Capacity Retention Rate Research Articles

Mechanochemistry induced mixed ionic/electronic conductive interphase enabling dendrite-free lithium metal anodes

High-energy-density lithium metal batteries have shown promising applications in drones and electrical vehicles. However, the growth of lithium dendrites and the formation of unstable solid electrolyte interphase (SEI) become the main factors restricting their development. In this study, dendrite-free lithium metal anodes (ZB@Li) were developed with ionic/electronic conductive interface layers by a solvent-free mechanochemical method. By rubbing zinc borate (ZB) powder on lithium foil, a mixed interface layer is formed with the generation of lithium borate phase and the Li–Zn alloy phase. The lithium borate phase provides a low diffusion energy barrier and high ionic conductivity for sufficient potential gradient to induce rapid deposition of ions on the interface layer. The Li–Zn alloy phase owns the lithiophilic characteristic and a high electronic conductivity. The combination of the two phases provides mixed ions/electrons paths with enhanced transport kinetics and realize uniform and planar deposition of lithium. As a result, the ZB@Li symmetrical cell exhibits a prolonged cycling performance of over 4,200 h and the ZB@Li||LFP (LFP= lithium iron phosphate [LiFePO4]) full cell shows a long cycle life for more than 500 cycles at 2 C with a high capacity retention rate of 84.6% at a high loading mass of 10 mg/cm2.

Temperature-responsive poly(3-decylpyrrole) endowing Li-ion batteries with thermal shutdown function and improved electrochemical performance

Exploring a simple way that can accurately respond to abnormal temperature increase within battery and then promptly shut down the corresponding thermally abused battery is crucial to improving the thermal safety of lithium-ion batteries (LIBs), yet still faces challenges. To counter this, a temperature-sensitive LCO-P3DPY cathode was constructed with a new conductive polymer, i.e., poly(3-decylpyrrole): poly(4-styrenesulfonic acid) (P3DPY: PSS). Safety tests demonstrated that P3DPY exhibited an exceptional positive temperature coefficient (PTC) effect at 100 °C, coinciding with the dangerous occurrence temperature (100 °C) of most LIBs. Consequently, the LCO-P3DPY cathode displayed a significant thermal shutdown in the immediate aftermath of thermal abuse within the battery, showing a capacity output of only 1.7 mAh g−1. Furthermore, LCO-P3DPY cathode not only exhibited excellent electrochemical stability in the battery environment, but also enhanced electrochemical performance, as compared with the traditional batteries at room temperature. After 200 charging-discharging cycles at 0.25C, LCO-P3DPY cathode was able to maintain a reversible capacity of 142.8 mAh g−1, corresponding to a capacity retention rate of 91.83 % that is better than that of blank LCO (62.86 %). This work provides a potential strategy to solve the thermal safety problem and simultaneously improve the electrochemical stability of LIBs.

The regeneration of natural stibnite with introduced oxide-based catalyst towards enhanced Li-storage properties

Owing to its excellent theoretical specific capacity, Sb2S3 captures widespread attention in the energy-storage field. However, it still suffers from volume expansion and sluggish electrochemical kinetics. Meanwhile, considering serious pollution and complex chemical preparation processes, stibnite is regarded as “first-hand” materials, displaying enormous energy-storage application potential; however, it is still limited by low-purity and high crystallinity. Herein, stibnite is purified and regenerated through physical chemical and vacuum gas-phase melting strategy to form high-properties stibnite-based electrode materials. Assisted by the introduction of lithium nitrate as an active medium, abundant sites and effective structural traits are formed, effectively promoting the reversibility of electrochemical kinetic processes. Utilized as lithium-ion battery anodes, the as optimized samples have a capacity of approximately 656.8 mAh g−1 with a capacity retention rate of 89.9 % at 0.5 A g−1. Even at 5.0 A g−1, the capacity of 483.3 mAh g−1 could be remained after 100 cycles. Supported by a detailed kinetic analysis, the enhancement of the surface-controlling behavior and the reduction of capacitive resistance are confirmed. Herein, the as-regenerated phase and the introduced oxide-based catalyst are beneficial to alleviate polysulfide shuttling and volume expansion, further accelerating ion/electron transfer behaviors. This work is expected to shed light on strategies to design promising mineral-based anodes for lithium-ion batteries.

Advanced 3D-Printed Potassium Ammonium Vanadate/rGO Aerogel Cathodes for Durable and High-Capacity Potassium-Ion Batteries.

A 3D-printed oxygen-vacancy-rich potassium ammonium vanadate/reduced graphene oxide (KNVOv/rGO) microlattice aerogel is designed for the cathode in high-performance K-ion batteries (KIBs). The 3D-printed KNVOv/rGO electrode with periodic submillimeter microchannels and interconnected printed filaments is composed of highly dispersed KNVOv nanobelts, wrinkled graphene nanoflakes, and abundant micropores. The well-defined 3D porous microlattice structure of the rGO backbone not only provides the interconnected conductive 3D network and the required mechanical robustness but also facilitates the penetration of the liquid electrolyte into inner active sites, consequently ensuring a stable electrochemical environment for K-ion intercalation/deintercalation within the KNVOv nanobelts. The 3D-printed KNVOv/rGO microlattice aerogel electrode has a high discharge capacity of 109.3 mAh g-1 with a capacity retention rate of 92.6% after 200 cycles at 50mA g-1 and maintains a discharge capacity of 75.8 mAh g-1 after 2000 cycles at 500mA g-1. The flexible pouch-type KIB battery consisting of the 3D-printed KNVOv/rGO has good mechanical durability and retains a high specific capacity under different forms of deformation such as bending and folding. The results provide valuable insights into the integration of advanced 3D-printed electrode materials into K-ion batteries and the design of flexible and wearable energy storage devices.

Surface to bulk design empowering Ni-rich layered oxide cathode in sulfide-based All-Solid-State batteries

All-solid-state batteries (ASSBs) employing sulfide solid electrolytes (SSE) and high-nickel layered oxide cathodes have attracted considerable attention, attributed to their superior safety and great potential for high energy densities. However, the interface compatibility between SSE and nickel-rich oxide cathode remains a challenge. Here, a dual-functional strategy of Li6.25La3Zr2Al0.25O12 surface coating and bulk Zr doping in LiNi0.8Co0.1Mn0.1O2 was proposed (NCM811@CD-LLZAO), aiming to enhance the interfacial compatibility toward sulfide-based ASSBs. The fabricated ASSBs exhibit an impressive capacity retention rate of 91.1% after 100cycles at 0.1C and can sustain an ultra-long cycling performance over 1000cycles at 1.0C. Remarkably, even at a high rate of 11.0C, the battery still maintains a high capacity, highlighting its excellent rate performance. The distribution of relaxation time (DRT) analysis reveals that the LLZAO buffering layer can enhance the kinetics at the cathode/electrolyte interface. Theoretical calculation further confirms that the strong Zr-O bond formed by Zr doping can stabilize the lattice oxygen and effectively prevent the sulfide solid electrolyte from further electrochemical oxidation, thereby enhancing the interfacial dynamic and stability. These encouraging results provide a new strategy for the practical application of high-energy–density ASSBs, enabling fast charge transfer, extended cycle longevity and enhanced safety.

N/O co-doped poly(γ-glutamic acid)/Ni2+/melamine/chitosan nanoparticle-based hollow graphite carbon spheres for aqueous zinc-ion hybrid supercapacitors

Hollow carbon spheres (HCSs) have attracted broad attention in aqueous zinc-ion hybrid supercapacitors (ZIHSCs) owing to their distinctive properties. However, traditional methods for fabricating HCSs face limitations, including complex multistep procedures, the use of corrosive chemicals, and stringent reaction conditions. In this work, biomass-based poly(γ-glutamic acid)/Ni2+/melamine/chitosan nanoparticles were used as the precursors to fabricate N/O co-doped hollow graphite carbon spheres (HGCSs). Thanks to the appropriate hydrophilic characteristic, specific surface area, pore size distribution, and electrical conductivity, the fabricated HGCSs cathode exhibited superior electrochemical properties. The assembled HGCSs-based ZIHSCs device showed a satisfactory specific capacitance of 133.2 mAh·g−1 at a current density of 1.0 A·g−1, high energy densities of 75.2 Wh·kg−1 at 10,000 W·kg−1 and 107.9 Wh·kg−1 at 1000 W·kg−1, respectively. Additionally, the assembled HGCSs-based ZIHSCs device displayed an exceptional cycling stability, enduring up to 10,000 cycles at 0.5 A·g−1 with a capacity retention rate of 98.1 %. This work provides a facile and novel strategy to prepare superior electrochemical performance biomass-based HGCSs cathode for ZIHSCs.

NiCoP@amorphous carbon composites with 3D core-shell structure for high-performance asymmetric supercapacitors

In this paper, a facile bio-templating method is proposed to prepare NiCoP coated on amorphous carbon (NiCoP@AC) composite electrode materials with using bagasse as template and carbon source. NiCoP nanowire network arrays precursors coating on bagasse substrate with high yield were prepared via a novel synthesis strategy utilizing the toluene-water interface reaction process, which subsequently formed as NiCoP@AC composite electrode materials after phosphating process. The assembled core-shell structure attenuated the volume expansion during charging and discharging, additionally, the overall electrical conductivity of the composite was also improved owing to the characteristic of bagasse biochar. The NiCoP@AC electrode exhibited high specific capacitance (1706 F g−1 at 1 A g−1), outstanding rate capability (82.1 % capacity retention from 1 to 20 A g−1) and good cycling stability (retaining 80.0 % capacitance over 5000 cycles). In addition, bagasse biomass activated carbon (BAC) was prepared via a typical alkaline activation process for the use as negative electrode. The as-fabricated NiCoP@AC//BAC supercapacitor displayed a high energy density of 46.2 Wh kg−1 at a power density of 807.3 W kg−1, and an excellent capacitance retention rate (88.5 % after 5000 cycles), suggesting that the as-prepared NiCoP@AC electrode materials have wide application prospects in high-performance supercapacitors.

High entropy Prussian Blue Analogues assisted by reduced graphene oxide for enhancing the lifespan of Sodium-ion batteries

In recent years, Prussian blue analogues (PBAs) have been regarded as one of the most promising cathode materials for Sodium-ion batteries (SIBs) due to their open structure, low cost, and high theoretical capacity. However, the problem of capacity degradation caused by phase transitions during the charge/discharge process has so far limited the applicability of PBAs. While the high entropy strategy can alleviate capacity decay induced by phase transitions, challenges such as low conductivity, material aggregation, and severe interface reactions between electrode materials and electrolytes still persist. Therefore, we used a simple and scalable one-step co-precipitation method to grow high entropy Prussian blue analogues (HEPBA) on reduced graphene oxide (rGO) to address these problems. The rGO not only inhibits material agglomeration but also separates the electrolyte from the electrode material to prevent severe interface reactions. Meanwhile, the Warburg impedance is reduced and the Na+ diffusion performance is improved. When high entropy Prussian blue grown on an rGO matrix (HEPBA@rGO) is utilized as the cathode in a half-cell, it exhibits high discharge specific capacity (115.2 mAh g−1 at 100 mA g−1), long cycling stability (retaining 84.6 mAh g−1 after 1000 cycles), and good rate capability (62 mAh g−1 at 15 C). The full battery with HEPBA@rGO as the cathode and hard carbon as the anode has a high specific discharge capacity (100.12 mAh g−1 at 100 mA g−1), good stability (capacity retention rate of 81 % after 150 charge/discharge cycles), and good rate performance (72.5 mAh g−1 at 5 C). This study provides valuable insights for the development of SIBs.

Ti-Substituted O3-NaNi0.5Mn0.3Ti0.2O2 Material with a Disordered Transition Metal Layer and a Stable Structure.

O3-type NaNi0.5Mn0.5O2 (NNM) is very competitive for sodium-ion batteries (SIBs) due to its high capacity and easy production. Nevertheless, the intricate phase transitions during the charging-discharging significantly impede its practical application. This paper proposes a strategy for successfully synthesizing NaNi0.5Mn0.3Ti0.2O2 (NNMT) by combining coprecipitation and a high-temperature solid-state method. This method introduces Ti elements while retaining the electrochemically active Ni2+ content, thus, the NNMT has a high initial specific capacity of 151.4 mAh g-1 at 1 C. It is demonstrated that introducing Ti4+ leads to the transition metal layers becoming disordered by ex situ XRD, thus mitigating the irreversible phase transition of the material. In addition, Ti4+ does not have an outer electron, which can reduce electron delocalization in the transition metal layer and improve the material's cyclic stability. The NNMT possesses a capacity retention rate of 60.66% after 150 cycles, much higher than the initial NNM's 18.96%. It also exhibits an excellent discharge capacity of 86.8 mAh g-1 at 5 C. In conclusion, the cycling and rate performance of the Ti-substituted NNMT are greatly improved without capacity loss, which offers innovative concepts for the modification means of the SIBs layered oxide cathode materials.

Batch Preparation and Performance Study of Boehmite-Based Electrospun Nanofiber Separators for Lithium-Ion Batteries.

The design and preparation of high-performance separators for lithium-ion batteries (LIBs) have far-reaching practical significance in enhancing the overall performance of LIBs. Electrospun nanofiber separators (ENSs) have the characteristics of large specific surface area, high porosity, small pore size and good affinity with the electrolyte, making them become ideal candidates for LIB separators. In this work, polyacrylonitrile (PAN)/polyurethane (PU) (PAU) ENSs loaded with boehmite (BM) particles (BM/PAU ENSs) were mass-produced using spherical section free surface electrospinning (SSFSE), and used as LIB separators. Their morphology, structures and performances were tested and characterized. The results showed that all BM/PAU ENSs maintained excellent thermal dimensional stability in the range of 140-180 °C, and had good electrolyte wettability and high porosity. The composite BM/PAU-2 ENS with the best performance had a porosity of 52.5%, an electrolyte uptake rate of 822.1%, and an ionic conductivity of 1.97 mS/cm. Additionally, the battery assembled with BM/PAU-2 separator also demonstrated best electrochemical performance, cycling performance, and rate capability, with a capacity retention rate of 94.4% after 80 cycles at 0.5 C, making it a promising high-performance separator for LIBs.

Localized nitride strategy to construct interfacial and electronic modulated WO3/WN nanoparticles for superior lithium-ion storage

The interfacial effect is important for the tungsten trioxide (WO3)-based anode to achieve superior lithium-ion storage performance. Herein, the interfacial effect was constructed by in-situ surface direct nitridation reaction at 600 ℃ for 30 min of the as-synthesis WO3 nanoparticles (WO3/WN). X-ray photoelectron spectroscopy (XPS) analysis confirms evident chemical interaction between WO3 and WN via the interfacial covalent bond (WON). This WO3/WN anode shows a distinct interfacial effect for an efficient interatomic electron migration. Electrochemical kinetic analysis shows enhanced pseudocapacitance contribution. The galvanostatic intermittent titration technique (GITT) result demonstrates improved charge transfer kinetics. Ex-situ X-ray diffraction (XRD) analysis reveals the reversible oxidation and reduction reaction of the WO3/WN anode. The density functional theory (DFT) result shows that the evident interfacial bonding effect can enhance the electrochemical reaction kinetics of the WO3/WN anode. The discharge capacity can reach up to 546.9 mA h g−1 at 0.1 A g−1 after 200 cycles. After 2000 cycles, the capacity retention is approximately 85.97 % at 1.0 A g−1. In addition, the WO3/WN full cell (LiFePO4/C//WO3/WN) demonstrates excellent rate capability and capacity retention ratio. This in-situ surface nitridation strategy is an effective solution for designing an oxide-based anode with good electrochemical performance and beyond.

N‐Doped Carbon Coated Bimetallic CoFe2O4 Nanomembranes as An Enhanced Negative Electrode for Asymmetric Supercapacitors

AbstractIn‐suit nitrogen‐doped carbon layer coated on CoFe2O4 nanomembrane (NC−CoFe2O4) directly grown on carbon cloth was successfully fabricated. The electrochemical performance was conveniently manipulated by regulating the molar ration of Co2+ : Fe3+ (molar ration=1 : 2, CoFe2O4 nanomembrane, 2.9 F cm−2). Nitrogen‐doped (N‐doped) carbon coating strategy on CoFe2O4 nanomembrane (NC−CoFe2O4) via annealing of polypyrrole (PPy) was presented and NC−CoFe2O4 nanomembranes displayed a prominent capacitance of 12.1 F cm−2 (2563.8 F g−1) at 5 mA cm−2. More important, the composite demonstrated more stable microstructure and showed long‐term cycling stability (16.0 % decrease after 7000 cycles), which was significantly better than the unmodified CoFe2O4 (55.8 % decrease after 1000 cycles). To verify the practicability of the materials, an aqueous asymmetric supercapacitor has been fabricated using NC−CoFe2O4 composite anode and MnO2/CNTs cathode, and the device has a remarkable wide operating voltage range of 1.9 V. In addition, the assembled device has an exceptional specific capacity of 1.3 F cm−2 at 10 mA cm−2, high energy density (43.3 Wh kg−1 at a power density of 642.9 W kg−1), and also with a good capacity retention rate of 84.9 % after 1000 cycles.

Phosphate ions functionalized metal-organic framework-derived cobalt oxide with improved redox reactivity for high-performance alkaline aqueous Zn-ion batteries

Alkaline aqueous Zn/Co3O4 batteries (AZCBs) have captured significant attention within the field of scalable grid energy storage due to their high output voltage (>1.8 V), superior safety profile, and low manufacturing cost. Nevertheless, the intrinsic Co3O4 material experiences limitations in terms of low electronic conductivity and insufficient active sites, consequently constraining its electrochemical performance in AZCBs. To address this challenge, this investigation focuses on the use of phosphate ions functionalized Co3O4 (referred to as PCO) material derived from cobalt-based metal-organic frameworks (Co-MOFs) as a cathode electrode in AZCBs. Both theory calculations and experimental verification illustrate that the functionalization with phosphate ion enhances the active sites for electrochemical redox reactions and increases the electrical conductivity of intrinsic Co3O4. Consequently, a pouch cell configuration of PCO-2||Zn with the optimized PCO-2 sample as cathode exhibits a high capacity of 162.0 mAh g−1, a maximum energy density of 265.7 Wh kg−1, a maximum power density of 16.39 kW kg−1. Furthermore, excellent long-term stability is observed, with the capacity retention rate reaching 92.3 % over 5000 cycles at a high current density of 5 A g−1. Additionally, the constructed fibrous flexible solid-state device also demonstrates notable long-term stability, with a capacity retention of 96 % after 2000 cycles under a high current density of 10 mA cm−2, and performs well under different deformation statuses. This successful approach may hold potential for the exploration of other cathode materials, such as Mn or V-based compounds, which may exhibit high performance in aqueous zinc-based batteries.

Highly Graphitized Coal Tar Pitch-Derived Porous Carbon as High-Performance Lithium Storage Materials.

Because of its high specific capacity and superior rate performance, porous carbon is regarded as a potential anode material for lithium-ion batteries (LIBs). However, porous carbon materials with wide pore diameter distributions suffer from low structural stability and low electrical conductivity during the application process. During this study, the calcium carbonate nanoparticle template method is used to prepare coal tar pitch-derived porous carbon (CTP-X). The coal tar pitch-derived porous carbon has a well-developed macroporous-mesoporous-microporous hierarchical porous network structure, which provides abundant active sites for Li+ storage, significantly reduces polarization and charge transfer resistance, shortens the diffusion path and promotes the rapid transport of Li+. More specifically, the CTP-2 anode shows high charge capacity (496.9 mAh g-1 at 50 mA g-1), excellent rate performance (413.6 mAh g-1 even at 500 mA g-1), and high cycling stability (capacity retention rate of about 100 % after 1,000 cycles at 2 A g-1). The clean and eco-friendly large-scale utilization of coal tar pitch will facilitate the development of high-performance anodes in the field of LIBs.

Effects of surfactants on the morphologies, structures, and electrochemical activities of WO3/Ag2O nanocomposites for supercapacitor electrodes

For energy storage, supercapacitors have been extensively developed. Among them, pseudocapacitors that use faradaic reactions of conductive polymers and transition metal oxides exhibit high electrochemical performance. In this study, WO3-based electrodes for high-performance pseudocapacitors were designed with Ag2O and various surfactants, with the aim to extend of the potential range and shape control of WO3 crystals. The WO3/Ag2O nanocomposites were prepared on a carbon cloth via chemical bath deposition with different types of surfactants: cetyltrimethylammonium bromide (CTAB), sodium dodecyl sulfate (SDS), and Pluronic F-127. Both Ag and the surfactants affected the morphology of the WO3 crystals; their crystal sizes were decreased, and the crystallinity was improved. The specific capacitance of the WO3/Ag2O nanocomposite was 621 F/g at 5 mV/s, whereas that of WO3 was 397 F/g. Furthermore, the specific capacitance of the nanocomposites increased with the use of surfactants: 960 F/g for WO3/Ag2O@Pluronic F-127, 641 F/g for WO3/Ag2O@CTAB, and 846 F/g for WO3/Ag2O@SDS at 5 mV/s. WO3/Ag2O@Pluronic F-127 had superior capacitance and exhibited a charge/discharge capacitance retention rate of 135 % after 2000 cycles at 5 A/g. The symmetric electrode configuration of WO3/Ag2O@Pluronic F-127 exhibited a maximum energy density of 85 W h kg−1 and a power density of 670 W kg−1. These results highlight the significant potential of the WO3/Ag2O@Pluronic F-127 nanocomposite electrode for future energy storage devices.

Crystal water-capturing and film-forming bifunctional electrolyte additive for stabilizing sodium iron hexacyanoferrate cathode for Na-ion batteries

Due to its affordability, strong structural stability, and high rate capability, rhombohedral sodium ferrous hexacyanoferrate (FeHCF) has been identified as a potential cathode material for sodium ion batteries. Nevertheless, the presence of inherent crystal water and the susceptibility of its interface stability significantly hinder its capacity and cycling performance. In this study, we propose a novel modification approach involving the addition of ZnCl2 to effectively capture crystal water and facilitate the in-situ formation of a ZnO coating on the FeHCF surface. Due to the decreased crystal water content and the presence of stable ZnO interphases, the occurrence of side reactions between the electrode and electrolyte, as well as crystal particle cracks in FeHCF during repeated sodiation/desodiation processes, is effectively reduced. Consequently, the modified FeHCF demonstrates an extended operational lifespan of 1000 cycles, with an initial discharge capacity of 112.0 mAh/g and a capacity retention rate of 77.8 % at a current rate of 1C within the voltage range of 2.0–4.2 V. Our research offers valuable insights into the removal of crystal water and the engineering of incident interfaces to enhance the cycle life of FeHCF cathodes in sodium-ion batteries.

Retarding the capacity fading and voltage decay of Li-rich Mn-based cathode materials via a compatible layer coating for high-performance lithium-ion batteries.

Li-rich Mn-based layered oxides have been considered as the most promising cathode candidate for high energy density lithium ion batteries. However, the practical application of Li-rich Mn-based layered oxides is hindered due to the capacity fading and voltage decay accompanied with structure transition from the layered structure to spinel phase during cycling. Herein, a facile surface structure repair via Ce modification is reported. The structural analysis of the bulk and coating layer was carried out using XRD, XPS, SEM and TEM, which confirmed the successful doping of Ce and formation of a Li2CeO3 coating on the surface. The modified sample LLO-2 delivers a discharge specific capacity of 263.5 mA h g-1 at 0.1C and capacity retention rate with 88.1% at 0.2C after 100 cycles compared to 250.2 mA h g-1 and 75.6% for the pristine sample. The enhanced performance could be because Ce doping enlarges the lattice parameter, which may contribute to accelerating the Li+ diffusion rate. Moreover, the newly formed Li2CeO3 coating with oxygen vacancies could inhibit the loss of lattice oxygen and protect the electrode surface by suppressing the attack from the electrolyte. This work provides an effective approach to design Li-rich Mn-based layered oxides with improved electrochemical performance.

Tetraphenylanthraquinone and Dihydroxybenzene-Tethered Conjugated Microporous Polymer for Enhanced CO2 Uptake and Supercapacitive Energy Storage.

Conjugated microporous polymers (CMPs) feature extended excellent porosity properties and fully conjugated electronic systems, making them highly effective for several uses, including photocatalysis, dye adsorption, CO2 capture, supercapacitors, and so on. These polymers are known for their high specific surface area and adjustable porosity. To synthesize DHTP-CMPs (specifically TPE-DHTP CMP and Anthra-DHTP CMP) with abundant nitrogen (N) and oxygen (O) adsorption sites and spherical structures, we employed a straightforward Schiff-base [4 + 2] condensation reaction. This involved using 2,5-dihydroxyterephthalaldehyde (DHTP-2CHO) as the primary building block and phenolic OH group source, along with two distinct structures: 4,4',4″,4"'-(ethene-1,1,2,2-tetrayl)tetraaniline (TPE-4NH2) and 4,4',4″,4"'-(anthracene-9,10-diylidenebis(methanediylylidene))tetraaniline (Anthra-4Ph-4NH2). The synthesized Anthra-DHTP CMP had a remarkable BET surface area (BETSA) of 431 m2 g-1. Additionally, it exhibited outstanding thermal stability, as shown by a T d10 of 505 °C. Furthermore, for practical implementation, the Anthra-DHTP CMP demonstrates a significant capacity for capturing CO2, measuring 1.85 mmol g-1 at a temperature of 273 K and 1 bar. In a three-electrode test, the Anthra-DHTP CMP has a remarkable specific capacitance of 121 F g-1 at 0.5 A g-1. Furthermore, even after undergoing 5000 cycles, it maintains a capacitance retention rate of 79%. Due to their outstanding pore characteristics, abundant N and O, and conjugation properties, this Anthtra-DHTP CMP holds significant potential for CO2 capture and supercapacitor applications. This work will pave the way for the development of materials based on DHTP-CMPs and their postmodification with additional groups, facilitating their use in photocatalysis, photodegradation, lithium battery applications, and so on.

Consecutive covalent bonds reconstruct robust dual-interfaces by carbonized binder to enable conductive-additive-free durable silicon anode

The substantial volume expansion and poor electrical conductivity tremendously hinder the utilization of high silicon (Si) content anode with compelling capacity. Herein, we propose an efficient strategy to stabilize Si-based anodes by carbonization of the slurry-casting Si electrode with a conductive polyoxadiazole (POD) binder. Such POD-derived materials can form a nitrogen/sulfur-rich carbon network, not only serving as a resilient scaffold to buffer the volume swelling and firmly adhere the Si to the current collector by robust dual-interfaces bonding but also evolving into a conductive matrix to facilitate the electron/ion transport. The conductive-additive-free Si electrode possesses a high Si content of up to 84 %. It exhibits a high initial Coulombic efficiency (86.34 %), competitive gravimetric capacity (3340 mAh g−1), stable cycling performance (the capacity retention rate reaches 79 % after 1000 cycles), commercial-level areal capacity (5.32 mAh cm−2), and outstanding rate capability (1673 mAh g−1 at 5.0 A g−1). This work offers a scalable modification idea and forward-looking perspective for high-performance Si-based anodes in next-generation lithium-ion batteries.

Promoting uniform lithium deposition with Janus gel polymer electrolytes enabling stable lithium metal batteries

AbstractLithium metal batteries (LMBs) are desirable candidates owing to their high‐energy advantage for next‐generation batteries. However, the practical application of LMBs continues to be constrained by thorny safety issues with the formation and growth of Li dendrites. Herein, the ZIF‐67 MOFs are in situ coupled onto a single face of 3D porous nanofiber to fabricate an asymmetric Janus membrane, harnessing their anion adsorption capabilities to promote the uniform deposition of Li ions. In addition, the poly(ethylene glycol) diacrylate and trifluoromethyl methacrylate are introduced into nanofiber skeleton to form Janus@GPE, which preferentially reacts with Li metal to form a LiF‐rich stable SEI layer to inhibit Li dendrite growth. Importantly, the synergistic effect of the MOFs and stable solid electrolyte interphase (SEI) layer results in superior cycling performance, achieving a remarkable 2500 h cycling at 1 mA cm−2 in the Li/Janus@GPE/Li configuration. In addition, the Janus@GPE electrolyte has a certain flame retardant, which can self‐extinguish within 3 s, improving the safety performance of the batteries. Consequently, the Li/Janus@GPE/LFP flexible pouch cell exhibits favorable cycling stability (the capacity retention rate of 45 cycles is 91.8% at 0.1 C). This work provides new insights and strategies to improve the safety and practical utility of LMBs.image