Commercial carbonate electrolytes suffer from ion transport difficulty in bulk electrolytes and interphase at low temperatures, bringing challenges to the application of lithium-ion batteries (LIBs) at low temperatures. Herein, the ester solvent of methyl propionate (MP) with low melting point and low viscosity was used to tackle ion transport difficulty in electrolytes. Fluorinated ester was further added to accelerate interfacial transport through intermolecular interactions. The influence of fluorinated esters with different fluorination degrees on the solvation structure of electrolytes and the performance of batteries was further studied. As a result, methyl pentafluoropropionate (M5F) with five fluorine atoms was selected for its optimal interactions with both Li+ and MP solvent in the primary solvation structure, contributing to desired solvation structure for fast interfacial transport. The LiFePO4 (LFP)||graphite cell with LiFSI-MP-M5F electrolyte exhibited a high cyclability of 85.8% after 120 cycles and retained 81.2% of room-temperature capacity when charged and discharged at -30 degrees C. 1 Ah LFP||graphite pouch cell with high cathode loading (20 mg/cm2 ) in LiFSI-MP-M5F electrolyte exhibited 0.85 Ah capacity when charged and discharged at -20 degrees C. This work provides a guidance for electrolyte design by synergistic fluorinated and non-fluorinated solvents for LIBs at low-temperature application. (c) 2025 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.

Inverted-structure Si/Poly (3,4-ethyldioxythiophene)/poly (styrene sulfonate) (PEDOT: PSS) solar cells have superior photovoltaic performance. The blocking of hole carrier transmission caused by energy band mismatch still are pressing issues. In this work, MoS2 quantum dots (QDs) is introduced into PEDOT: PSS to prepare n-Si/PEDOT-MoS2 solar cells. The detailed results show the incorporation of MoS2 QDs can enhance the band energy level and work function of PEDOT: PSS films, and lower the surface valence band energy level, which means the electron blocking ability and hole extraction ability of films are simultaneously enhanced. In addition, the conductivity and uniformity of PEDOT: PSS films are improved. Combined with textured silicon wafer structures, a Si/PEDOT: PSS solar cell with a record efficiency of 18.06% was achieved. Our work evidences that the band engineering based on Mo-based compounds is a valid technical solution for improving the PCE of Si/PEDOT: PSS solar cells.

Atomic-scale solid-gas interface (SGI) dynamics remain elusive due to transient intermediates, complex interfacial environments, and challenges of real-time characterization. Using an environmental transmission electron microscopy cell as a microreaction chamber combined with atomic-resolution in-situ imaging, here we directly visualize SGI reactions at the interface of transition metal oxidate WO2.72 nanowire under reactive gas environments. We reveal that initial SGI interactions trigger surface restructuring into a dual-layer configuration, consisting of an uppermost amorphous layer and an underlying lattice-distorted condensed region. The amorphous surface layer acts as a quasi-liquid precursor reservoir that promotes reversible crystalline-amorphous transformations and short-range ordering for critical nucleus formation, while the roughened, defect-rich subsurface interface provides energetically favorable sites for WS2 nucleation and vertical growth. Furthermore, in-situ atomic-scale observations of MoS2 nucleation and growth via SGI reactions demonstrate the generality of this mechanism. The atomistic processes governing interfacial reconstruction and nucleation are further corroborated by theoretical calculations. Our results establish a dual-layer-mediated reconstruction pathway during SGI reactions, overturning the conventional view of atomically sharp and static reaction fronts. Moreover, these findings provide insights into multistep phase-transition-governed WS2 nucleation and growth, enabling controlled synthesis of 2D WS2 and MoS2 toward atomic-scale manufacturing.

Aqueous zinc-ion batteries (AZIBs) have drawn great attention owing to the high intrinsic safety, high power density and numerous advantages of the zinc metal anode. As a cathode material for AZIBs, vanadium pentoxide has a high theoretical capacity of 589 mA h g-1, but it suffers from sluggish Zn2+ diffusion kinetics and rapid capacity degradation. Herein, a co-intercalation strategy of polyaniline (PANI) and alkali cations (Li+, Na+, and K+) is employed to enhance the Zn2+ storage capability of vanadium oxides. As control groups, the sample with only PANI intercalation and the sample without PANI and alkali cation intercalation are synthesized. The evolution of the phase, interlayer distance, morphology and structure for the five samples is investigated. Compared with the intercalation of only PANI, the co-intercalation of PANI and alkali cations further enlarges the interlayer distance (14.80 Å) and maintains the tremelliform nanosheet structure. This co-intercalation strategy promotes the Zn2+ diffusion kinetics, enhances the stability of the layered structure and improves the electronic conductivity. As a result, the electrochemical performance is significantly improved, showing high capacity (409.2 mA h g-1 at 0.2 A g-1), excellent rate capability (261.8 mA h g-1 at 5 A g-1), and favorable cycling stability (capacity retention of 65.4% after 1200 cycles at 5 A g-1).

Next-generation lithium-ion batteries demand high-voltage cathodes that combine exceptional stability with ultrafast charging capability. Cobalt-free spinel-type oxides, owing to their high operating voltage, energy density, and cost effectiveness, are leading candidates, yet their cycle life is still constrained by intrinsic chemo-electro-mechanical instabilities. Here, by leveraging compositionally complex doping, we reconfigure the reaction thermodynamics of a high-voltage spinel cathode by extending its solid-solution regime to higher states of charge, enabling ultrafast charging while maintaining robust chemo-electro-mechanical stability. Multimodal characterization reveals that the reshaped reaction pathway effectively suppresses high-temperature intragranular cracking, interfacial rock salt phase transformation, and parasitic byproduct accumulation, thereby preserving efficient three-dimensional Li+ diffusion. The cathode delivers unprecedented ultrafast-charging durability, achieving 81.8% after 4000 cycles at 10 C (25 °C) and 82.0% after 1000 cycles at 3 C (60 °C). Our work demonstrates that compositionally complex doping can effectively modulate the thermodynamics of phase transformation and enhance the chemo-electro-mechanical stability of high-voltage spinel cathodes, providing new insights into the design of durable fast-charging cathode materials.

Three new A 2 B-type copper( iii ) corrole complexes were synthesized and their electrocatalytic HER performance was evaluated both in organic and aqueous media.

Elevating the cut-off voltage (>= 4.5 V) of Ni-rich cathodes can maximize the energy density but triggers severe oxidation of carbonate electrolytes and the formation of a fragile cathode-electrolyte interphase (CEI). To address this dilemma, we propose precisely manipulating the interfacial solvation structure via a bifunctional molecule, (trimethylsilyl)acetonitrile (TSAN). Featuring nitrile (-C N) and trimethylsilyl (-TMS) groups, TSAN operates through a synergistic "anchor-steric hindrance" mechanism. The -C N group preferentially participates in the Li' primary solvation sheath and anchors to the cathode surface, while the bulky -TMS group simultaneously repels carbonate solvents via steric hindrance. TSAN induces spatial heterogeneity of the solvation structure in the bulk electrolyte and the cathode interface region, which enriches anions within the primary solvation sheath at the cathode interface. This interfacial solvation structure directs the in-situ formation of a robust, ultra-compact, and inorganic-rich CEI, which is distinct from conventional sacrificial additives. With 5 wt% TSAN, NCM811 parallel to graphite cells demonstrate outstanding high-voltage stability, retaining 81.4% capacity after 600 cycles at 4.5 V. This synergistic functional group regulation of interfacial solvation structure offers a strategy for high-voltage electrolytes of lithium-ion batteries. (c) 2026 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

Sulfur and organosulfur compounds have emerged as promising cathode materials for high-energy lithium batteries owing to their high theoretical capacity, element abundance, and structural tunability. However, either sulfur or organosulfur cathodes are difficult to achieve high capacity, cyclic stability, and redox kinetics at the same time due to the inherent trade-off. Herein, a solid-liquid biphasic organochalcogen cathode is reported to overcome this performance trade-off for next-generation lithium batteries. The in situ cross-linking between an organosulfur polymer and a small-molecule organoselenium compound significantly enhances the charge transfer and ionic diffusion kinetics of the cathode. Furthermore, the small-molecule organoselenium and intermediate products could be immobilized within the cathode by the polar functional groups within organosulfur, resulting in cycling performance that is markedly superior to that of cathodes using inorganic elemental sulfur paired with organoselenium. Benefiting from this complementary effect, the optimized cathode exhibited ultra-long cycle stability with capacity decay of 0.017% per cycle within 2,700 cycles at 2 mA g-1 and achieved a high areal capacity of 11.36 mAh cm-2. This biphasic organochalcogen cathode strategy provides a rational design paradigm for lithium-organic batteries with excellent comprehensive performance.

Batteries based on redox chemistry, such as lithium-sulfur and lithium-oxygen, can store more energy than conventional lithium-ion batteries. However, their chemical reactions are limited by sluggish and incomplete conversion reactions, especially those involving insulating solid intermediates (for example, Li2S2 and Li2O2), in which electrocatalysts play a decisive role. Here, through a large-scale theoretical analysis, we propose an electronic property criterion that emphasizes the efficient conduction of ions and electrons as essential for high catalytic activity. Guided by this insight, we have designed a CoCo dual-atom catalyst that accelerates the conversion of solid insulating Li2S2 and Li2O2 intermediates by effective orbital coupling, making these intermediates conductive and catalytically active. This strategy enables the fabrication of high-energy lithium-sulfur pouch cells at the ampere hour scale, achieving a specific energy of 459 Wh kg-1. Our results extend the fundamental understanding of rate-determining solid-phase reactions in redox chemistry and provide principles for the design of electrocatalysts for use in energy storage systems.

Correction for ‘Unraveling the interfacial compatibility of ultrahigh nickel cathodes and chloride solid electrolyte for stable all-solid-state lithium batteries’ by Feng Li et al. , Energy Environ. Sci. , 2024, 17 , 4187–4195, https://doi.org/10.1039/D4EE01302F.

Lithium sulfur batteries (LSBs) have good potential for next-generation energy storage. However, the practical applications of LSBs are restricted by the shuttle effect of lithium polysulfides (LiPS) and uncontrollable Li deposition. Here, potassium selenocyanate (KSeCN) is proposed as a bifunctional electrolyte additive that can synergistically regulate both the cathode and anode electrode/electrolyte interfaces due to its optimum orbital energy levels. KSeCN promotes the formation of a hybrid organic-inorganic cathode electrolyte interface (CEI) that inhibits the shuttle effect and boosts the conversion kinetics of LiPS by incorporating conductive Se into the cathode. In addition, KSeCN facilitates an inorganic-rich solid electrolyte interface (SEI), promoting homogeneous Li+ deposition and suppressing Li dendrite growth. Correspondingly, LSBs with the KSeCN additive achieve a low capacity decay rate of 0.05% per cycle over 1000 cycles with excellent stability, while Li-S pouch cells operate stably for ∼140 cycles. Li‖Li symmetric cells exhibit a reduced hysteresis voltage and extended cycling lifetimes exceeding 1000 h. This work demonstrates a promising additive design strategy for high-performance LSBs through interfacial chemistry engineering.

Alkaline direct air capture promises scalable CO2 removal but remains constrained by poorly understood interfacial microenvironments. Pfeilsticker et al. report operando Raman mapping in a custom flow cell to visualize carbonate and bicarbonate distributions across the gas-liquid boundary layer, revealing how diffusion-reaction coupling and local alkalinity depletion govern CO2 absorption and guide interface-informed process design.

Lithium-sulfur (Li-S) batteries have garnered increasing attentions due to their ultrahigh energy density. However, their practical applications are significantly impeded by the shuttle effect of polysulfides, the corrosion of lithium anodes, and the formation of lithium dendrites. Here, we design a dual-function cottonseed proteinbased separator coating (Mn-P-CPI) by synchronously grafting phosphate groups and metalloporphyrin compounds, which is capable of adsorbing and catalyzing polysulfides. As such, the assembled Li-S battery not only exhibits much-improved specific capacity (up to 983.5 mAh g- 1 at 1C), but also maintains high cycling stability (the capacity attenuation is only 0.066% per cycle). More notably, Mn-P-CPI can serve as the binder of cathode electrode benefiting from its abundant active groups. By simultaneously employing Mn-P-CPI as electrode binder and separator coating, the battery displays a high specific capacity (752.8 mAh g- 1 at 0.5C) under 2.11 mg cm- 2 of sulfur loading and the exceptional rate performances (719.3 mAh g- 1 at 3C). This strategy offers a promising alternative to develop a high-performance separator coating for Li-S batteries, as well as opens up a feasible way for realizing the application of biomass materials in the field of energy storage.

An anion-enriched solvation structure is crucial for electrolytes in establishing stable electrode-electrolyte interfaces and facilitating rapid Li+ transport kinetics. However, even a well-designed solvation structure can be sensitive to temperature variations, compromising the long-term cycling stability of batteries over wide temperature ranges. Herein, we design an electrolyte with temperature-independent anion-enriched solvation structures, by leveraging the ionic solvation/association equilibrium of Li+ in solvation structures based on the formation entropy (∂ΔG/∂T = -ΔS) counterbalancing of the mixed salts. This strategy effectively stabilizes the anion-enriched solvation structure and ensures the formation of robust inorganic interphases over a wide temperature range. Specifically, the electrolyte enables stable operation of Li||LiNi0.8Mn0.1Co0.1O2 cells from -70 to 80 °C at a high charging voltage of 4.6 V, maintaining long-term cycling stability with no observable capacity decay over 1000 cycles at -20 °C. Further toward practical application, 4.5 V Ah-level Si/C||LiNi0.9Mn0.05Co0.05O2 pouch cells achieve 92% capacity retention after 500 cycles over 250 days of operation at -20 °C. This work underscores the critical importance of understanding solvation structures from a thermodynamic perspective for the rational design of electrolytes, enabling their efficient implementation in batteries and other electrochemical systems.

Developing efficient electrocatalysts for hydrogen evolution reaction (HER) is a hot topic of energy chemistry. In this work, a series of triaryl corrole gallium(III) complexes (1Ga4Ga) bearing an increasing number (0-3) of pentafluorophenyl groups were synthesized and used as HER electrocatalysts to investigate the effect of meso- electron-withdrawing substituents on the electrocatalytic HER activity of Ga(III) corroles. In the organic phase or neutral aqueous medium, the catalysts' HER activity follows 4Ga > 3Ga > 2Ga > 1Ga, showing that electron-withdrawing groups can markedly enhance the electrocatalytic performance of the Ga(III) corroles. 4Ga delivers TOFmax values of 740.32 s(-1) and 1090.95 s(-1) when TFA and TsOH are used as proton sources respectively. In neutral aqueous system, 4Ga also serves as an efficient HER electrocatalyst, affording a Faradaic efficiency of 89.35%. Density functional theory (DFT) calculations further corroborate these findings, and the Gibbs free energy profile indicates that 4Ga has the lowest free energy barrier for HER.

Polymer electrolyte shows great promise for enabling solid-state batteries with intrinsic safety. However, it faces a fundamental challenge in the trade-off between ionic conductivity and robustness, stemming from conflicting requirements for polymeric chain segment mobility. In this work, we design a crosslinked poly(vinyl ethylene carbonate) (PVEC)-based electrolyte, incorporating hydrogen bond contained crosslinker to create a covalent and hydrogen bond dual-crosslinked architecture. The covalent crosslink from C = C group reactions and complementary N-H O hydrogen bond crosslink synergistically restricts polymer chain segment mobility while modulating the Li+ coordination environment, thus enabling exceptional robustness without sacrificing ionic transport. The optimized electrolyte simultaneously achieves high ionic conductivity (2.1 x 10-4S cm-1 at 25 degrees C) and enhanced Young's modulus (2.51 MPa). When implemented in LiFePO4||Li cells, the cell delivers a high capacity of 150.2 mAh g-1 and maintains 92 % capacity after 10 0 0 cycles at 0.5 C. Furthermore, it maintains superior performance under high cathode loading or low-temperature operation. This strategy provides a remarkable design for developing polymer electrolytes, paving a promising route toward practical solid-state lithium batteries with enhanced safety and cycle life. (c) 2026 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.

Pushing lithium cobalt oxide (LCoO2) toward extremely high-voltage operation up to 5V is critical to boosting a battery's energy density for future compact electronics. However, its degradation mechanisms at such extreme voltages remain unexplored. Here, we employ machine-learning-aided super-resolution electron microscopy to directly visualize, at atomic resolution, how LCoO2 structurally deteriorates under 5 V for the first time. We discover that deep delithiation activates global deformation in which in-plane shear breaks the O3 lattice into nanoscale mosaics of O1 and reoriented O3 domains, while out-of-plane distortions drive cracking and kinetically trapped structural motifs. Upon extended cycling, these coupled chemomechanical processes evolve into a frustrated surface architecture comprising intertwined misoriented domains and antiphase boundaries. Building on these mechanistic insights, we deliver a proof-of-concept demonstration that rationally designed codoping provides a targeted route to mitigate the coupled deformation and phase-degradation cascade, markedly pushing the cycling stability of LiCoO2 toward unprecedented ultrahigh voltage. Our work establishes a new paradigm for materials optimization by leveraging atomic-scale diagnostics to mitigate degradation at its origin.

ABSTRACT Room‐temperature sodium–sulfur polyacrylonitrile (SPAN) batteries are regarded as promising energy storage technology due to their high energy density, low cost, and high safety. However, dendrite growth in sodium anodes and dissolution shuttling effects in sulfur cathodes hinder their practical application. Here, we designed and achieved a solvation structure dominated by tridentate coordination by regulating the solvation configuration between sodium ions and diglyme through solvation strategies. The results indicate that the tridentate solvation structure not only reduces the dissolution shuttling of sodium polysulfide but also promotes the formation of a stable double‐layer inorganic electrolyte interface on the surface of the Na anode. The Na‐SPAN batteries achieved a high capacity retention of 97.46% after 1138 cycles and a calendar life exceeding 1 year at room temperature. Moreover, assembled Na‐SPAN batteries maintained 94.7% of their initial capacity after 445 cycles at 50°C. This work provides a well‐designed electrolyte principle for constructing a low‐cost, long‐cycle‐life room‐temperature Na‐SPAN battery.

Lithium-sulfur (Li-S) batteries are regarded as one of the most promising next-generation energy storage systems due to their high theoretical energy density and cost-effectiveness. However, the practical application is hindered by sluggish redox kinetics, polysulfide shuttling, and low active material utilization, especially under high sulfur loading and lean electrolyte conditions. Herein, we report a dual-reaction interlayer composed of 2, 5-dimercapto-1, 3, 4-thiadiazole (DMTD) and conductive carbon (Ketjen Black/single-walled carbon nanotube) to address these issues. This dual-reaction interlayer not only strongly anchors lithium polysulfides but also promotes their in-situ polymerization into short-chain solid-state sulfur-rich intermediates. This process transforms the conventional "solid-liquid-solid" sulfur redox pathway into a hybrid "solid-liquid-solid" and "solid-solid" conversion route, which significantly lowers the energy barrier of polysulfide conversion and enhances the completeness and reversibility of redox reactions. Specifically, it achieves a capacity of 1292 mA h g- 1 at 0.1 C, 822 mA h g- 1 at 3 C and 705 mA h g- 1 after 50 cycles at 0.2 C under a sulfur loading of 3.5 mg cm- 2, electrolyte/ sulfur ratio of 8 mu L mg- 1. This work provides insights into the regulation of reaction kinetics of lithium polysulfide reduction, contributing to the development of advanced practical Li-S batteries.