High Discharge Capacity Research Articles

Synthesis of hierarchical porous carbon scaffold derived from red kidney bean peels for advanced Li–Se and Na–Se batteries

Incorporating selenium into high-surface-area carbon with hierarchical pores, derived from red kidney bean peels via simple carbonization/activation, yields a superior Li–Se battery cathode material. This method produces a carbon framework with 568 m2 g−1 surface area, significant pore volume, and improves the composite’s electronic conductivity and stability by mitigating volume changes and reducing lithium polyselenide dissolution. The Se@ACRKB composite, containing 45 wt% selenium, shows high discharge capacities (609.13 mAh g−1 on the 2nd cycle, maintaining 470.76 mAh g−1 after 400 cycles at 0.2 C, and 387.58 mAh g−1 over 1000 cycles at 1 C). This demonstrates exceptional long-term stability and performance, also applicable to Na–Se batteries, with 421.36 mAh g−1 capacity after 200 cycles at 0.1 C. Our study showcases the potential of using sustainable materials for advanced battery technologies, emphasizing cost-effective and scalable solutions for energy storage.

Gradient Lithium Ion Regulation Current Collectors for High-Performance and Dendrite-Free Li Metal Batteries.

Lithium metal anode has attracted wide attention due to its ultrahigh theoretical specific capacity, lowest reduction potential, and low density. However, uncontrollable dendritic growth and volume change caused by uneven Li+ deposition still seriously hinder the large-scale commercial application of lithium metal batteries, even causing serious battery explosions and other safety problems. Hence, gold nanoparticles with a gradient distribution anchored on 3D carbon fiber paper (CP) current collectors followed by the encapsulation of polydopamine (PDA) (CP/Au/PDA) are constructed for stable and dendrite-free Li metal anodes for the first time. Significantly, lithiophilic Au nanoparticles showing a gradient distribution in the carbon fiber paper could guide the transfer of Li+ from the outside to the inside of the CP/Au/PDA electrode as well as lower the nucleation overpotential of Li, thereby obtaining the uniform Li deposition. Meanwhile, the PDA layer could in situ be converted to Li-PDA which could serve as an efficient Li+ conductor to further facilitate uniform Li+ transport among the whole CP/Au/PDA electrode. Besides, 3D carbon fiber paper could effectively accommodate the volume change during the plating/stripping process of Li metal. As a result, CP/Au/PDA electrodes deliver a low nucleation overpotential (∼9 mV) and a high Coulombic efficiency (mean value of ∼98.8%) at a current density of 1 mA cm-2 with the capacity of 1 mA h cm-2. Furthermore, Li@CP/Au/PDA electrodes also can demonstrate an ultralow voltage hysteresis (∼20 mV) and a long cycle life (1000 h) in symmetric cells. Finally, with LiFePO4 (LFP) as the cathode, the Li@CP/Au/PDA-LFP full cell delivers a high discharge capacity of 136 mA h g-1 even after 350 cycles at 1C, exhibiting a per cycle loss as low as 0.01%. This gradient lithium ion regulation current collector is of great significance for the development of lithium metal anodes.

Incorporation of electronically and ionically conductive additives in high-loading sulfur cathodes in lean-electrolyte lithium–sulfur cells

Low-cost, high-energy-density lithium–sulfur electrochemical batteries have emerged as a promising solution for next-generation energy-storage technologies. To facilitate the practical application of such batteries, it is necessary to address the remaining scientific and engineering challenges, especially those associated with the high-loading sulfur cathode in a lean-electrolyte cell. In this study, we investigate the electrochemical and overall performance of lithium–sulfur cells with a high-loading sulfur cathode. Notably, this cathode is fabricated using a novel hot-pressing method and incorporates electronically and ionically conductive additives, specifically lithium lanthanum titanate (LLTO) and carbon black, respectively. Material analysis reveals the uniform distribution of additives in the cathodes, with the ionically conductive LLTO effectively adsorbing and converting polysulfides and carbon black enhancing the cathode conductivity. Electrochemical analysis of the lean-electrolyte cells shows that the incorporation of LLTO improves cell performance, with enhanced discharge capacity of 715–836 mAh g−1 at C/5–C/10 rates and notable capacity retention after 100 cycles, compared with cathodes without additives or with carbon black. Further investigations demonstrate the superior performance of the cell incorporating LLTO in a LiNO3-free electrolyte, attributable to the promotion of ion transport and polysulfide adsorption by LLTO, resulting in high discharge capacities (846 mAh g−1 at C/10), efficiency (93–99 %), and stability. Overall, this study compares the effects of electronically and ionically conductive additives on cell performance and highlights the effectiveness of the ionically conductive LLTO. The incorporation of such additives offers innovative solutions to the key challenges for the development of high-performance energy-storage devices.

Empowering Low-Temperature Lithium-Sulfur Batteries: Unlocking the Potential of Transition Metal Alloy-Based Cathode Materials.

At low temperatures, lithium-sulfur (Li-S) batteries have poor kinetics, resulting in extreme polarization and decreased capacity. In this study, we investigated the electrochemical performance of Li-S batteries utilizing transition metal alloy-based cathode materials. Specifically, binary transition metal alloys (FeNi, FeCo, and NiCo) are integrated into a porous carbon nanofiber (CNF) matrix as composite cathode material. Our findings reveal that alloying metallic Ni with Fe in the FeNi@CNFs composite enhances the catalytic conversion of sulfur species, mitigating the shuttle effect and improving battery performance even under low temperatures. Li-S batteries employing a Li2S6/FeNi@CNFs cathode exhibited a significantly high initial discharge capacity of 1655 mAh g-1 at 0.1 C. Even at the higher current density of 10 C, the Li2S6/FeNi@CNFs composite can still reach an ultrahigh specific capacity of 828 mAh g-1. In addition, Li2S6/FeNi@CNFs demonstrated exceptional initial discharge capacities of 890.5 and 382.7 mAh g-1 at 0.1 C under -20 and -40 °C, respectively. With an initial capacity of 392.02 mAh g-1 and a capacity retention rate of 88.86% (after 60 cycles) at 0.2 C, the conversion of LiPSs in Li2S6/FeNi@CNFs is significantly enhanced even at ultralow temperatures of -40 °C. The findings of this study hold significant implications for the advancement of extremely low-temperature Li-S batteries.

An Electron-Coupled Co-ZrO2 Nanodot Heterojunction Electrocatalyst with Lewis Acid-Base Site Pairs Enables High Redox Reaction Kinetics of Li-S Batteries.

Using electrocatalysts is effective in solving the slow reaction kinetics of polysulfides in Li-S batteries, but designing stable electrocatalysts with an integrated adsorption-catalysis-desorption system is challenging. Here, we report a stable metal-semiconductor (Co-ZrO2) heterojunction electrocatalyst fabricated by assembling electron-coupled Co-ZrO2 nanodots into macroporous carbon nanofibers. The Co-ZrO2 contact causes interfacial electron enrichment and electron transfer from Co to ZrO2, which creates abundant Lewis-acid sites on Co that can adsorb polysulfides. Simultaneously, the enriched interfacial electrons can activate the S-S bond and boost the catalytic conversion of long-chain polysulfides, while the ZrO2 with Lewis-base sites facilitate the desorption of short-chain polysulfides from the electrocatalyst. Moreover, the nanodot heterojunctions show great chemical stability and high redox reaction kinetics of polysulfides. Li-S batteries show high discharge capacities of 954.5 mA h·g-1 at 0.5 C with a retention of 84.9% over 200 cycles, and 710.2 mA hg-1 at 1 C with a retention of 98.6% over 200 cycles. This study provides an effective strategy for developing active and durable electrocatalysts for Li-S batteries.

Organic montmorillonite modified polyethylene oxide based polymer electrolyte for dendrite-free flexible solid-state lithium metal batteries

Polyethylene oxide (PEO) based solid-state electrolytes are known for the low manufacturing cost and excellent processability, but their practical application is paved with thorns including the inferior ionic conductivity, low Li+ transfer number and insufficient Li dendrite blocking ability. Herein, we propose organic montmorillonite (OMMT) with expanded layer spacing (1.97 nm) as versatile fillers to construct PEO-OMMT electrolyte, in which OMMT not only increases Li+ transfer number (0.56) and ionic conductivity (7.15 × 10−4 S cm−1), providing fast ionic transport channels, but also endows PEO with high mechanical strength, resulting remarkable Li dendrite blocking ability (>2100 h). Additionally, the high dielectric constant and Lewis-rich polar sites of OMMT facilitate the dissociation of lithium salts and the rapid formation of LiF and Li3N-rich solid electrolyte interface layers. Impressively, the LiFePO4|PEO-OMMT|Li cell shows a high initial capacity (154.4 mAh g−1 at 0.5C) with ultralong cycling lifespan (>1200 cycles). Similarly, the LiNi0.83Mn0.05Co0.12O2|PEO-OMMT|Li cell retains a high discharge capacity of 151.5 mAh g−1 after 100 cycles at 0.2C. This work highlights the indelible contributions of OMMT functionalized fillers in improving the interfacial stability of PEO based solid-state electrolytes, paving a feasible avenue for the practical application of solid-state lithium metal batteries.

Enhancing the electrochemical properties of Li-rich layered oxide cathodes by a facile Fe/Ti integrated modification strategy

Li-rich layered oxide cathodes have gained much attention due to their high specific capacity, high operating voltage, and environmental friendliness. However, poor rate performance, rapid capacity and voltage decay during cycling have hindered its commercial application. In this work, a Fe/Ti integrated modification strategy is proposed to construct a LiFeTiO4 spinel phase coating on the surface of Li1.2Mn0.54Ni0.13Co0.13O2, effectively reducing interfacial side reactions and suppressing the irreversible oxygen release, while doping with Fe3+ and Ti4+ ions can effectively broaden the lithium diffusion channel and enhance the structural stability. As a result, the modified sample with 2 wt% of Fe/Ti demonstrates excellent cycling stability with a superior capacity retention of 91% after 400 cycles at 1C and good rate performance with a high specific discharge capacity of 216 mAh g−1 at 2C. Moreover, the initial Coulombic efficiency of the modified sample is also improved. This integrated modification strategy offers a new design to promote the large-scale application of Li-rich Mn-based cathode materials.

A sulfur-infiltrated mesoporous silica/CNT composite-based functional interlayer for enhanced Li–S battery performance

The design and construction of functional interlayers for lithium–sulfur (Li–S) batteries has attracted much attention and was demonstrated to be effective to alleviate the notorious “shuttle effect.” An often neglected issue is that the introduction of interlayer will reduce the overall energy density of the battery. In this work, we report a sulfur-infiltrated mesoporous silica/carbon nanotube (CNT) composite as an interlayer for Li–S batteries. The mesoporous silica with large surface area (842 m2 g−1) and pore volume (0.85 cm3 g−1) can not only ensure abundant exposed sites for polysulfide capture but also accommodate a large amount of sulfur inside the pore structure. CNT was composited with silica to enhance the electronic conductivity of the interlayer, which is beneficial for fast sulfur redox reaction kinetics and improved utilization of sulfur. Compared to the pristine and CNT-modified separator, the mesoporous silica/CNT composite-modified separator enables better cycling stability and rate performance. More importantly, it was demonstrated that separately incorporating sulfur into a cathode and interlayer enables better battery performance than locating all the sulfur in the cathode. At a total sulfur loading of 4 mg cm−2 (3 mg cm−2 sulfur on the cathode and 1 mg cm−2 on the mesoporous silica/CNT interlayer), a high initial discharge capacity of 1410 mAh g−1 and a retained capacity of 952 mAh g−1 after 100 cycles were exhibited. This work provides important guidance for future design of functional interlayers for practical Li–S batteries.

Amorphous titanium dioxide and polyaniline dual modifying silicon for highly enhanced lithium-ion storage

Silicon (Si) anode material is promising in the next generation of lithium-ion batteries (LIBs) with high energy densities for its much higher capacity (4200 mAh/g) than that of commercial graphite (372 mAh/g). However, silicon anode material with low electronic conductivity suffers a huge volume variation and accompanies side reactions during alloyed and de-alloyed process. Here, we design an inner amorphous titanium dioxide (TiO2) and an outer flexible conductive polyaniline (PANI) network dual modified Si@TiO2@PANI material for LIBs, where the TiO2 avoids the side reactions and the PANI network layer buffers the volume expansion and increases the electronic conductivity. The as-prepared Si@TiO2@PANI exhibits a high initial discharge capacity of 3050 mAh/g and maintains 1583 mAh/g after 200 cycles at 0.5 A/g. It even delivers the discharge capacity of 1002 mAh/g after 600 cycles at 1 A/g, as well as an excellent rate ability with discharge capacity of 1890, 1260 and 432 mAh/g at the high current density of 1, 2 and 5 A/g, respectively. Our strategy shows that the innovative design of double buffer layers on Si can synergistically promote stability and accelerate kinetics of Li+ transport, offering novel resolution strategy to enhance the performance of Si-based anodes for LIBs.

Cu-substituted Na0.75Ni0.17Cu0.08Mn0.75O2 cathode with suppressing P2-O2 phase transition and air-stable for high-performance sodium-ion batteries

P2-Na0.75Ni0.25Mn0.75O2 cathode material with high specific capacity and high operating voltage is favored by researchers. However, the complex phase transition (P2-O2) at high voltage and the rapid capacity decay caused by Na+/vacancy ordering seriously restrict its application. In this study, a series of Cu-substituted P2-type Na0.75Ni0.25-xCuxMn0.75O2 (x = 0, 0.02, 0.04, 0.06, 0.08, 0.1) cathodes are synthesized. The Na0.75Ni0.17Cu0.08Mn0.75O2 cathode achieves a high initial discharge capacity of 133.6 mAh g−1 and remains 80.5 % of this capacity after 150 cycles at 0.1C, outperforming the performance of other compositions. Investigations into the superior electrochemical performance of Na0.75Ni0.17Cu0.08Mn0.75O2 through a multi-technique approach, including in-situ X-ray diffraction (XRD), ex-situ X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT), elucidate the underlying mechanisms. The results show that the introduction of Cu2+ in Na0.75Ni0.25Mn0.75O2 can successfully regulate the ratio of Naf/Nae, with enhanced cell performance when Na+ occupies more Nae sites compared to Naf sites. In-situ XRD confirms that the Cu substitution for Ni stabilizes the P2 structure during the charge–discharge process and inhibits the unfavorable P2-O2 phase transition at high voltage. In addition, Cu-substituted cathode materials exhibit a good effect on improving air stability, attributed to the higher Cu2+/Cu3+ redox potential. This unique substitution mechanism offers a novel perspective for understanding the structure-performance relationship of P2-type cathode materials and provides important support for the design of air-stable, high-performance cathode materials.

Synthesis of MoS2/Co9S8@CoNC by impregnation and calcination for highly efficient lithium-O2 batteries

The activity of electro-catalyst on oxygen cathode is a key factor affecting the property of lithium-O2 batteries (LOBs). In this work, zeolitic imidazolate framework (ZIF–67) was impregnated in (NH4)2MoS4 solution, and then through centrifugation and calcination, nano-MoS2 and Co9S8 were grown on the surface of CoNC skeleton. The composite has mesoporous structure and abundant active groups such as Co, Co9S8, Co-N bond, Mo-N bond and active edges of MoS2 with sulfur vacancies. The coating of ultra-thin MoS2 nanosheets can improve the stability of CoNC skeleton. The Mo component induces the transformation of amorphous carbon of CoNC to graphitic carbon during calcination in order to improve conductivity of the composite. This study shows that MoS2/Co9S8@CoNC is good electro-catalyst for O2 reduction and evolution reactions (ORR/OER). The LOBs with MoS2/Co9S8@CoNC oxygen cathode show high specific discharge capacity (18162 mA h g−1) and good cycle performance (304 cycles).

Structure engineering with sodium doping for cobalt-free Li-rich layered oxide toward improving electrochemical stability

Structure engineering of the Li-rich layered cathodes to overcome insufficient structural stability and the rapid decay of capacity and voltage is crucial for commercializing of the materials for the lithium-ion batteries. Alkali metal element doping at the lithium sites has proven to be a feasible approach to boost the performance of the Li-rich layered oxides. Herein, the Na+-doping strategy in the lithium slabs is introduced to modify the structure of the cobalt-free layered Li-rich oxide, Li1.2Ni0.2Mn0.6O2. It is revealed that the doped Na+ ions can promote the activation of the Li2MnO3 phase, endowing the materials with high initial discharge capacity of 284.2 mAh g−1 at 0.1C. Due to the pillaring effect of the doped Na+ ions in the lithium slabs and the induced formation of oxygen vacancies, the electrochemical stability of the material is significantly improved, providing a capacity retention of 94.0 % after 100 cycles at 0.5C. The voltage decay per cycle is only 2.0 mV, less than 3.2 mV of the Li1.2Ni0.2Mn0.6O2. The results suggest that the facile strategy of introducing Na+ ions into the lithium slabs is an efficient approach for optimizing structure design of the Li-rich layered oxides for the lithium-ion batteries.

Elevating Discharge Voltage of Li2CO3-Routine Li-CO2 Battery over 2.9 V at an Ultra-Wide Temperature Window.

The Li-CO2 batteries utilizing greenhouse gas CO2 possess advantages of high energy density and environmental friendliness. However, these batteries following Li2CO3-product route typically exhibit low work voltage (<2.5 V) and energy efficiency. Herein, we have demonstrated for the first time that cobalt phthalocyanine (CoPc) as homogeneous catalyst can elevate the work plateau towards 2.98 V, which is higher than its theoretical discharge voltage without changing the Li2CO3-product route. This unprecedented discharge voltage is illustrated by mass spectrum and electrochemical analyses that CoPc has powerful adsorption capability with CO2 (-7.484 kJ mol-1) and forms discharge intermediate of C33H16CoN8O2. Besides high discharge capacity of 18724 mAh g-1 and robust cyclability over 1600 hours (1000 mAh g-1 cut-off) at a current density of 100 mA g-1, the batteries show high temperature adaptability (-30-80 °C). Our work is paving a promising avenue for the progress of high-efficiency Li-CO2 batteries.

Elevating Discharge Voltage of Li2CO3‐Routine Li−CO2 Battery over 2.9 V at an Ultra‐Wide Temperature Window

AbstractThe Li−CO2 batteries utilizing greenhouse gas CO2 possess advantages of high energy density and environmental friendliness. However, these batteries following Li2CO3‐product route typically exhibit low work voltage (&lt;2.5 V) and energy efficiency. Herein, we have demonstrated for the first time that cobalt phthalocyanine (CoPc) as homogeneous catalyst can elevate the work plateau towards 2.98 V, which is higher than its theoretical discharge voltage without changing the Li2CO3‐product route. This unprecedented discharge voltage is illustrated by mass spectrum and electrochemical analyses that CoPc has powerful adsorption capability with CO2 (−7.484 kJ mol−1) and forms discharge intermediate of C33H16CoN8O2. Besides high discharge capacity of 18724 mAh g−1 and robust cyclability over 1600 hours (1000 mAh g−1 cut‐off) at a current density of 100 mA g−1, the batteries show high temperature adaptability (−30–80 °C). Our work is paving a promising avenue for the progress of high‐efficiency Li−CO2 batteries.

Rationally Designed Li-Ag Alloy with In-Situ-Formed Solid Electrolyte Interphase for All-Solid-State Lithium Batteries.

All-solid-state lithium batteries (ASSLBs) with sulfide-based solid electrolytes have attracted significant attention as promising energy storage devices, owing to their high energy density and enhanced safety. However, the combination of a lithium metal anode and a sulfide solid electrolyte results in performance degradation, owing to lithium dendrite growth and the side reactions of lithium metal with the solid electrolyte. To address these issues, a Ag-based Li alloy with a favorable solid electrolyte interphase (SEI) was prepared using electrodeposition and applied to the ASSLB as an anode. The electrochemically formed SEI layer on the Li-Ag alloy primarily comprised LiF and Li2O with high mechanical strength and Li3N with high ionic conductivity, which suppressed the formation of lithium dendrites and short-circuiting of the cell. The symmetric cell with the Li-Ag alloy achieved a critical current density of 1.6 mA cm-2 and maintained stable cycling for over 2000 h at a current density of 0.6 mA cm-2. Consequently, the all-solid-state lithium cell assembled with the Li-Ag alloy anode with SEI, Li6PS5Cl solid electrolyte, and LiNi0.78Co0.10Mn0.12O2 cathode delivered a high discharge capacity of 185 mAh g-1 and exhibited good cycling performance in terms of cycling stability and rate capability at 25 °C.

MXene Supported Electrodeposition Engineering of Layer Double Hydroxide for Alkaline Zinc Batteries.

The main challenges faced by aqueous rechargeable nickel-zinc batteries are their comparatively low energy density and poor cycling stability, mainly due to the limited capacity and reversibility of existing Ni-based cathodes. Moreover, the preparation procedures of these cathodes are complex and not easily scalable, which makes them less promising for large-scale energy storage. Herein, we utilized MXene as a functional additive to effectively improve the electrodeposition preparation of NiCo layered double hydroxides (LDH). Benefiting from the improved interfacial contact between nickel foam (NF) and platting solution and the enhanced ionic conductivity of platting product based on MXene additives, the resulting binder-free NiCo LDH electrode can achieve ultrahigh areal loading (~65 mg cm-2) with abundant active surface for redox reactions and maintained short transport pathway for ion diffusion and charge transfer. Furthermore, the as-fabricated alkaline NiCo LDH-based battery delivers high discharge capacity, up to 20.2 mAh cm-2 (311 mAh g-1), accompanied by remarkable rate performance (9.6 mAh cm-2 or 148 mAh g-1 at 120 mA cm-2). Due to the high structural and chemical stability of MXenes/LDH-based electrode, excellent cycling life can also be achieved with 88.6 % capacity retention after 10000 cycles. In addition, ultrahigh areal energy density (31.2 mWh cm-2) and gravimetric energy density (465 Wh kg-1) can be simultaneously achieved. This work has inspired the design of advanced cathode materials to develop high-performance aqueous zinc batteries.

The Impact of Oxygen Content in O-Doped MoS2 on the Kinetics of Polysulfide Conversion in Li-S Batteries.

Polysulfide shuttle and sluggish sulfur redox kinetics remain key challenges in lithium-sulfur batteries. Previous researches have shown that introducing oxygen into transition metal sulfides helps to capture polysulfides and enhance their conversion kinetics. Based on this, further investigations are conducted to explore the impact of oxygen doping levels on the physical-chemical properties and electrocatalytic performance of MoS2. The findings reveal that MoS2 doped with high-content oxygen exhibits enhanced conductivity and polysulfides conversion kinetics compared to MoS2 with low-content oxygen doping, which can be attributed to the alteration of crystal structure from 2H-phase to the 1T-phase, the introduction of increased Li-O interactions, and the effect of defects resulting from high-oxygen doping. Consequently, the lithium-sulfur batteries using high-oxygen doped MoS2 as a catalyst deliver a high discharge capacity of 1015 mAh g-1 at 0.25C and maintain 78.5% capacity after 300 more cycles. Specifically, lithium-sulfur batteries employing paper-based electrodedemonstrate an areal capacity of 3.91 mAh cm-2 at 0.15C, even with sulfur loading of 4.1mg cm-2 and electrolyte of 6.7µL mg-1. These results indicate that oxygen doping levels can modify the properties of MoS2, and high-oxygen doped MoS2 shows promise as an efficient catalyst for lithium-sulfur batteries.

Self-assembled 3D CoSe-based sulfur host enables high-efficient and durable electrocatalytic conversion of polysulfides for flexible lithium-sulfur batteries

Lithium-sulfur (Li-S) batteries are considered as promising candidates for next-generation energy storage systems. However, the commercial applications are severely limited by the sluggish kinetics and shuttling effect. Herein, we have designed an integrated free-standing functional CoSe-CNF-GO-MXene (CCGM) sulfur host with a “point-line-plane” 3D porous structure for Li-S batteries. The two-dimensional (2D) graphene, MXene and one-dimensional (1D) nanocellulose fibers combined with zero-dimensional (0D) transition metal selenide (CoSe) shows good electrical conductivity and enhanced catalytic performance, respectively. Additionally, the rationally designed porous structure (from 0D to 3D) demonstrates well-connected ion/electron transport channels, conferring the good kinetic performance. Electrochemical tests show that CoSe catalytic materials with moderate adsorption energies can catalyse both precipitation and dissolution processes of Li2S, enabling fast conversion kinetics. The density functional theory (DFT) calculations show that the synergistic effect of CoSe, Ti3C2Tx, and graphene can improve the chemisorption and catalytic performance. As a result, the 3D porous S@CCGM cathode exhibits a high initial discharge capacity of 1205.1 mAh g−1 at 0.2C and good long-term cycling performance with a low decay rate of 0.055 % per cycle at 1C. Furthermore, the gel electrolyte Li-S pouch cell successfully passes the 0–180° bending test, nailing test, and cutting test. Such design offers a new perspective for the commercialization of safe and flexible electrochemical energy-storage devices especially in Li-S batteries.

Ammonium vanadate doped by transition bivalent metal ions for high-performance zinc-ion batteries

Vanadium-based materials are considered as promising cathode materials in aqueous zinc-ion (Zn2+) batteries (AZIBs) because of their abundant valence states and adjustable ion diffusion channels. However, the slow kinetics of the Zn2+ intercalation and the instability of the layered structure during long cycle are the bottlenecks restricting their further development. In this paper, the transition bivalent manganese ions (Mn2+) are introduced into ammonium vanadate (NH4V4O10) to partly replace the NH4+ ions to prepare a high-performance AZIB cathode. After doping transition bivalent Mn2+, the interlayer spacing of NH4V4O10 is enlarged, providing a broadened channel for the diffusion of Zn2+ accordingly. The results reveal that the electrode with the optimal doping quantity has a very high discharge capacity (539.4 mAh/g at 0.2 A/g) and excellent cyclic stability (85.3 % retention of the initial capacity after 3000 cycles at 5 A/g). A highly competitive energy density of 378 Wh kg−1 at 362 W kg−1 is delivered by the corresponding AZIB. Moreover, this method is a general and effective strategy for developing high-performance AZIB cathode materials, as demonstrated by the consistent crystal structure and stable cycling properties for NH4V4O10 doped with other transition bivalent metal cations.

Hollow and Porous N‐Doped Carbon Framework as Lithium‐Sulfur Battery Interlayer for Accelerating Polysulfide Redox Kinetics

AbstractLithium‐sulfur batteries (LSBs) have become one of the most powerful candidates for next‐generation battery technologies due to their high theoretical energy density and low cost. However, the notorious shuttle effect of soluble lithium polysulfides (LiPSs) and sluggish conversion reaction kinetics cause low sulfur utilization and inferior cycle life. Rational catalyst design on hierarchical pore structures and composition optimization is highly desired to realize synergetic enrichment, accommodation, and catalytic redox capacity of sulfur species. In this consideration, the hollow and porous N‐doped carbon framework is prepared, in which Co nanoparticles (NPs) are evenly embedded (denoted as Co‐HMCF) to modulate electron cloud density of carbons. Electrochemical tests and density functional theory (DFT) calculations demonstrate that Co‐HMCF could simultaneously deliver superior catalytic activity in accelerating LiPSs conversion as well as Li2S nucleation/decomposition to improve overall sulfur redox kinetics. Consequently, the Co‐HMCF interlayer significantly improves the battery performance, including high discharge capacity output (1538 mAh g−1 at 0.2 C), stable long‐term cycle (0.047% capacity decay per cycle for 800 cycles at 1.0 C), and exceptional rate capacity (582 mAh g−1 at 5.0 C).