reaction path evolution, and energy descriptors. This opens a new gateway for developing highly efficient hydrogenation catalysts and provides innovative strategies for catalyst design.
The thermal gradient effect induced by bamboo particle size significantly influences the microstructure and sodium storage performance of derived hard carbon anodes. This study systematically investigates bamboo powders with three distinct particle sizes carbonized at 1400°C. Characterization reveals that medium-sized particles (~52.7 μm) optimize thermal gradients, yielding hard carbon (HCM) with balanced graphite-like domains (interlayer spacing ~0.397 nm) and closed pores. HCM exhibits superior reversible capacity (310 mAh g−1 at 20 mA g−1) and cycling stability (93.4% retention after 100 cycles). In contrast, smaller particles form excessive defects, while larger particles develop heterogeneous structures due to pronounced thermal gradients. Coin full cells (HCM//Prussian blue) demonstrate practical viability with 86.05% capacity retention after 200 cycles. This work elucidates the “particle size-thermal gradient-microstructure-performance” relationship, providing a design strategy for high-performance sodium-ion battery anodes.
Alkaline water electrolysis systems have emerged as a highly promising technology for hydrogen production. Metal-organic frameworks (MOFs) have demonstrated significant potential as electrodes due to their tunable pore structures, high-density active sites, and atomic-level design precision, offering enhanced catalytic activity and long-term stability under high current density conditions (> 500 mA cm−2). This review provides a systematic summary of recent advances in MOF-based materials for high-current-density alkaline water electrolysis. First, the key challenges posed by high current densities, such as mass transport limitations, bubble blockage, and structural deactivation, are discussed. Next, innovative material design strategies are introduced, focusing on critical aspects like tailoring metal active centers, functionalizing organic linkers to optimize the electronic structure, employing dimensional engineering (2D/3D hierarchical porous architectures) to enhance mass transfer, and introducing defect/interface engineering to improve activity and stability. The subsequence section evaluates the performance breakthroughs of MOFs and their derivatives under industrially relevant current densities (≥ 1 A cm−2). Finally, future research directions are highlighted, including enhancing intrinsic conductivity, unraveling dynamic catalytic mechanisms under operating conditions, and developing scalable electrode fabrication methods.
The advancement of low-cost Pt-based intermetallic catalysts is of substantial importance for the effective implementation of high-efficiency zinc–air batteries (ZABs). However, designing efficient catalysts that exhibit both high catalytic activity and stability presents significant challenges. To overcome this issue, we have designed a hybrid catalyst comprising ordered PtM (M = Fe, Co, and Ni) intermetallic nanoparticles uniformly anchored to atomically dispersed M-N-C substrates by integrating a freezing microchemical displacement method with a high-temperature anchoring-reduction strategy. The Pt-NC layer formed during synthesis inhibits Pt nanoparticle migration and aggregation during annealing, which represents a key advantage over traditional methods that often require thick protective coatings. X-ray absorption fine structure analysis reveals that Pt–N bonds form between the nanoparticles and M-N-C support, building strong metal-support interactions through electron transfer and thus significantly enhancing structural stability. Furthermore, theoretical calculations reveal that the structurally ordered PtM intermetallics induce strong electron effects and optimize the d-band center of Pt. The synergistic effects of the ordered PtM electronic structure and its interaction with the M-N-C substrates result in significantly enhanced ORR activity for PtCo@CoNC. This catalyst achieves a mass activity of 1.23 mA/µgPt and a specific activity of 1.14 mA/cm2Pt, outperforming the commercial Pt/C catalyst, which shows values of 0.16 mA/µgPt and 0.22 mA/cm2Pt. When utilized in ZABs, the PtCo@CoNC demonstrates superior performance, yielding a higher open-circuit voltage (1.486 V) and peak power density (179.47 mW cm−2) compared to Pt/C-based devices, highlighting the practical advantages of the ordered PtM@MNC design.
The electrocatalytic CO2 reduction reaction (CO2RR) to formate provides a sustainable pathway for CO2 conversion. Indium oxide (In2O3)-based catalysts have exceptional selectivity toward formate; however, the regulation and effects of crystalline structure on their performance need to be thoroughly investigated. Herein, we present the methodically controlled synthesis of In2O3 catalysts with unique crystallographic structures: rhombohedral In2O3 (h-In2O3), cubic In2O3 (c-In2O3), and mixed-phase In2O3 (h/c-In2O3), and conduct a comprehensive evaluation of their performance in CO2RR to formate. Remarkably, the h-In2O3 catalyst demonstrates a Faradaic efficiency of formate (~95%) and current density surpassing both c-In2O3 and h/c-In2O3. In addition, the h-In2O3 catalyst exhibits excellent comprehensive performance in terms of operating potential range (−0.87 ~ −1.27 V vs. RHE), catalyst stability (70 h), pH range of electrolyte (3.00 ~ 14.00), and CO2 concentration (20% ~ 100%). Density functional theory studies reveal that among various phases and facets of In2O3, the (104) facet of the h-In2O3 most effectively stabilizes the critical reaction intermediate, a contribution that is key to its enhanced activity for formate generation from CO2RR. This investigation elucidates key insights into the engineering crystalline structure of In2O3 catalysts pertinent to CO2RR, thereby presenting a methodical approach for developing highly efficient electrocatalysts.
Hydrogel electrolytes have emerged as promising candidates for flexible zinc-ion batteries (ZIBs) owing to their intrinsic mechanical robustness and biocompatibility. However, realizing high electrochemical performance and long-term operational stability remains a significant challenge, primarily due to the low ionic conductivity of hydrogel matrices and the uncontrolled growth of zinc dendrites, along with parasitic side reactions at the zinc anode interface. In this work, we propose a vertically aligned, zincophilic porous polyacrylamide-based hydrogel electrolyte (o-PAM) featuring strong interfacial adhesion. The unique structure, characterized by a locally alternating gel–liquid phase distribution, effectively overcomes the limitations of conventional hydrogel electrolytes by facilitating rapid Zn2+ transport and ensuring uniform ion deposition. This design bridges the ionic conductivity gap between gels and liquid electrolytes while mitigating Zn2+ concentration gradients. Moreover, the incorporation of multifunctional lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) into the hydrogel not only enhances the electrolyte–anode interfacial adhesion, thereby lowering interfacial resistance, but also contributes to electrochemical stability. The abundant hydrogen bond acceptors in LiTFSI interact with water molecules to form hydrogen bonds, reducing the activity of free water and effectively suppressing side reactions such as hydrogen evolution (HER). As a result, the o-PAM hydrogel electrolyte delivers a high Zn2+ transference number of 0.65 and an impressive ionic conductivity of 20.14 mS cm−1. In Zn||o-PAM||Zn symmetric cells, the electrolyte demonstrates outstanding cycling stability, with a lifespan of 3000 h at 1 mA cm−2. Furthermore, a full Zn||o-PAM||I2 cell exhibits remarkable capacity retention of 95.4% after 500 cycles at 1 mA cm−2. These results highlight a promising strategy for the rational design of high-performance hydrogel electrolytes for next-generation zinc-ion batteries.
Recent studies have indicated that the heterovalent states and vacancy defect structures in bimetallic oxysulfide play a crucial role in pollutant reduction reactions. However, systematic investigations into the synergistic coupling between heterovalent states and vacancy defect structures during the photocatalytic hydrogen evolution reaction (PHER) remain scarce. Herein, a tungsten/oxygen (W/O) co-doped Ag2S bimetallic oxysulfide (AgWOS) with heterovalent W5+/W6+ states and sulfur vacancy (Vs) defects was synthesized via a facile thermohydrolysis method. The combination of W-doping and hydrazine-driven conditions induces abundant Vs defects, which act as active sites for water adsorption and activation, thereby facilitating proton generation in the PHER process. Moreover, the hydrazine-driven condition promotes the formation of heterovalent W5+/W6+ states, which provide efficient electron transfer channels between W5+ and W6+ to boost PHER performance. The optimized AgWOS-2 with a balanced heterovalent n(W5+)/n(W6+) ratio and a high concentration of Vs achieves an impressive PHER rate of 1074.2 µmol·h−1 and an apparent quantum efficiency of 6.21% at 420 nm in pure water. Density functional theory calculations reveal that the synergy between heterovalent states and vacancy defects lowers the water dissociation barrier, accelerates *H generation, and boosts electron transfer between W5+ and W6+. Moreover, S-3p and O-2p orbital hybridization suppresses photocorrosion and improves catalyst stability, enabling AgWOS-2 to retain 91.6% of its initial PHER activity after ten cycles. This study elucidates the synergistic interaction mechanism between heterovalent states and vacancy defects in a bimetallic oxysulfide, offering valuable insights for the rational design of efficient and durable PHER catalysts.
Designing efficient and stable oxygen evolution reaction (OER) electrocatalysts for anion exchange membrane water electrolysis (AEMWE) systems is critical for sustainable energy conversion. Here, we demonstrate a strain engineering strategy through hydrothermal impregnation to anchor W single atoms on MnO2 nanofibers, effectively modulating their electronic structure. The introduced tensile strain weakens the metal-oxygen bond strength, triggering a transition of the OER mechanism from the adsorbate evolution mechanism to the lattice oxygen-mediated mechanism-oxygen vacancy site mechanism (LOM-OVSM). The optimized W2.06%-MnO2 exhibits superior OER performance with an overpotential of 230 mV at 10 mA cm−2. When applied in an AEMWE cell, it requires 1.77 V to drive 1 A cm−2 and demonstrates continuous operation for over 450 h. This study provides fundamental insights into strain-induced modulation of reaction pathways and offers a practical strategy for designing advanced electrocatalysts toward scalable green hydrogen production.
Overcoming the sluggish acidic oxygen evolution reaction (OER) is critical for advancing proton exchange membrane water electrolysis (PEMWE) toward large-scale green hydrogen production, yet its development is hindered by the intrinsic trade-off between activity and stability. Herein, we introduce a controllable synthesis strategy to engineer RuO2 assemblies from ultrasmall Ru nanocrystals supported on carbon via air annealing for efficient acidic OER. This process concurrently induces a Ru-to-RuO2 crystal transformation and facilitates carbon thermal decomposition, yielding a catalyst (Ru-nano/C-300) with markedly enhanced electrochemically active surface area (ECSA) and superior OER performance, requiring only 218 mV at 10 mA cm−2, and exhibiting a Tafel slope of 43.8 mV dec−1 and a mass activity 21-fold higher than commercial RuO2 (c-RuO2) at 1.5 V vs. reversible hydrogen electrode (RHE). Tetramethylammonium cation (TMA+) poisoning experiments combined with in-situ spectroscopic analyses verify that the catalysts predominantly operate via the adsorbate evolution mechanism (AEM) pathway, while electron paramagnetic resonance (EPR) results indicate that suppressing oxygen vacancy formation is crucial for the reaction mechanism. These results demonstrate vacancy suppression coupled with morphology engineering as a powerful strategy to develop both efficient and durable catalysts for acidic OER.
Graphene–based porous two-dimensional (2D) materials are pivotal for advanced health, yet their translation faces three intertwined bottlenecks: scalable synthesis, quantifiable biological risks, and cradle-to-grave sustainability. Emerging paradigms now focus on developing green, surface–engineered porous nanomaterials that simultaneously display high biocompatibility, minimal cytotoxicity, and potent anticoagulant activity, enabling seamless deployment across in vitro diagnostics, targeted drug delivery, antimicrobial coatings, photothermal and gene therapies, and multimodal bioimaging. For the first time in a decade of numerous reviews on graphene's biomedical applications, this review focuses specifically on porous graphene two-dimensional materials. It systematically addresses three intertwined challenges and their solutions: controllable synthesis, biological risks, and full-lifecycle sustainability. We specifically highlight state-of-the-art functionalization strategies for porous nanomaterial preparation (e.g., mechanical exfoliation, chemical vapor deposition, oxidation–reduction, liquid-phase exfoliation, electrochemical exfoliation and SiC epitaxial growth method), alongside their potential risks to the human body, particularly interface mechanism with cell membranes, deoxyribonucleic acid (DNA), proteins, enzymes, cells, tissues, and organs. Current limitations and future research directions are critically discussed, emphasizing the role as a sustainable porous 2D nanomaterial platform. Beyond addressing healthcare challenges, high–performing graphene–based 2D nanomaterials unlock transformative opportunities for next-generation technologies.
Lithium–sulfur (Li–S) batteries exhibit notable advantages, such as lower cost, due to the abundance and affordability of sulfur, coupled with superior gravimetric and volumetric energy densities, ample sulfur reserves, and a reduced environmental footprint. These compelling attributes render Li–S batteries a highly promising energy storage technology, attracting significant global interest. However, their practical deployment is hindered by critical challenges at the cathode–electrolyte interface, including structural degradation (such as heterogeneous Li2S deposition), unstable interphase layers, and the detrimental lithium polysulfides shuttle effect. Addressing these issues requires concerted efforts to optimize both the electrode and interface to improve overall battery performance. This review systematically delineates these interfacial challenges and discusses corresponding mitigation strategies, with emphasis on electrolyte design to form stable cathode–electrolyte interphases, control Li2S deposition behavior, and suppress the shuttle effect through modulation of solid–liquid–solid reaction pathways, their transition to solid–solid conversion routes, and the optimization of solid–solid pathways themselves. Finally, the article offers key perspectives aimed at advancing the fundamental understanding of interfacial phenomena and designing stable battery configurations, with the ultimate goal of stimulating further research and accelerating the commercialization of Li–S batteries.
Aqueous zinc-ion batteries (AZIBs) have garnered considerable attention due to their superior safety, affordability, and eco-friendliness. However, the uncontrolled growth of zinc dendrites and the parasitic hydrogen evolution reaction (HER) severely limit their cycling stability and practical lifespan. In this study, sodium p-aminobenzenesulfonate (SABS) is introduced into ZnSO4-based electrolytes as a functional additive. SABS not only reconstructs the Zn2+ solvation sheath but also forms stable complexes with Zn2+, facilitating the in-situ formation of a robust three-dimensional networked solid electrolyte interphase (SEI) on the zinc anode surface. As a result, Zn||Zn symmetric cells exhibit ultra-stable cycling performance exceeding 2000 h at 1 mA cm−2, while Zn||Cu asymmetric cells maintain over 2000 cycles at 5 mA cm−2 with high Coulombic efficiency. The underlying mechanism of interfacial stabilization and SEI-like interphase formation is further elucidated by combining ex situ structural/chemical characterizations with density functional theory (DFT) calculations. Moreover, the Zn||I2@AC full cell containing SABS additives exhibits excellent specific capacity and long-term cycling performance over a wide range of current densities. This work provides a promising electrolyte additive strategy to enhance the interfacial stability and electrochemical performance of AZIBs through coordinated solvation and interphase regulation.
The development of electrocatalysts with excellent water splitting and 5-hydroxymethylfural oxidation reaction (HMFOR) performance can relieve energy challenges and environmental issues. This study constructs a self-supported CeO2-Ni3N/NF composite on nickel foam (NF) through an elemental modification strategy, developing an electrocatalyst with outstanding electrochemical water splitting and HMFOR performance. The modified CeO2 introduces oxygen vacancy defects in Ni3N and optimizes its electronic structure. The reaction mechanism of HMFOR was explored using in situ characterizations, revealing that CeO2 not only promotes the complete reconstruction of Ni3N into active NiOOH species but also enhances charge transfer of the HMFOR process. CeO2 modulates the adsorption of reactant on the Ni active sites, thereby mitigating the reduction in reaction activity caused by competitive adsorption. Additionally, CeO2 reduces the activation energy needed for the intermediate step from *FFCA to *FDCA. By substituting the anodic reaction with HMFOR, the voltage for water splitting can be reduced, while simultaneously generating valuable organic compounds during hydrogen evolution. Specifically, utilizing HMFOR to replace the traditional anodic reaction in water electrolysis only needs 1.43 V to realize 50 mA cm−2, with a Faradaic efficiency (FE) for cathodic hydrogen evolution approaching 100%, a superior HMF conversion rate (93.6%), and FDCA yield (93.4%). This research provides significant insights for designing transition metal-based catalysts with excellent electrolytic water and HMFOR performance.