Rechargeable Research Articles

Comparative Analysis of Graphitization Characteristics in Bamboo and Oak Charcoals for Secondary Battery Anodes

When compared to natural graphite, artificial graphite has advantages such a longer cycle life, faster charging rates, and better performance. However, the process of producing it, which frequently uses coal, raises questions about the impact on the environment and the depletion of resources. Eco-friendly, wood-based graphite must be developed in order to solve these problems. This study assessed and investigated the characteristics of charcoals derived from bamboo and oak which were utilized to produce graphite. After heating to 1500 °C at 10 K/min, 86.87 wt% of oak charcoal and 88.33 wt% of bamboo charcoal remained, indicating a yield of more than 85% when charcoal was graphitized. Depending on the species of wood, different-sized pores showed different shapes as the graphitization process advanced, as revealed by SEM surface analyses. The carbon atoms seen in the XRD crystal development changed into graphite crystals when heated to 2400 °C, and the isotropic peaks vanished. Bamboo charcoal has a higher degree of crystallinity than other wood-based charcoals, such as oak charcoal, which is made up of turbostratic graphite, according to Raman spectroscopic research. Lithium-ion batteries employ bamboo charcoal as their anode material. At this point, the values for soft carbon were determined to be 196 mAh/g and for hard carbon to be 168 mAh/g at a current density of 0.02 A/g.

Challenges and Prospects of Low-Temperature Rechargeable Batteries: Electrolytes, Interfaces, and Electrodes.

Rechargeable batteries have been indispensable for various portable devices, electric vehicles, and energy storage stations. The operation of rechargeable batteries at low temperatures has been challenging due to increasing electrolyte viscosity and rising electrode resistance, which lead to sluggish ion transfer and large voltage hysteresis. Advanced electrolyte design and feasible electrode engineering to achieve desirable performance at low temperatures are crucial for the practical application of rechargeable batteries. Herein, the failure mechanism of the batteries at low temperature is discussed in detail from atomic perspectives, and deep insights on the solvent-solvent, solvent-ion, and ion-ion interactions in the electrolytes at low temperatures are provided. The evolution of electrode interfaces is discussed in detail. The electrochemical reactions of the electrodes at low temperatures are elucidated, and the approaches to accelerate the internal ion diffusion kinetics of the electrodes are highlighted. This review aims to deepen the understanding of the working mechanism of low-temperature batteries at the atomic scale to shed light on the future development of low-temperature rechargeable batteries.

Design Double Layered Anode for Stably Introducing Lithium Source to Achieve Sulfur‐Carbon Full Batteries

AbstractLithium‐sulfur batteries offer high energy density but face great safety and cycle life challenges due to the use of Li metal anode. Replacing the Li metal anode with pre‐lithiated carbon anodes can thoroughly address cycling stability and safety issues. Directly contacting Li foil with graphite electrode is one of the most efficient and simple strategy to introduce a high content of lithium source into the sulfur‐carbon full batteries. However, the 100% lithiation of the graphite anode through the direct contact method generates excessive heat and stress heterogeneity, which leads to electrode structure cracking and electrochemical properties fading. This study implements a double‐layer anode to mitigate these issues. A thin layer of hard carbon placed between graphite and Cu foil limits heat generation and stress heterogeneity due to its structural and electrochemical stability. Additionally, differing from traditional electrochemical lithiation, this method gains better solid electrolyte interphase (SEI) for the graphite anode after several cycles. This research highlights the mass production potential of coupling high energy density lithium source‐free cathode materials with various lithium source‐free anodes for constructing long‐cycle and high‐safety rechargeable batteries.

Regulating the Spin‐State of Cobalt in Three‐Dimensional Covalent Organic Frameworks for High‐Performance Sodium‐Iodine Rechargeable Batteries

Although the catalytic activity is heavily reliant on the electronic structure of the catalyst, understanding the impact of electron spin regulation on electrocatalytic performance is still rarely investigated. This work presents a novel approach involving the single‐atom coordination of cobalt (Co) within metalloporphyrin‐based three‐dimensional covalent organic frameworks (3D‐COFs) to facilitate the catalytic conversion for sodium‐iodine batteries. The spin state of Co is modulated by altering the oxidation state of the porphyrin‐centered Co, achieving optimal catalysis for iodine reduction. Experimental results demonstrate that CoII and CoIII are incorporated into the 3D‐COFs, exhibiting spin ground states of S = 1/2 and S = 0, respectively. The low spin state of CoIII is favorable to hybridize with the sp 3d orbitals of I3‐, thus facilitating the conversion of I3‐ to I‐. Density‐functional theory (DFT) calculations further reveal that the presence of CoIII enhances iodide adsorption and accelerates the formation of NaI in 3D‐COFs‐CoIII, thereby promoting its rapid kinetic behaviors. Notably, the I2@3D‐COFs‐CoIII cathode achieves a high reversible capacity of 227.7 mAh g‐1 after 200 cycles at 0.5 C and demonstrates exceptional cyclic stability, exceeding 2000 cycles at 10 C with a minor capacity fading rate of less than one 0.01% per cycle.

Testing the Stability of NASICON Solid Electrolyte in Seawater Batteries

Rechargeable batteries play a crucial role in the utilization of renewable energy sources. Energy storage systems (ESSs) are designed to store renewable energy efficiently for immediate use. The market for energy storage systems heavily relies on lithium-ion batteries due to their high energy density, capacity, and competitiveness. However, the increasing cost and limited availability of lithium make long-term use challenging. As an alternative to Li-ion batteries, rechargeable seawater batteries are gaining attention due to their abundant and complementary sodium ion active materials. This study focuses on the preparation and characterization of Na3.0Zr2Si2PO12- and Na3.15Zr2Si2PO12-type ceramic membranes and testing their stability in seawater batteries used as solid electrolyte. From the surface analysis, it was observed that the Na3.15Zr2Si2PO12 powder showed a specific surface area of 2.94 m2/g compared to 2.69 m2/g for the Na3.0Zr2Si2PO12 powder. The measured NASICON samples achieved ionic conductivities between 7.42 × 10−5 and 4.4 × 10−4 S/cm compared to the NASICON commercial membrane with an ionic conductivity of 3.9 × 10−4 S/cm. Battery testing involved charging/discharging at various constant current values (0.6–2.0 mA), using Pt/C as the catalyst and seawater as the catholyte.

Constructing Sulfur‐Heterocyclic Aromatic Amine Polymer with Multiple‐Redox Active Sites for Long‐Lifespan and All‐Organic Aqueous Magnesium Ion Batteries

AbstractOrganic polymer materials have attracted much attention in rechargeable aqueous magnesium ion batteries (AMIBs) due to their sustainability and structural designability. However, the ionic storage capability is hindered by their insufficient redox‐active sites, dissolvability in aqueous electrolytes, and short‐range conjugated structures, resulting in low energy density and poor cycling stability. Herein, a sulfur‐heterocyclic aromatic polyimide‐based organic polymer (PTDBS) is constructed with multiple redox‐active sites and long‐range conjugate, which is employed as active material for AMIB anode, achieving an outstanding Mg2+ storage capability. Benefitting from the introduced thioether bonds, PTDBS possesses an enhanced electronic conductivity and additional redox‐active sites for reversible Mg2+ coordination, thus ensuring high redox activity and superior electron affinity. As a result, the PTDBS electrode delivers ultrafast and stable Mg2+ storage in an MgCl2 aqueous electrolyte with a superior rate capacity of 98.6 mA h g−1 at 10.0 A g−1, and remarkable cycling stability over 7500 cycles with a capacity retention rate of 90.0%. Notably, the all‐organic aqueous full cell, realized by coupling the PTDBS anode and the polyindole cathode, achieves a high energy density and long lifespan. This work lays the foundation for the development of highly stable all‐organic electrode materials for large‐scale aqueous energy storage.

Operando Investigation of Al Plating Regimes on HOPG in [EMImCl]:AlCl3 by Electrochemical Reflection Anisotropy Spectroscopy

Rechargeable aluminium batteries show promise as next‐generation systems with a more abundant material base than lithium technology. However, the stable native oxide on top of aluminium metal electrodes leads to poor cell performance. Graphite, on the other hand, is a so far rarely investigated alternative that can be used as both the anode and cathode. Here, metallic aluminium is deposited at the anode, while AlCl4– is intercalated at the cathode. For both cases, understanding the electrode–electrolyte interface is crucial for improving the performance of the battery. In this work, we use reflection anisotropy spectroscopy to study the evolution of the interface under applied potentials. We find that the cathode exhibits an irreversible swelling of the top‐most graphite layer due to AlCl4– intercalation as well as the formation of an SEI during the first voltammetry cycle. On the anode, the electrodeposition of aluminium is initially well‐ordered. However, the evolution of the surface morphology depends on the applied potential, with island‐like growth at less cathodic potentials, and layer‐by‐layer growth at more anodic potentials. With the optical operando spectroscopy, we can follow these qualitatively different plating and stripping regimes in a time‐resolved manner.

Assessing Yield Disparities: Anticipated versus Optimal Rooftop Photovoltaic Systems and Implications for Prosumer Viability

Solar photovoltaics, especially rooftop systems also called distributed solar photovoltaics, are crucial in the ongoing energy transition. Modeling these systems is vital to understanding their role in a decentralized energy system. While ground‐mounted photovoltaic power plants are easier to model, generalizing yield profiles for rooftop systems is challenging. This study aims to estimate yield loss effects for rooftop solar photovoltaic systems compared to optimized ground‐mounted systems. Anticipated yield losses are 18% for residential, 7% for commercial, and 4% for industrial rooftop systems. The impact on residential prosumers’ viability is assessed by comparing prosumer system optimization results with and without yield losses. Results show a non‐uniform change in installed solar photovoltaic and battery capacities, with a tendency to compensate for reduced yields by increasing photovoltaic capacity by up to 20%, given favorable cost prospects by 2050. The annualized total cost of energy for prosumer households could therefore increase by up to 20% by 2050. Despite yield reductions, installing a solar photovoltaic prosumer system remains more favorable than relying entirely on‐grid electricity. This study highlights the importance of considering yield losses in rooftop solar photovoltaics and the significant role of prosumers despite identified yield losses.

A Feasible Strategy for High-Performance Aqueous Zinc-Ion Batteries: Introducing Conducting Polymer.

Aqueous zinc ion batteries (AZIBs) offer great potential for large-scale energy storage because of their high safety, low cost and acceptable energy density. However, the cycle life of AZIBs is inevitably affected by parasitic reactions and dendritic growth caused by multiple factors such as electrode, electrolyte and separator, which pose significant obstacles to the practical application of AZIBs. To address these challenges, conducting polymer (CP) based materials have gained widespread attention in the realm of rechargeable batteries due to the adjustable band gap, controllable morphology, and excellent flexibility of CPs. In particular, CPs exhibit remarkable conductivity, low dimensionality, and doping characteristics, making them highly promising for integration into the AZIB system. In this review, the problems associated with the cathode, anode, electrolyte, and separator of AZIBs are discussed, and the application of CPs for their modification is summarized. The review provides a comprehensive analysis of the action mechanisms involved in the CP modification process and offers valuable insights for the design and development of CPs that can be effectively utilized in AZIBs. Additionally, the review presents a promising outlook of this research field, aiming to further advance the application of low-cost and high-performance CPs and their composites in AZIBs.

Regulating the Spin-State of Cobalt in Three-Dimensional Covalent Organic Frameworks for High-Performance Sodium-Iodine Rechargeable Batteries.

Although the catalytic activity is heavily reliant on the electronic structure of the catalyst, understanding the impact of electron spin regulation on electrocatalytic performance is still rarely investigated. This work presents a novel approach involving the single-atom coordination of cobalt (Co) within metalloporphyrin-based three-dimensional covalent organic frameworks (3D-COFs) to facilitate the catalytic conversion for sodium-iodine batteries. The spin state of Co is modulated by altering the oxidation state of the porphyrin-centered Co, achieving optimal catalysis for iodine reduction. Experimental results demonstrate that CoII and CoIII are incorporated into the 3D-COFs, exhibiting spin ground states of S = 1/2 and S = 0, respectively. The low spin state of CoIII is favorable to hybridize with the sp 3d orbitals of I3-, thus facilitating the conversion of I3- to I-. Density-functional theory (DFT) calculations further reveal that the presence of CoIII enhances iodide adsorption and accelerates the formation of NaI in 3D-COFs-CoIII, thereby promoting its rapid kinetic behaviors. Notably, the I2@3D-COFs-CoIII cathode achieves a high reversible capacity of 227.7 mAh g-1 after 200 cycles at 0.5 C and demonstrates exceptional cyclic stability, exceeding 2000 cycles at 10 C with a minor capacity fading rate of less than one 0.01% per cycle.

Techno-financial analysis of 100 % renewable electricity for the south west region of the UK by 2050

In the UK, the transition to 100 % Renewable Energy Systems is a critical strategy in addressing climate change, aligning with the UK government's 2050 net-zero objective. This study explores the potential for such a transformation within the South West region of the UK by 2050. EnergyPLAN16.2 software was utilised for scenario modelling and the fmincon algorithm in MATLAB for optimisation analysis. The focus was on two scenarios involving hybrid renewable energy systems incorporating onshore wind, solar, offshore wind, and two energy storage systems which are lithium-ion battery energy storage and hydrogen fuel cell energy storage. The optimisation process entailed two stages: determining renewable energy configurations for cost-efficient coverage of annual electricity demand and computing the minimum energy storage capacity to ensure a constant power supply. The results suggest an optimal configuration of 4,460 MW onshore wind, 9,880 MW solar, 6,982 MW offshore wind, and 2,273,662 MWh of lithium-ion battery energy storage for 100 % hybrid renewable energy systems in the South West region of the UK in 2050. This configuration achieves the lowest annual cost of 3208 M£/year, with a balanced wholesale electricity price ranging from 4.3p/kWh to 6.6p/kWh and a levelized cost of energy of 6.44p/kWh. Furthermore, hydrogen fuel cell storage systems can be another alternative, however, the present study showed it is not economical enough compared to lithium-ion battery storage systems. This research broadens the understanding of hybrid renewable energy systems implementation in large regions, offering valuable insights for sustainable energy planning in the South West region of the UK.

Metal-organic framework-derived in situ-grown Cu2Sb@NC octahedra for high-performance stable lithium/sodium storage

Intermetallic compounds are considered a special class of alloy-type anode materials that show great potential for use in lithium/sodium-ion batteries due to their inherent advantages, such as high specific capacity and enhanced safety features. However, their practical application is often impeded by the substantial volume changes that occur during the insertion and extraction of Li+/Na+ ions, leading to capacity decay and reduced service life. To address this challenge, we developed a novel composite material comprising Cu2Sb nanoparticles encapsulated within a N-doped octahedral carbon matrix (Cu2Sb@N-C). This composite structure features a heteroatom-doped conductive network, a three-dimensional carbon framework, and finely dispersed Cu2Sb nanoparticles. Benefiting from the heteroatom-doped conductive network, three-dimensional carbon framework and ultrafine Cu2Sb nanoparticles, they not only provide a penetrating network for the fast transfer of charge carriers and improve the accessibility of ions, but also alleviate the agglomeration and volume expansion of Cu2Sb during cycling. For LIBs, the material exhibited a reversible capacity of 1001.0 mAh/g after 330 cycles at 0.2 A/g, while maintaining a substantial capacity of 565.5 mAh/g after 1000 cycles at 1.0 A/g. In the case of SIBs, the material exhibited a capacity of 375.6 mAh/g after 100 cycles at 0.2 A/g. Post-cycling electrode analyses revealed that the Cu2Sb@N-C anode material retained its structural integrity, demonstrating its ability to withstand the continuous insertion and extraction of Li+/Na+ ions. This research contributes insights into the effective design of innovative high-capacity alloy-based anode materials for advanced secondary batteries.

Rational Design of 3D Hierarchical Fe3S4 for Superior Sodium‐Ion Battery Anode Material

AbstractAmong various transition metal sulfides, iron‐based sulfides have attracted wide attention due to their abundant resources, low cost, and non‐toxicity, showing considerable research value in the field of secondary batteries. Thereinto, Fe3S4 has a high theoretical specific capacity of 785 mAh g−1. However, at present, the research related to Fe3S4 anode for sodium‐ion batteries (SIBs) is still in its infancy, and it also suffers from severe volume expansion and limited preparation. Therefore, to further boost its sodium storage potential, the Fe3S4@rGO composite with hierarchical structure and carbonaceous network is proposed in this study. Beneficial from the ingenious hierarchitectures and flexible graphene coating, the Fe3S4@rGO anode exhibits outstanding sodium storage performance, which can deliver a high capacity of 603 mAh g−1 after 1500 cycles with a superior capacity retention of 98%. The micron flower‐like structure composed of 2D nanosheets can provide sufficient active sites and promote the rapid transport of Na+. Meanwhile, the 3D interconnected graphene carbon network makes a crucial contribution to alleviating volume changes and enhancing electrical conductivity. This work reveals the application potential of Fe3S4 as an anode electrode for SIBs and provides available insights for the development of other electrode materials.

Separator‐Supported Electrode Configuration for Ultra‐High Energy Density Lithium Secondary Battery

AbstractSignificant efforts are being made to develop high‐performance battery materials, particularly active materials. However, material‐dependent strategies for increasing energy density face challenges such as raw material costs and supply limitations, reducing their versatility to some extent. In this regard, the development of efficient battery designs can be a universal approach to increasing the energy density of lithium‐ion batteries with relatively low dependence on material properties. Herein, a novel configuration of an electrode‐separator assembly is presented, where the electrode layer is directly coated on the separator, to realize lightweight lithium‐ion batteries by removing heavy current collectors. Even on the hydrophobic separator, a poly(vinyl alcohol) binder enables uniform and scalable coating of aqueous electrode slurries through molecular interactions with the separator surface. Moreover, carbon nanotubes are utilized to reinforce the electronic conduction of the electrode, providing consistent electronic pathways regardless of SEI formation. Furthermore, owing to the superior permeability of liquid electrolytes through this electrode‐separator assembly, a multilayered electrode‐separator assembly can be suggested to further increase energy density when combined with a lithium metal anode. This lithium metal battery can achieve an areal capacity of ≈30 mAh cm−2 and an enhanced energy density of over 20% compared to conventional battery configurations.

Nickel Hexacyanoferrate as Cathode for Sodium‐ion Batteries: Effects of the Synthesis Conditions on the Material Properties

The increment in the energy demand and the limited availability of materials for manufacturing large‐scale energy storage batteries based on Li‐ion chemistry has increased the study of alternative technologies, including Na‐ion batteries. The quest for superior electrochemical performances has led to the developing of new cathodes, such as Prussian blue and its analogs. Among the different members of this family of materials, KNi[Fe(CN)6] has attracted great attraction because of its low synthesis cost and excellent stability. Multiple synthesis approaches based on coprecipitation methods have been explored to optimize its capacity to intercalate sodium; however, the effects of the synthesis conditions on the structural and electrochemical properties of KNi[Fe(CN)6] remain vague. Therefore, in this work, we propose a detailed analysis of how the main synthesis parameters define the structural and electrochemical properties of KNi[Fe(CN)6].

Analysis of the interfacial reaction between Si-based anodes and electrolytes in Li-ion batteries.

To ensure optimal operation of electrochemical energy storage devices, a precise design of the interfaces formed between the electrodes and the electrolyte is essential. Si is a promising anode active material for Li-ion batteries owing to its high theoretical capacity; however, the large volume change associated with Li absorption and release hinders its practical applications. The development of high-performance storage batteries depends on the construction of an electrode-electrolyte interface that facilitates Li+ movement. To this aim, the authors have developed Si-specific interface observation methods. In this feature article, we review and discuss recent advances in the reaction behavior of Si-based anodes, particularly at the Si electrode-electrolyte interface.

EMBRYONIC FLOWER 1 regulates male reproduction by repressing the jasmonate pathway downstream transcription factor MYB26.

The evolutionarily conserved Polycomb repressive complexes (PRC) mediate genome-wide transcriptional silencing and regulate a plethora of development, as well as environmental responses in multicellular organisms. The PRC2-catalyzed trimethylation of lysine 27 on histone H3 (H3K27me3) is recognized by reader-effector modules of PRC1 to implement gene repression. Here, we report that the Arabidopsis (Arabidopsis thaliana) H3K27me3 effector EMBRYONIC FLOWER 1 (EMF1) interacts with and constrains the R2R3 DNA binding transcription factor MYB26 by a eudicot-conserved motif in the stamen. MYB26 activates the transcription of two NAC domain genes, NAC SECONDARY WALL THICKENING PROMOTING FACTOR1 (NST1) and NST2, whose encoded proteins mediate anther secondary cell thickening in jasmonate (JA)-regulated stamen maturation. In this process, the transcriptional activity of MYB26 is negatively modulated by the JAZ-PRC repressive complex to precisely regulate the expression of NST1 and NST2. Disruption of EMF1 repression stimulates MYB26, leading to the excessive transcription of the two NAC genes and male sterility. Our results reveal a novel mechanism in polycomb-mediated gene silencing and illustrate that the plant Polycomb complex regulates stamen development by preventing the hypersensitivity of JA responses in male reproduction.

Microstructure regulation of WxV1-xO2(B) nanorods with improved electrochemical properties

VO2(B) is regarded as a highly promising cathode material for secondary batteries due to its outstanding theoretical specific capacity and unique expansion tunnel structure, which facilitates reversible insertion and extraction of metal ions. Nonetheless, inherent structural instability, suboptimal ion/electron transport, and constrained capacity resulting from low redox potentials pose challenges to its wider adoption. Hence, in this paper, we proposed a strategy for synthesizing gradient concentration-doped WxV1-xO2(B) nanorods via a one-step hydrothermal method to solve the above problems. The experimental results demonstrated that as the W ion content increased, all fabricated WxV1-xO2(B) nanorods exhibited a monoclinic crystal phase along with noticeable lattice distortion. The positron annihilation lifetime spectra indicated that vacancy clusters were the predominant defect types in WxV1-xO2(B) nanorods. The synergistic effects of grain sizes and vacancy defects contributed to the superior electrochemical performance observed in the W0.01V0.99O2(B) sample. The capacitor retention reached 88.76 % at 0.10 A/g after 1000 charge/discharge cycles. These results had provided experimental foundation for improving electrochemical properties of WxV1-xO2(B) in metal ion secondary batteries.

Optimizing Aqueous Zinc-Sulfur Battery Performance via Regulating Acetonitrile Co-Solvents and Carbon Nanotube Carriers.

Rechargeable aqueous zinc-sulfur batteries (AZSBs) are gaining attention due to their high energy density, ultra-stable discharge platform, and safety. However, poor liquid/solid reaction processes at the anode and cathode reduce reaction kinetics, and the severe dissolution of polysulfides causes shuttle effects during discharge/charge cycles, hindering practical applications. Improving performance requires optimizing both the cathode and electrolyte. Herein, we design an organic-inorganic hybrid electrolyte (zinc trifluoromethanesulfonate and trace iodine monomer dissolved in an acetonitrile/water co-solvent (AN-X)) and a partially exfoliated multi-walled carbon nanotube (PECNT) hosted sulfur (S@PECNTs) cathode for AZSBs. The sulfur is highly dispersed along the PECNTs with appropriate wettability at the electrode/electrolyte interface using AN-3 as the electrolyte. Meanwhile, this electrolyte inhibits hydrogen evolution at negative potentials and promotes uniform Zn ion stripping/plating. Expressively, the AN-3-based AZSB exhibits a high discharge capacity of 1370 mAh g-1 with excellent Coulombic efficiency (79.9%), outstanding rate capability, and cycling performance. These improvements are attributed to the synergistic effect between the S@PECNTs and the AN-3 electrolyte, which reduces Rct to enhance reaction kinetics and blocks the dissolution and shuttle effect of polysulfides, ensuring a reversible reaction between zinc and sulfur.

In situ reduction-sulfurized FeS2 based on iron oxide as electrocatalyst for rechargeable Li-O2 batteries

In situ reduction-sulfurized FeS2 based on iron oxide as electrocatalyst for rechargeable Li-O2 batteries