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Li and Zn metal batteries are the most promising candidates to replace conventional Li-ion batteries. However, a series of issues, especially dendrites caused by uneven deposition of cations during charge-discharge cycles, hinder their practical application. Here, we proposed a facile separator modification method which combines physical and chemical forces to regulate uniform and rapid deposition of both Li

Energy storage materials 50, 464 - 472 (2022). doi:10.1016/j.ensm.2022.05.048, A cathode/anode compatible aqueous zinc triflate electrolyte is proposed by reorganizing the solvation structure of the electrolyte using an acetonitrile co-solvent. Acetonitrile notably alters the hydrogen bonds of the electrolyte, reducing the activity of water. Using this electrolyte, a ZnǁV2O5 full-cell exhibits high Coulombic efficiency, long cycle life and high rate capability. The interactions between electrolyte, cathode and Zn anode are clarified based on comprehensive in operando and ex situ experiments and molecular dynamics simulations. The addition of acetonitrile does not change the bulk ion storage of V2O5, but the unique electrode-electrolyte interfacial films with specific compositions and spatial distribution protect the Zn and V2O5 electrodes and improve the interfacial kinetics of the electrodes, thus significantly promoting the cycling performance of the full cell. This cathode/anode compatible electrolyte can overcome the challenges of both the cathode and anode which would promote aqueous rechargeable zinc batteries into practical application., Published by Elsevier, Amsterdam

Aqueous zinc energy storage devices, holding various merits such as high specific capacity and low costs, have attracted extensive attention in recent years. Nevertheless, Zn metal anodes still suffer from a short lifespan and low Coulombic efficiency due to corrosion and side reactions in aqueous electrolytes. In this paper, we construct an artificial Sn inorganic layer on Zn metal anode through a facile strategy of atoms exchange. The Sn layer suppresses Zn dendrite growth by facilitating homogeneous Zn plating and stripping during charge and discharge processes. Meanwhile, the Sn protective layer also serves as a physical barrier to decrease Zn corrosion and hydrogen generation. As a result, The Sn-coated anode (Sn|Zn) exhibits a low polarization voltage (∼34 mV at 0.5 mAh/cm2) after 800 testing hours and displays a smooth and an even surface without corrosion. Moreover, the zinc ion capacitor (Sn|Zn|| activated carbon) is assembled with an enhanced capacity of 42 mAh/g and a capacity retention of 95% after 10000 cycles at 5 A/g. This work demonstrates a feasible approach for the commercialization of aqueous Zn-based energy storage devices.

A fundamental understanding of the nucleation and growth behaviors of Zn metal anodes over a wide range of temperatures is of great value for suppressing Zn dendrite growth. However, work focused on the early nucleation and growth behavior of Zn metal at various temperatures is still absent. Here, we study the effect of cycling temperature on Zn nuclei size and areal density and find that low temperature induces a smaller and dense nucleus, which prevents the formation of dendrites. Based on this finding, a cooling-treatment-based self-healing strategy is developed to in situ eliminate dendrites, which effectively prolongs the lifespan of the Zn anode by 520%. This novel self-healing strategy could be employed as a reliable strategy for restoring batteries in situ to reach a longer lifespan.

Dendrite growth and side reactions of Zn metal anodes remain unresolved obstacles for practical application of aqueous Zn ion batteries. Herein, a two-dimensional (2D) organic-inorganic heterostructure with controlled thickness was constructed as a protective layer for a Zn metal anode. The reduction of uniformly distributed polyoxometalate in the layer causes a negative charge density gradient, which can accelerate zinc ion transfer, homogenize zinc deposition, and shield sulfates at the electrode interface, while the exposed hydrophobic alkyl chain of the layer can isolate the direct contact of water with the Zn anode. As a result of the synergetic effect, this 2D organic-inorganic heterostructure enables high Zn plating/stripping reversibility, with high average Coulombic efficiencies of 99.97% for 3700 cycles at 2 mA cm(-2). Under high Zn utilization conditions, a high areal-capacity full cell with hundreds of cycles was demonstrated.

Aqueous zinc metal batteries with mild acidic electrolytes are considered promising candidates for large-scale energy storage. However, the Zn anode suffers from severe Zn dendrite growth and side reactions due to the unstable interfacial pH and the absence of a solid electrolyte interphase (SEI) protective layer. Herein, a novel and simple mixed electrolyte strategy is proposed to address these problems. The mixed electrolytes of 2 M ZnSO

Magnesium ion batteries have attracted increasing attention as a promising energy storage device due to the high safety, high volumetric capacity, and low cost of Mg. However, the strong Coulombic interactions between Mg2+ ions and cathode materials seriously hinder the electrochemical performance of the batteries. To seek a promising cathode material for magnesium ion batteries, in this work, (NH4)2V6O16·1.5H2O and water-free (NH4)2V6O16 materials are synthesized by a one-step hydrothermal method. The effects of NH4+ and lattice water on the Mg2+ storage properties in these kinds of layered cathode materials are investigated by experiments and first-principles calculations. Lattice water is demonstrated to be of vital importance for Mg2+ storage, which not only stabilizes the layered structure of (NH4)2V6O16·1.5H2O but also promotes the transport kinetics of Mg2+. Electrochemical experiments of (NH4)2V6O16·1.5H2O show a specific capacity of 100 mA·h·g-1 with an average discharge voltage of 2.16 V vs Mg2+/Mg, highlighting the potential of (NH4)2V6O16·1.5H2O as a high-voltage cathode material for magnesium ion batteries.

Redox mediators (RMs) have a substantial ability to govern oxygen reduction reaction (ORR) in Li-O

Fe/Co-based diatomic catalysts decorated on an N-doped graphene substrate are investigated by first-principles calculations to improve the electrochemical properties of Li–S batteries. Our results demonstrate that FeCoN8@Gra not only possesses moderate adsorption energies towards Li2S n species, but also exhibits superior catalytic activity for both reduction and oxidation reactions of the sulfur cathode. Moreover, the metallic property of the diatomic catalysts can be well maintained after Li2S n adsorption, which could help the sulfur cathode to maintain high conductivity during the whole charge–discharge process. Given these exceptional properties, it is expected that FeCoN8@Gra could be a promising diatomic catalyst for Li–S batteries and afford insights for further development of advanced Li–S batteries.

The shuttle effect of lithium polysulfides (LiPSs) is a fundamental problem restricting the commercialization of lithium–sulfur batteries. A polar conductive substrate serving as the sulfur positiv...

Transition metal oxychlorides (TMOCl) have attracted great attention as promising cathode materials for chloride ion batteries (CIBs). However, current research on TMOCl has been mainly focused on FeOCl and VOCl. On the other hand, the theoretical study of anionic rechargeable batteries faces the difficulty of predicting the discharge voltage of the electrode materials based on the half-cell system. Herein, a reliable theoretical voltage formula for CIBs is proposed based on a full-cell system with Li/LiCl as the reference anode. A high throughput screening method for TMOCl is applied among 16 transition metals. After the screening according to energetic and dynamic stability, Co is identified, which can form a new cathode material of CoOCl. Compared to FeOCl and VOCl, CoOCl has a higher discharge voltage, which is beneficial for achieving a larger energy density. The small crystal field splitting energy and exchange splitting energy of Co3+ result in higher electronic conductivity. In addition, the uniform Cl− binding environment leads to a low Cl− diffusion barrier of 0.37 eV, which is much smaller than that of VOCl (0.65 eV) and FeOCl (0.58 eV).

The unique properties of MXenes that arise from terminating functional groups and oxidation of MXenes make them attractive for application in photovoltaic devices like perovskite solar cells (PSCs). Here, oxidation of Ti3C2Tx hydrocolloid was carried out to tune its properties desirable for an electron transport layer (ETL) in low-temperature processed PSCs. The calculations of the energy levels were carried out using the Vienna ab initio simulation package (VASP) code based on density functional theory (DFT). Oxidation of Ti3C2Tx can generate Ti–O bonds and effectively reduce the macroscopic defects of the film fabricated by spin-coating, while a transition from metallic material to semiconductor occurred after heavy oxidation. A better matching of energy levels between perovskite and ETL layer in the case of a hybrid of oxidized and pristine Ti3C2Tx renders a champion power conversion efficiency (PCE) of 18.29%. The improvement in PCE can be attributed to the increased electron mobility in the ETL, which promotes electron transport and reduces the electron–hole recombination. Hence, by presenting a simple method for high performance in PSCs by MXene-derived materials, this work demonstrates the great potential of these materials for applications in low-temperature processed PSCs and other photovoltaic technologies.

NH4+ preintercalated V2O5·nH2O nanobelts with a large interlayer distance of 10.9 A were prepared by the hydrothermal method. The material showed a large specific capacity of 391 mA·h·g-1 at the 500 mA·g-1 current density in aqueous rechargeable zinc batteries. In operando synchrotron X-ray diffraction demonstrated that the material experienced reversible solid-solution reaction and two-phase transition during charge-discharge cycling, accompanied by the reversible formation/decomposition of a ZnSO4Zn3(OH)6·5H2O byproduct. In operando X-ray absorption spectroscopy confirmed the reversible reduction/oxidation of V, together with small changes in the VO6 local structure. The formation of byproduct was attributed to the dehydration of [Zn(H2O)6]2+, which concurrently improved the desolvation of [Zn(H2O)6]2+ into Zn2+. Bond valence sum map analysis and electrochemical impedance spectroscopy demonstrated that the byproduct improved the charge transfer kinetics of the electrode. Cyclic voltammetry and galvanostatic intermittent titration technique showed that the electrode reaction was dominated by ionic intercalation where the discharge capacity in the voltage window of 1.4-0.85 V was attributed to the intercalation of [Zn(H2O)6]2+, followed by the intercalation of Zn2+ at 0.85-0.4 V.

Controlling morphology, adopting metal cations and introducing crystal water are three effective strategies to improve the electrochemical performance of various battery electrodes. However, the effects of simultaneously applying these three strategies to aqueous rechargeable zinc batteries (ARZBs) are rarely demonstrated. Herein, hierarchical H11 Al2 V6 O23.2 (HAVO) microspheres were successfully prepared using a simple hydrothermal method, and used as cathode material for ARZBs. The as-prepared HAVO microspheres exhibited superior electrochemical performance than the dehydrated AlV3 O9 (AVO) microspheres, i. e. they have a larger specific capacity of 390.4 mA h g-1 at 100 mA g-1 , a better rate capability of 191.4 mA h g-1 at 5000 mA g-1 and a higher cycling stability of up to 1000 cycles with a capacity retention of 80.9 %. The excellent electrochemical performance of HAVO is due to the synergistic effects of the shortened ion diffusion distance in primary HAVO nanosheets, the improved electronic conductivity, and structural stability by adopting Al3+ into the lattice, the enhanced charge transfer properties and ion diffusion coefficient of the electrode due to the existence of crystal water. Therefore, this work may offer a new route for the design and synthesis of more advanced electrode materials for ARZBs.

Sodium (Na) metal batteries have attracted increasing attention and gained rapid development. However, the processing, storing, and application of Na metal anodes are restricted by its inherent stickiness and poor mechanical properties. Herein, an MXene (Ti3C2Tx)-coated carbon cloth (Ti3C2Tx-CC) host is designed and synthesized, which shows a highly metallic conductive and sodiophilic surface. After a thermal infusion treatment, a Na-Ti3C2Tx-CC composite with rigidity and bendability is obtained and employed as a metal anode for Na ion batteries. The Na-Ti3C2Tx-CC electrodes present stable cycling performance and high stripping/plating capacity in both an ether-based (up to 5 mA·h·cm-2) and a carbonate-based (up to 8 mA·h·cm-2) electrolyte. The fundamental protection mechanism of MXene Ti3C2Tx is investigated. Ti3C2Tx efficiently induces Na's initial nucleation and laterally oriented deposition, which effectively avoids the generation of mossy/dendritic Na. The arrangement of Na atoms deposited on the MXene surface inherits the MXene atomic architecture, leading to a smooth "sheet-like" Na surface. Meanwhile, a flexible Na-based Na-Ti3C2Tx-CC∥Na3V2(PO4)3 device is assembled and exhibits capable electrochemical performance.

Titanium-substituted LiTix Fe1-2x SO4 F (x=0, 0.01, 0.02, 0.03) cathode materials were synthesized by a solvothermal method. X-ray diffraction, X-ray photoelectron spectroscopy, and Mossbauer spectroscopy were used to investigate the effects of Ti substitution on the structure of LiFeSO4 F, and it was shown that Ti substitutes the Fe(2) site. First-principles calculations and UV-visible spectroscopy demonstrate that Ti substitution reduces the bandgap of LiFeSO4 F which improves the electronic conductivity from 8.3×10-12 S cm-1 to 3.9×10-11 S cm-1 . CI-NEB and BV calculations show that the Li diffusion energy barriers along the (100), (010) and (101) directions are decreased after Ti substitution, and the Li diffusion coefficient is increased from 4.99×10-11 cm2 S-1 to 1.59×10-10 cm2 S-1 . The improved electronic conductivity and ionic diffusivity mean that the Ti-substituted material shows improved electrochemical properties compared to the pristine LiFeSO4 F.

Hydrogen evolution reaction (HER) is vital for sustainable energy production and plays a key role in achieving a hydrogen economy. Herein, density functional theory calculations are used to screen ...

Soluble redox mediators (RMs) are one of the most promising approaches for reducing charging overpotentials in Li–O2 batteries. However, this auspicious strategy still in its infancy and raises new scientific problems needing to be clarified, such as the influence of RMs with different charge–transfer or different molecular structure (same redox functional group) on Li2O2 oxidation behavior. Herein, the realities of Li2O2 oxidation by some RMs, including lithium bromide, tetrathiafulvalene, 2,2,6,6–tetramethyl–1–piperidinyloxy, and 2–azaadamantane–N–oxyl, were investigated using detailed experimental results and first–principles calculations. Among these RMs studied, single electron–reaction RMs exhibited a more stable charging curve at lower potential than that of multiple electron–reaction RMs. Besides, the RM molecular with smaller steric effects and higher electron–donating power exhibited higher catalytic activity thus a lower charging overpotential. These findings offered a guidance direction for subsequent explorations and optimization of high performance RMs, which might further facilitate development for Li–O2 batteries.

Magnesium ion batteries (MIBs) have attracted increasing attention due to their advantages of abundant reserves, low price, and high volumetric capacity. However, the large Coulombic interactions o...

The ORR and OER properties of a series of recombinant single atom catalysts (SACs) prepared by recombining Pt single atoms on 26 representative MXenes were comprehensively studied by first-principles calculations. The stability of Pt atoms on the MXene surface was studied using formation energies and diffusion energy barriers. Charge transfer analysis showed that the Pt atoms not only acted as the catalytic center of the SACs but also behaved as a charge transfer medium between the MXene substrate and the reactants. The catalytic properties of the recombinant SACs were dependent on several interacting factors including the Pt-5d states, the work functions of the recombinant systems, the electronegativity of the submetals, and the vacant electron orbitals of the C/N and O/F elements of the MXenes. In all the recombinant SACs under investigation, V-, Ti-, Nb-, and Cr-based MXenes, including Ti2CF2-VF-Pt, Ti3C2F2-VF-Pt, V2CO2-VO-Pt, Nb2CF2-VF-Pt, Nb4C3F2-VF-Pt, Cr2TiC2F2-VF-Pt, Ti3(C,N)2-CO2-VO-Pt, and Ti3(C,N)2-NO2-VO-Pt, were screened as promising ORR catalysts. In particular, three F-terminated ones (Nb2CF2-VF-Pt, Nb4C3F2-VF-Pt, and Cr2TiC2F2-VF-Pt) were proposed as effective ORR/OER bifunctional catalysts. The results revealed the highly active nature of the selected SACs and highlighted the great potential of MXenes as efficient ORR and OER catalysts.

NASICON-structured Na4MnV(PO4)3 has been recognized as a potential positive electrode material for sodium-ion batteries, but its electrochemical mechanism during de(sodiation) has not been well understood. In this work, the structural transformation, charge transfer, and ionic diffusion properties of Na4MnV(PO4)3 were comprehensively studied by first-principles calculations combined with experimental studies. The results revealed two independent Na sites, Na(1) and Na(2), in the structure of Na4MnV(PO4)3, but only Na(2) can be extracted between 2.5 and 3.8 V. Extraction of the first Na+ caused charge transfer on V3+ and was associated with a solid-solution reaction. In addition, Na+ migrated along the 3D channels in the NASICON structure with low energy barriers of

Lithium metal batteries are promising next generation energy storage devices. However, uncontrolled lithium dendrite growth and inevitable side reactions of traditional organic liquid electrolytes with electrodes are obstacles to their practical applications. Herein, a new ionogel electrolyte with an organic–inorganic semi-interpenetrating network is designed by the confinement of ionic liquid within a NH2 pendent group optimized cross-linked poly(ionic liquid) copolymer backbone and glass fiber scaffold. The ionogel electrolyte shows superior physicochemical properties, including improved lithium ion transmission, high mechanical strength, wide electrochemical window, non-leakage, non-volatility and fire resistance. In Li//Li symmetric cells fabricated with this ionogel electrolyte, repeated Li plating/stripping could last over 1800 h without significant dendrite formation. Besides, the full cells paired with a high-voltage Li3V2(PO4)3 cathode present excellent cycling stability with a capacity retention of 83% after 1000 cycles (0.5C rate, 3.0–4.3 V) and 91% after 100 cycles (0.2C rate, 3.0–4.8 V). This study presents a new strategy for the use of organic–inorganic semi-interpenetrating networks for designing new composite ionogel electrolytes with desirable properties for high-voltage LMBs.

Developing highly active, stable, and conductive bifunctional oxygen reduction (ORR) and oxygen evolution (OER) catalysts is a key step for fuel cells and metal–air batteries. Herein, an effective idea for designing bifunctional catalysts is presented by regulating the surface electronic structures of Nb2CT2 (T = O, F, and OH) using Pt/Pd single atoms. The results indicated that Pt-doped systems (Nb2CO2–VO–Pt, Nb2CF2–VF–Pt) were the most promising bifunctional ORR/OER catalysts. In particular, Nb2CF2–VF–Pt was even better than landmark Pt(111) and IrO2(110) catalysts, with relatively low overpotentials of 0.40 V and 0.37 V for ORR and OER, respectively. The high catalytic nature of Nb2CF2–VF–Pt was explained by electronic structures, volcano plots, and charge transfer mechanisms, which mainly depended on the electron donor capacity and synergistic effects from F-terminated groups and Pt noble metals. Moreover, 100% utilization of Pt was achieved for the designed bifunctional catalysts with a minimum radius between two adjacent active centers. This was the first design of a bifunctional ORR/OER catalyst based on Nb2CT2 and highlighted a new perspective on the application of MXenes.

Two-dimensional transition metal dichalcogenides are promising anode materials for Na ion batteries (NIBs). In this study, we carried out a comprehensive investigation to analyze the structural, electrochemical characteristics, and diffusion kinetics of bulk WX

A novel metallic carbon allotrope, Q-carbon, was discovered using first-principles calculations. The named Q-carbon possessed a three-dimensional (3D) cage structure formed by carbon atoms with three ligands. The energy distribution of electrons in different orbitals revealed that Q-carbon has a low degree of s-p orbital hybridization. The calculated Li

The difficult Mg2+ desolvation of chloride-based electrolytes and slow Mg2+ diffusion in the cathode seriously hinder the electrochemical performance of Mg-ion batteries (MIBs). To solve these problems, a high performance MIB cell was built using a VS2 nanosheet cathode and with 0.4 M (PhMgCl)2-AlCl3/tetrahydrofuran (APC/THF) and 50 wt.% 1-butyl-1-methylpiperidinium chloride (PP14Cl) as the electrolyte. The resulting system showed a large capacity of 348 mA h g−1 at 20 mA·g−1 current density and excellent rate capability with a 214 mA h g−1 capacity at 2.0 A·g−1 current density. A thorough experimental and theoretical study showed that Mg2+ desolvation energy was reduced from 3.0 to 0.67 eV under the catalytic effects of PP14+. Moreover, large-sized PP14+ was inserted into the VS2 interlayer during the first discharge and permanently resided in the material. As a result, the interlayer spacing of VS2 was largely expanded, which improved the Mg2+ diffusion coefficient by three orders of magnitude to 10−10–10−12 cm−2 s. The reduced Mg2+ desolvation energy by the catalytic effects of PP14+, together the improved Mg2+ diffusion kinetics by the interlayer expansion effect of PP14+, provided a significant implement way towards development of high performance and practical MIBs by electrolyte regulation.

MXenes have been used as substrate materials for single-atom catalysts (SACs) due to their unique two-dimensional (2D) structure, high surface area, and high electronic conductivity. Oxygen is the primary terminating group of MXenes; however, all of the reported Pt SACs till now are fabricated with F-terminated MXenes. According to the first-principles calculations of this work, the failure of using O-terminated MXenes as substrates is due to the low charge density around Pt and C, which weakens the catalytic activity of Pt. By adjusting the electronic structure of M2C using a second submetal with a lower work function than M, 18 potential bifunctional Pt SACs are constructed based on O-terminated bimetal MXenes. After further consideration of some important practical application factors such as overpotential, solvation effect, and reaction barriers, only four of them, i.e., Cr2Nb2C3O2-VO-Pt, Cr2Ta2C3O2-VO-Pt, Cr2NbC2O2-VO-Pt, and Cr2TaC2O2-VO-Pt, are screened as bifunctional oxygen reduction reaction/oxygen evolution reaction (ORR/OER) catalysts. All of these screened SACs are originated from Cr-based MXenes, implying the significance of Cr-based MXenes in designing bifunctional Pt SACs.

An artificial organic/inorganic composite protecting film for lithium metal anode with one-side surface pits structure was prepared by poly(vinylidene fluoride-co-hexafluoropropylene) and Al2O3+LiNO3 inorganic additives. Due to the unique surface structure, the composite film can not only serve as an artificial protective film, but also act as an additional lithium plating host, which synergistically enabled the lithium metal anode to adapt to high current densities meanwhile maintain dendrite-free during long-term cycling. As a result, the protected lithium metal anode can operate stably for 1000 h at a high current density of 10.0 mA cm-2. When paired with a LiFePO4 or sulfur cathode, the full cells with unflooded electrolyte showed significantly improved cycling performance, demonstrating great potential of this artificial protecting film in lithium metal batteries.

Magnesium ion batteries have attracted increasing attention as a promising energy storage device due to the high safety, high volumetric capacity, and low cost of Mg. However, the strong Coulombic interactions between Mg

Metallic anodes have high theoretical specific capacities and low electrochemical potentials. However, short-circuit problems caused by dendritic deposition and low Coulombic efficiency limit the cyclic life and safety of metallic anode-based batteries. Herein, dendrite-free and flexible three-dimensional (3D) alkali anodes (Li/Na-Ti3C2Tx-rGO) are constructed by infusing molten lithium (Li) or sodium (Na) metal into 3D porous MXene Ti3C2Tx-reduced graphene oxide (Ti3C2Tx-rGO) membranes. First-principles calculations indicate that large fractions of functional groups on the Ti3C2Tx surface lead to the good affinity between the Ti3C2Tx-rGO membrane and molten alkali metal (Li/Na), and the formation of Ti-Li/Na, O-Li/Na, and F-Li/Na mixed covalent/ionic bonds is extremely critical for uniform electrochemical deposition. Furthermore, the porous structure in Li/Na-Ti3C2Tx-rGO composites results in an effective encapsulation, preventing dendritic growth and exhibiting stable stripping/plating behaviors up to 12 mA·cm-2 and a deeper capacity of 10 mA·h·cm-2. Stable cycling performances over 300 h (750 cycles) at 5.0 mA·cm-2 for Li-Ti3C2Tx-rGO and 500 h (750 cycles) at 3.0 mA·cm-2 for Na-Ti3C2Tx-GO are achieved. In a full cell with LiFePO4 cathodes, Li-Ti3C2Tx-rGO electrodes show low polarization and retain 96.6% capacity after 1000 cycles. These findings are based on 2D MXene materials, and the resulting 3D host provides a practical approach for achieving stable and safe alkali metal anodes.

Transition metal oxides and sulfides have been intensively investigated as host materials for the S cathode in lithium-sulfur (Li-S) batteries; however, the distinctions between them in battery operation have remained unclear. In this study, VO2 and VS2 nanosheets were systematically studied as host materials for Li-S batteries through theoretical calculations and experimental testing. First-principles calculations demonstrated that VS2 showed more favorable properties, including the inherent semi-metallic conductivity of VS2 , moderate adsorption strength for Li2 Sn , fast Li+ transport with a low diffusion barrier, and accelerated surface redox reactions with a low Li2 S decomposition barrier. In comparison, the low electronic conductivity and strong adsorption strength of VO2 increased Li+ diffusion as well as Li2 S decomposition barriers of the electrode, resulting in relatively poor rate capability and cycle stability. In experiments, the VS2 @S electrode exhibited superior electrochemical performance compared with VO2 @S, giving a large capacity of 713 mAh g-1 at 5 C and a low capacity fading rate of 0.13 % per cycle over 200 cycles at 1 C. The constructed relationships between S cathode and host materials could guide the future design of high-performance S cathodes for Li-S batteries.

A modified gel polymer electrolyte (GPE) with boron nitride (BN) additive was designed to boost the electrochemical performance of rechargeable lithium metal battery, which consists of Li-rich layered cathode and possesses a high energy density. BN, electron insulator and ion conductor, has excellent thermodynamic and electrochemical stability. BN particles were well dispersed in polyvinylidene fluoride-co-hexafluoropropylene (PVDF-HFP) polymer matrices and thus substantially enhanced the electrochemical and physical properties of the GPEs. With only 0.5 wt% BN additive, it remarkably improved the mechanical modulus and ionic conductivity (to 4.1 × 10−4 S∙cm−2) of GPEs, which was beneficial for suppressing lithium dendrite formation and fast ion transportation, respectively, thereby enabling high-performance lithium metal batteries with ultra-long cycle life and high safety at ambient temperature (25 °C) and high temperature (55 °C).

Multiple negative factors, including the poor electronic conductivity of sulfur, dissolution and shuttling of lithium polysulfides (Li2Sn), and sluggish decomposition of solid Li2S, seriously hinder practical applications of lithium-sulfur (Li-S) batteries. To solve these problems, a general strategy was proposed for enhancing the electrochemical performance of Li-S batteries using surface-functionalized Ti3C2 MXenes. Functionalized Ti3C2T2 (T = N, O, F, S, and Cl) showed metallic conductivity, as bare Ti3C2. Among all Ti3C2T2 investigated, Ti3C2S2, Ti3C2O2, and Ti3C2N2 offered moderate adsorption strength, which effectively suppressed Li2Sn dissolution and shuttling. This Ti3C2T2 exhibited effective electrocatalytic ability for Li2S decomposition. The Li2S decomposition barrier was significantly decreased from 3.390 eV to ∼0.4 eV using Ti3C2S2 and Ti3C2O2, with fast Li+ diffusivity. Based on these results, O- and S-terminated Ti3C2 were suggested as promising host materials for S cathodes. In addition, appropriate functional group vacancies could further promote anchoring and catalytic abilities of Ti3C2T2 to boost the electrochemical performance of Li-S batteries. Moreover, the advantages of a Ti3C2T2 host material could be well retained even at high S loading, suggesting the potential of surface-modified MXene for confining sulfur in Li-S battery cathodes.

Due to the high discharge voltage and a favorable theoretical capacity, Na2FePO4F have been attracted much attention as the viable cathode materials for sodium-ion storage. However, the low intrinsic electronic conductivity of Na2FePO4F suppresses its practical applications. Herein, ion doping strategy is employed to improve the electrochemical performance of Na2FePO4F as the cathode of sodium ion batteries. We first used density functional theory (DFT) calculation to screen the optimum dopants by evaluating the structural, electronic and electrochemical properties of metal-doped Na2FePO4F. Our calculation results indicate that the Co-doped Na2FePO4F is the most promising candidate for practical applications. To further prove the validity of metal doping, Na2Fe0.94Co0.06PO4F/C was synthesized by sol-gel method and showed superior electrochemical performance compared with the pristine material. The specific capacity of the Na2Fe0.94Co0.06PO4F/C is 99.93 mAh g−1 at 0.2 C and the discharge capacity retention is 62.1% after 400 cycles at 1 C.

High-performance solid-state electrolytes with healability to repair mechanical damages are important for the fabrication of Li-ion batteries (LIBs) with enhanced safety and prolonged service life. In this study, we present the fabrication of healable, highly conductive, flexible, and nonflammable ionogel electrolytes for use in LIBs by loading ionic liquids and Li salts within a hydrogen-bonded supramolecular poly(ionic liquid) copolymer network. The ionogel electrolytes exhibit ionic conductivities as high as 10

Two-dimensional (2D) metal carbides, MXene, present the promising application for the energy storage system. Among the MXene family, Ti2CTx as the lightest material, shows its unique electrochemical performance. Herein, Ti2CTx is synthesized by selective etching Al layer from the Ti2AlC. With the optimized HF treating condition, Ti2CTx displays high volumetric capacitance and remarkable rate ability. Moreover, the Ti2CTx//Ti2CTx symmetric supercapacitor is designed and assembled, which presents capable capacitance, outstanding rate performance and excellent cycling performance. The remarkable electrochemical performance is attributed to its 2D structure and high electronic conductivity. This work demonstrates the potential application of the Ti2CTx for the supercapacitors and provides a template to design high-performance supercapacitors with 2D electrode materials.

Cobalt sulfides based on conversion mechanisms are considered as promising anode materials for sodium-ion batteries due to their appropriate working voltage and high practical capacities. But the severe volume change and structure transformation make their cycle stability and rate capability unsatisfactory. In this study, metal-organic framework derived Co9S8@carbon yolk-shell nanocages (Co9S8@CYSNs) was prepared and its direct conversion mechanism was carefully demonstrated for the first time by various spectroscopic techniques and first-principles calculations. The unique hierarchical structure of Co9S8@CYSNs composed of Co9S8 nanoparticles dispersed in amorphous carbon matrix inside a rigid carbon shell was capable of accelerating the conversion reaction, shortening the Na+ diffusion distance and providing a fast electron transport channel. Benefiting from the accelerated electrochemical reactions and high activities of nanosized particles, the Co9S8@CYSNs exhibited a large discharge capacity of 549.4 mA h g-1 at 0.1 A g-1. In addition, a superior rate performance of 100 mA h g-1 at 10 A g-1 and excellent cycle stability with a very low capacity decay of 0.019% per cycle over 800 cycles at 10.0 A g-1 were achieved because of the confine effect of the carbon shell and improved charge transfer reactions of the electrode.

The insufficient charge extraction in chlorophyll-based solid-state solar cells (CSSCs) limits the photovoltaic performance, resulting in low photon-to-electron conversion efficiency. In this work, we employ poly(3-hexylthiophene) (P3HT) as a hole transporter to improve the charge extraction in CSSCs with a carboxylated chlorophyll sensitizer (H2Chl-1) adsorbed on mesoporous TiO2 as an electron acceptor and self-aggregates of a zinc chlorophyll derivative (ZnChl-2) as an electron donor. P3HT enhances the photon-to-electron conversion in both 300–540 nm and 660–725 nm wavelength regions. The charge recombination of CSSCs was suppressed by addition of P3HT to the ZnChl-2 aggregate layer that is spin-coated on H2Chl-1 adsorbed TiO2, as evidenced by the increased recombination resistance in the electrochemical impedance spectroscopy. As a result, the incident photon-to-electron conversion efficiency of the redmost peak of CSSCs with P3HT layer achieves a maximum value of 70.8%, and the power conversion efficiency is substantially enhanced from 2.1% to 3.1%.