Aqueous zinc-ion batteries (ZIBs) hold great promise for energy storage applications. Nevertheless, the realization of high-capacity ZIBs with extended cycle durability remains a significant scientific challenge, predominantly attributed to two inherent limitations: the uncontrollable dendritic growth and concomitant side reactions. In this study, we present a polymer electrolyte membrane denoted as TAC, which addresses these challenges by enhancing the uniform distribution of zinc ions. By incorporating phenolic hydroxyl groups from tannic acid (TA) onto the surface of cellulose fibers, TAC is synthesized, which not only effectively shields both the front and back surfaces of the zinc anode from corrosive effects of the liquid electrolyte, but also exhibits a high liquid-retention capacity under pressures up to 5 MPa. Combining density functional theory simulations with experimental investigations, we demonstrate that the phenolic hydroxyl groups from TA actively engage with zinc ions, thereby significantly reducing the desolvation energy during the plating/stripping processes of the zinc anode. The assembled battery utilizing 1% TAC achieves remarkable performance, retaining 83.1% of its discharge capacity after 1,000 cycles at a current density of 5 C. Moreover, it exhibits high reversibility, high coulombic efficiency of 99.9%, and an impressive lifespan exceeding 2,300 h at 0.5 mA cm-2. Furthermore, 1% TAC demonstrates excellent cycling stability across four different electrolyte systems [ZnSO4, Zn(CF3SO3)2, Zn(OAc)2, and ZnCl2], highlighting its outstanding compatibility across diverse electrolyte compositions. The exceptional performance of the assembled batteries underscores the efficacy of our design, offering a novel strategy for the development and fabrication of polymer electrolyte membranes tailored for aqueous ZIBs.
The increasing demand for efficient energy storage has led to increased research on sodium-ion batteries (SIBs) as a promising alternative to lithium-ion batteries. However, the anode materials currently employed in lithium-ion batteries are not suitable for SIBs, highlighting the need for the development of appropriate anode materials. In this study, cellulose- and lignin-rich residues extracted from wood biomass were converted to hard carbon, and their performance as anode materials for SIBs was evaluated. Cellulose and lignin were separated from larch wood using a deep eutectic solvent, followed by carbonization to produce CF-1300C and LF-1300C, respectively. Lignin undergoes partial graphitization at elevated temperatures, enhancing its electrical conductivity and forming ion insertion and extraction pathways. LF-1300C demonstrated higher crystallinity than CF-1300C owing to this graphitization and featured an interlayer spacing of approximately 0.43 nm, which facilitates sodium-ion insertion. Consequently, LF-1300C achieved a higher initial discharge capacity and Coulombic efficiency (350 mAh g-1 and 74%, respectively) than CF-1300C (331 mAh g-1 and 71%, respectively). Furthermore, LF-1300C exhibited a 21% and 84% improvement in rate capability and cycle retention, as compared with CF-1300C. These results indicate that hard carbon with a partially graphitized structure exhibits significant potential for use as an anode material in SIBs, especially in cases where existing crystalline materials present challenges. This study highlights the advantages of lignin-derived hard carbon as a superior anode material for SIBs, providing an eco-friendly and scalable solution for energy storage.
Lithium-sulfur (Li-S) batteries stand out due to their high theoretical energy density, natural abundance of sulfur, and cost-effectiveness. Despite these advantages, challenges such as the shuttle effect of lithium polysulfides, electrode degradation, and safety concerns hinder their commercialization. Recent advances have focused on integrating molybdenum-based nitrides and carbides to address these issues. These materials offer advantages such as tunable compositions, adjustable lattice structures, semi-metallic conductivity, and enhanced catalytic activity and electron transport. In this mini-review, we delve into the unique physicochemical properties of molybdenum-based nitrides and carbides and the associated composites and their roles in improving the properties of Li-S batteries and discuss their applications as sulfur cathodes and interlayers, mechanisms of lithium polysulfides adsorption, and effects on reaction kinetics. This review aims to consolidate existing knowledge, identify research gaps, and inspire future advancements in Li-S battery technology, paving the way for high-performance, sustainable energy storage solutions.
Hydrogel-based ionic thermoelectric (i-TE) materials that rely on ion migration driven by thermal gradients have emerged as promising candidates for efficient low-grade heat harvesting. They offer high Seebeck coefficients, mechanical flexibility, and biocompatibility, making them especially attractive for wearable electronics and biomedical applications. Among various i-TE materials, hydrogels are particularly notable due to their unique structure and ability to modulate ion diffusion via interactions between the polymer network and ionic species. Despite increasing interest in hydrogel-based i-TE materials, the fundamental mechanisms governing thermodiffusive ion transport remain poorly understood, especially when compared to the more established thermo-galvanic processes. Moreover, the unique composite architecture of these materials combining polymer matrices with diverse ionic components presents significant challenges for rational design and performance optimization. This review addresses these challenges by systematically analyzing the fundamental mechanisms of hydrogel-based i-TE materials, with a particular focus on the Soret effect and the roles of polymer networks and ionic conductors. It also provides critical insights into practical applications such as wearable thermoelectric generators and capacitive energy storage devices. Furthermore, we propose innovative strategies to overcome key limitations, those related to long-term stability and mechanical durability. By consolidating current knowledge and identifying future research opportunities, this review establishes a foundation for the development of next-generation flexible and efficient hydrogel-based i-TE materials.
Enhancing the catalytic activity of sulfur cathode hosts is critical for suppressing the shuttle effect and accelerating the polysulfides redox kinetics in lithium-sulfur (Li-S) batteries. However, efficient polysulfide adsorption and catalysis conversion rely on synergistic interactions between the catalyst and the supporting carrier, particularly in optimizing catalytic site density and electron/ion transport rates. Herein, we modulate the carrier-catalyst heterointerface to enhance polysulfide conversion. Metallic 1T-phase MoS2 nanospheres are uniformly dispersed onto the nitrogen-doped graphene (N-G) sheets, forming a composite host material (1T-MoS2/N-G) for Li-S batteries. N-G serves as both a conductive substrate for charge transfer and a support for catalyst loading, while 1T-MoS2, rich in catalytic sites, functions as an efficient electrocatalyst, promoting ion diffusion, adsorbing soluble polysulfides, and accelerating their transformation into solid lithium sulfide. Benefiting from these structural and catalytic advantages, the S/1T-MoS2/N-G cathode exhibits an initial capacity of 1,296.8 mAh g-1 at 0.2 C and demonstrates outstanding cycle stabilization, with a capacity decay rate of only 0.015% per cycle over 500 cycles at 1.0 C. Even under demanding conditions, such as a sulfur loading of 6.5 mg cm-2 and a lean electrolyte of
Protonic solid oxide fuel cells (P-SOFCs), as a promising power generation technology, have garnered increasing attention due to their advantages of cleanliness, high efficiency, and high reliability. As a critical component of
We investigated the anisotropic thermoelectric properties of Bi0.4Sb1.6Te3 (BST) composites with heavy metallic high-entropy alloy TaNb2HfZrTi (HEAx) (x = 0, 0.1, 0.5, and 1.0 vol%), synthesized by ball-milling, mixing, and
In the continued evolution toward high-performance lithium (Li)-ion batteries, cobalt (Co) has presented itself as a major obstacle due to its price, toxicity and supply. Thus, Co-free, Li-rich layered oxide cathodes (CF-LLC) have garnered interest for their exclusion of cobalt and high theoretical capacity. Nevertheless, CF-LLC suffers from issues such as sluggish kinetics, voltage fade and low early capacity due to the increase in cation mixing resulting from the absence of cation-ordering cobalt. To mitigate this, a sulfate coating was applied to the cathode carbonate precursor prior to lithiation, resulting in the formation of a Li2SO4-coated CF-LLC. The Li2SO4 coating prevents the agglomeration of primary particles during lithiation, thereby reducing the primary particle sizes. As a result, Li diffusion pathways are shortened, enhancing Li diffusivity. The coating also prevents transition metal dissolution by acting as a protective barrier against electrolytic reactions. With the Li2SO4 coating, first cycle capacity increased from 205.1 mAh∙g-1 to 259.0 mAh∙g-1, and first cycle Coulombic efficiency also increased from 76.6% to 83.6%. Moreover, after 100 cycles, the Li2SO4-coated sample showed a good 84.7% capacity retention and an improved average voltage fade per cycle of 2.79 mV.
Altermagnet is an uncommon category of antiferromagnets distinguished by their non-overlapping spin-bands, drawing significant attention from researchers. However, while reports on their electronic and magnetic properties are increasing rapidly, the study on the transport properties is still in early stage. Therefore, we explored the orientational spin-dependent transport features of altermagnet V2S2O using Boltzmann transport technique. This altermagnet had 1.15 eV direct band gap energy and a critical temperature of 746 K. We obtained a directional spin-dependent feature in the band structure whose effect spans through all the spin-dependent transport parameters. We found a low isotropic lattice thermal conductivity of magnitude 0.2 Wm-1K-1 at 300 K. Above all, the V2S2O altermagnet displayed a giant spin-dependent Seebeck coefficient of about 1.8 mVK-1 at 300 K and at a small electron or hole doping. This value is multiple times greater than reported values for most transport materials. Besides, we also found a maximum figure of merit of 0.86 in the hole-doped systems. Thus, our findings suggest the possibility of pure spin current generation for possible applications in spintronics and thermoelectricity.
Leather-based materials have found extensive use in the development of flexible sensing devices, energy harvesting, storage systems, and flexible circuits owing to their high biocompatibility, good breathability, comfort during wear, and robust mechanical properties. However, with the rapid evolution of flexible electronics, traditional fabrication methods for leather-based devices fail to fulfill the demands for high integration and practicality. In this work, an innovative fabrication method combining laser direct writing and inkjet printing technologies has been developed to prepare a self-powered triboelectric sensor array for human-computer interaction applications. This method offers significant advantages, including mask-free fabrication, high resolution, and fast processing. The resulting MXene/graphene/leather (MG/leather) electrode exhibits a narrow width (400 μm), high conductivity (1.46 S mm-1), strong adhesion strength (2.63 MPa), and high tensile strength (7.65 MPa). The MG/leather-based TENG achieves a maximum output voltage of 167.5 V, a current density of 1.1 mA m-2, a transferred charge of
Carbon-based materials, commonly used as commercial anodes in lithium/sodium ion batteries, nevertheless suffer from sluggish kinetic properties. Constructing electrode materials with one-dimensional nanostructures that offer convenient ion/electron transport pathways can improve Li+/Na+ storage behavior. Recently, metal
Highly efficient and stable bifunctional catalysts toward sluggish oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are critical for practical applications of rechargeable zinc-air batteries (ZAB). Heterostructure engineering is effective in boosting catalytic performances of the bifunctional catalysts. Here,
Sodium vanadium fluorophosphate [Na3V2(PO4)2F3, NVPF], as a sodium (Na) super ionic conductor material, has attracted significant interest as a very promising cathode material for sodium-ion batteries due to its structural stability, rapid ion transport capability, and high operating potential. However, the insulating [PO4] units in NVPF isolate the V atoms, which results in low intrinsic electron conductivity and poor overall electrochemical performance, and the high cost also represents critical challenge that has impeded its widespread use. In recent years, the research focus has shifted to an enhancement of scalable fabrication technologies and improvement of operational robustness under extreme conditions. This has meant a realignment of the research paradigm from the modification of single materials to an adaptive design of the entire battery system. This review assesses the research conducted on NVPF cathodes over the past three years from several perspectives, focusing on the feasible application of materials over a wide temperature range at high voltages, summarizing the challenges and required development strategies in future research.
Heterophase anatase/rutile junctions (A/R-HPJs) in TiO2 hold significant promise for photocatalysis, yet precise control over phase composition remains elusive. Here, we develop a novel polyol-solid surface/interface transesterification strategy to synthesize TiO2 A/R-HPJs with tunable mass ratios for photocatalytic seawater splitting and dye degradation. Mechanistic studies reveal that glucose-Ti complexes (GTCs) govern rutile formation, enabling a linear correlation between A/R mass ratios and GTC/Ti molar ratios. Increasing glucose particle surface area via grinding enhances rutile content, evidenced by amplified slope values in this linear relationship. This approach for constructing precise A/R TiO2 HPJs demonstrates generalizability across diverse polyols, non-solubilizing solvents, and titanium precursors. Phase-dependent carrier separation efficacy is highlighted, with optimized GT15 (optimal A/R ratio) exhibiting exceptional photocatalytic H2 evolution and pollutant degradation. Our work establishes a surface/interface engineering paradigm for precise heterophase control in metal oxides, addressing a critical gap in designing functional HPJs for energy and environmental applications.
Anion exchange membrane water electrolysis is one of the key technologies for production of green hydrogen, and developments of highly efficient and durable electrode catalysts in alkaline media are critical for its practical applications. Atomic scale synergy of high entropy materials empowers highly efficient water electrolysis catalysts. Here, Fe, Co, Ni, Cu, and Mo-based high entropy electrode catalysts, including high entropy alloys (FCNCuM) for cathodes and high entropy oxides (FCNCuMOX) for anodes, are developed for high-performance Anion exchange membrane water electrolysis. FCNCuMOX and FCNCuM exhibit outstanding catalytic efficiency toward oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), respectively, achieving ultralow overpotentials of 183 and 294 mV for OER and 38 and 230 mV for HER at 10 and 500 mA cm-2, respectively, in 1 M KOH. The anion exchange membrane water electrolyzer, using FCNCuMOX and FCNCuM as the anode and cathode catalysts, respectively, achieves an ultrahigh specific activity of 293 mA mg-1 and exhibits outstanding durability with decay of only 0.014% after a 100 h operation at 500 mA cm-2. In-situ Raman and in-situ X-ray absorption studies disclose that atomic scale synergy between Fe, Co, and Ni, the three main active centers, is responsible for the extraordinary OER activity, and density functional theory calculations reveal that atomic scale synergy between Mo and Ni leads to the outstanding HER performance.
The growing demand for high-energy storage, rapid power delivery, and excellent safety in contemporary Li-ion rechargeable batteries (LIBs) has driven extensive research into lithium manganese iron phosphates
Aqueous thermocells are promising techniques for the conversion of low-grade waste heat into electricity. However, current improvement strategies are mainly focused on single redox ions and sacrifice the electrical conductivity due to concentrated molecular additives. Herein, we report a chemical additives-regulated thermocell that introduced two ionic additives, guanidine hydrochloride and cysteamine hydrochloride, into 0.4 M ferri/ferrocyanide {[Fe(CN)6]3-/4-} electrolyte to simultaneously exert the selective crystallization effect on [Fe(CN)6]4- and the chemical regulation effect for [Fe(CN)6]3-, synergistically inducing concentration gradients of both redox ions between two electrodes, thereby improving the thermoelectric performance. Our thermocell obtained a high thermopower of 4.34 mV K-1 with comparable electrical conductivity and a Carnot-relative efficiency of 5.50% with minimal amounts of the two additives, showing adaptability to various cell orientations and thus different practical scenarios. A record-high thermopower of 9.06 mV K-1 and a Carnot-relative efficiency of 12.65% were achieved by adopting optimized concentrations of two additives under cold-over-hot orientation. A 20-unit module was developed to directly power various electronics, demonstrating its feasibility for low-grade heat harvesting.
Thermoelectric (TE) materials, capable of directly converting heat to electricity, offer a promising sustainable energy and waste heat recovery solution. Despite extensive research, a significant bottleneck remains: the synthesis of high-performance TE materials still relies heavily on trial-and-error approaches, which are time-consuming and resource-intensive. Moreover, while machine learning (ML) and design of experiments (DOE) have shown potential in optimizing synthesis processes across materials science, their systematic application to TE materials remains underexplored. In particular, very few reviews have addressed the integration of statistical and AI-guided methods for synthesizing and optimizing TE materials. This manuscript comprehensively reviews recent advances in statistical and artificial intelligence techniques for optimizing TE material synthesis. It first discusses the role of DOE in identifying critical synthesis parameters and explores various ML methods for predicting TE performance. This study then highlights case studies involving different TE material systems, synthesis strategies (e.g., ball milling, sputtering, electrodeposition), and ML-based performance prediction and optimization. This work fills a critical gap by linking data-driven optimization techniques with experimental synthesis in the TE field. It not only consolidates current knowledge but also sets the stage for future studies aiming to bridge material discovery and practical manufacturing. The insights presented are instrumental in accelerating the development of next-generation TE devices.
Thermoelectricity has long been recognized as a transformative technology for power generation and cooling, owing to its capability to convert heat directly into electricity and vice versa, thereby facilitating cost-effective and environmentally friendly energy conversion. Following a period of modest activity, the field has experienced a remarkable resurgence since 2000, driven by significant advancements in the development of a diverse array of new materials and compounds, alongside enhanced capabilities for controlled nanostructuring. This rapid growth and the innovative breakthroughs observed over the past two decades can be largely attributed to a deeper understanding of the physical properties at the nanoscale. Among the various thermoelectric materials, nanostructured variants exhibit the highest potential for commercial application due to their unprecedented thermoelectric performance, which arises from substantial reductions in thermal conductivity. However, further advancements will not rely solely on nanostructuring; they will also necessitate novel electronic structure design concepts that require a comprehensive understanding of the complexities of electronic and phonon transport. These developments present significant opportunities for thermoelectric energy harvesting, power generation, and cooling applications. This article aims to summarize and elucidate the breakthroughs reported in recent years, discuss future avenues that integrate nanostructuring concepts with the rich electronic structures of novel materials, and provide a critical overview of the future directions in thermoelectric materials research. Additionally, it offers a comprehensive overview of state-of-the-art thermoelectric materials and devices and a summary of the challenges associated with transitioning these materials into practical devices.
This work presents, for the first time, a direct comparison of the impact of applying elemental metallic stack precursors and bronze-based precursors to produce Cu2ZnSnSe4 (CZTSe)-based solar cells by sequential fabrication based on physical deposition methods. Scanning electron microscopy, energy-dispersive X-ray spectroscopy, and X-ray diffraction reveal an improved morphology, a higher compositional homogeneity, and a higher presence of binary alloys in the bronze-based precursor. Scanning electron microscopy observation also shows that bronze-based precursors improve the thickness homogeneity and the rear interface morphology of CZTSe absorbers, while Raman spectroscopy detects an improved crystalline quality and an improved structural micro-homogeneity at the absorber surface. The results of this work also demonstrate that germanium doping, which is required when applying elemental metallic stack precursors, can be avoided in the case of bronze-based precursors without compromising the efficiency of the solar cells. Thus, this work sheds light on the mechanisms induced by bronze-based precursors that contribute to producing high-efficiency CZTSe-based devices, so the expanded understanding of this precursor can help to further optimize such devices. Additionally, this work demonstrates that the bronze-based precursor reduces material, energy, and time consumption, which favors its possible scaling up to an industrial level.