Iron selenides with high capacity and excellent chemical properties have been considered as outstanding anodes for alkali metal-ion batteries. However, its further development is hindered by sluggish kinetics and fading capacity caused by volume expansion. Herein, a series of FeSe2 nanoparticles (NPs)-encapsulated carbon composites were successfully synthesized by tailoring the amount of Fe species through facile plasma engineering and followed by a simple selenization transformation process. Such a stable structure can effectively mitigate volume changes and accelerate kinetics, leading to excellent electrochemical performance. The optimized electrode ( FeSe2@C2) exhibits outstanding reversible capacity of 853.1 mAh g− 1 after 150 cycles and exceptional rate capacity of 444.9 mAh g− 1 at 5.0 A g− 1 for Li+ storage. In Na+ batteries, it possesses a relatively high capacity of 433.7 mAh g− 1 at 0.1 A g− 1 as well as good cycle stability. The plasma-engineered FeSe2@ C2 composite, which profits from synergistic effect of small FeSe2 NPs and carbon framework with large specific surface area, exhibits remarkable ions/electrons transportation abilities during various kinetic analyses and unveils the energy storage mechanism dominated by surface-mediated capacitive behavior. This novel cost-efficient synthesis strategy might offer valuable guidance for developing transition metal-based composites towards energy storage materials.

Si-based anodes are promising alternatives to graphite owing to their high capacities. However, their practical application is hindered by severe volume expansion during cycling. Herein, we propose employing a carbon support to address this challenge and utilize Si-based anode materials for lithium-ion batteries (LIBs). Specifically, carbon supports with various pore structures were prepared through KOH and NaOH activation of the pitch. In addition, Si was deposited into the carbon support pores via SiH4 chemical vapor deposition (CVD), and to enhance the conductivity and mechanical stability, a carbon coating was applied via CH4 CVD. The electrochemical performance of the C/Si/C composites was assessed, providing insights into their capacity retention rates, cycling stability, rate capability, and lithium-ion diffusion coefficients. Notably, the macrostructure of the carbon support differed significantly depending on the activation agent used. More importantly, the macrostructure of the carbon support significantly affected the Si deposition behavior and enhanced the stability by mitigating the volume expansion of the Si particles. This study elucidated the crucial role of the macrostructure of carbon supports in optimizing Si-based anode materials for LIBs, providing valuable guidance for the design and development of high-performance energy-storage systems.

In this study, carbon coating was carried out by physical vapor deposition (PVD) on SiOx surfaces to investigate the effect of the deposited carbon layer on the performance of lithium-ion batteries as a function of the asphaltene content of petroleum residues. The petroleum residue was separated into asphaltene-free petroleum residue (ASF) and asphaltene-based petroleum residue (AS) containing 12.54% asphaltene by a solvent extraction method, and the components were analyzed. The deposited carbon coating layer became thinner, with the thickness decreasing from 15.4 to 8.1 nm, as the asphaltene content of the petroleum residue increased, and a highly crystalline layer was obtained. In particular, the SiOx electrode carbon-coated with AS exhibited excellent cycling performance with an initial efficiency of 85.5% and a capacity retention rate of 94.1% after 100 cycles at a current density of 1.0 C. This is because the carbon layer with enhanced crystallinity had sufficient thickness to alleviate the volume expansion of SiOx, resulting in stable SEI layer formation and enhanced structural stability. In addition, the SiOx electrode exhibited the lowest resistance with a low impedance of 23.35 Ω, attributed to the crystalline carbon layer that enhanced electrical conductivity and the mobility of Li ions. This study demonstrated that increasing the asphaltene content of petroleum residues is the simplest strategy for preparing SiOx@C anode materials with thin, crystalline carbon layers and excellent electrochemical performance with high efficiency and high rate performance.

In this study, ester co-solvents and fluoroethylene carbonate (FEC) were used as low-temperature electrolyte additives to improve the formation of the solid electrolyte interface (SEI) on graphite anodes in lithium-ion batteries (LIBs). Four ester co-solvents, namely methyl acetate (MA), ethyl acetate, methyl propionate, and ethyl propionate, were mixed with 1.0 M LiPF6 ethylene carbonate:diethyl carbonate:dimethyl carbonate (1:1:1 by vol%) as the base electrolyte (BE). Different concentrations were used to compare the electrochemical performance of the LiCoO2/ graphite full cells. Among various ester co-solvents, the cell employing BE mixed with 30 vol% MA (BE/MA30) achieved the highest discharge capacity at − 20 °C. In contrast, mixing esters with low-molecular-weight degraded the cell performance owing to the unstable SEI formation on the graphite anodes. Therefore, FEC was added to BE/MA30 (BE/MA30-FEC5) to form a stable SEI layer on the graphite anode surface. The LiCoO2/ graphite cell using BE/MA30-FEC5 exhibited an excellent capacity of 127.3 mAh g− 1 at − 20 °C with a capacity retention of 80.6% after 100 cycles owing to the synergistic effect of MA and formation of a stable and uniform inorganic SEI layer by FEC decomposition reaction. The low-temperature electrolyte designed in this study may provide new guidelines for resolving low-temperature issues related to LIBs, graphite anodes, and SEI layers.

With the emergence of the new energy field, the demand for high-performance lithium-ion batteries (LIBs) and green energy storage devices is growing with each passing day. Carbon nanotubes (CNTs) exhibit tremendous potential in application due to superior electrical and mechanical properties, and the excellent lithium insertion properties make it possible to be LIBs anode materials. Based on the lithium insertion mechanism of CNTs, this paper systematically and categorically reviewed the design strategies of CNTs-based composites as LIBs anode materials, and summarized in detail the enhancement effect of CNTs fillers on various anode materials. More importantly, the superiorities and limitations of various anode materials for LIBs were evaluated. Finally, the research direction and current challenges of the industrial application of CNTs in LIBs were prospected.

Silicon-based anode materials have attracted significant interest because of their advantages, including high theoretical specific capacity (~4,200 mAh/g), low working potential (0.4 V vs Li/Li+), and abundant sources. However, their significant initial capacity loss and large volume changes during cycling impede the application of silicon-based anodes in lithium-ion batteries. In this work, we propose a silicon oxide (SiOx) anode material for lithium-ion batteries produced with a magnesio-thermic reduction (MTR) process adopting Boryeong mud as a starting material. Boryeong mud contains various minerals such as clinochlore [(Mg,Fe)6(Si,Al)4O10(OH)8], anorthite (CaAl2Si2O8), illite [K0.7Al2(Si,Al)4O10(OH)2], and quartz (SiO2). The MTR process with Boryeong mud generates a mixture of amorphous silicon oxides (SiOx and SiO2), and magnesium aluminate which helps to alleviate the volume expansion of the electrode during charge/discharge. To observe the effects of these oxides, we conducted various analyses including X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier-Transformation infrared spectroscopy (FT-IR), Brunauer-Emmett-Teller (BET) and cyclic voltammetry (CV) galvanic cell testing. The amorphous SiO2 and MgAl2O4 suppressed the volume expansion of the silicon-based anode, and excellent cycle performance was achieved as a result.

탄소중립을 달성하기 위해 이산화탄소를 포집, 활용, 저장하는 CCUS (carbon capture, utilization, and storage) 기 술이 주목받고 있다. 본 연구에서는 광물 탄산화 공정을 통해 이산화탄소를 탄산염으로 고정하고, 이를 전이금속 탄산염 기반 리튬이온배터리 (LIB) 음극재로 적용하였다. CO2를 탄산염으로 고정후, 이를 이용해 FeCO3를 제작하고, rGO와 PVP와 복합 화하여 음극활물질에 적용하였다. rGO는 전기전도도를 높이고 입자의 응집을 방지해 부피 팽창을 완화했으며, PVP는 계면 활성제로서 입자 표면을 안정화하여 구조적 안정성을 강화하였다. FeCO3-PVP-rGO 복합체 기반한 음극재에 대한 전기화학 테스트를 진행한 결과, FeCO3/rGO 복합체는 1,620 mA/g의 전류 밀도에서 50 사이클 이후에도 400 mAh/g의 용량을 유지하 였다. 본 연구는 CO2를 고부가가치 배터리 소재로 전환하여 차세대 에너지 저장 기술에 기여할 가능성을 시사한다.

All-solid-state lithium batteries (ASSLBs) are receiving attention as a prospective next-generation secondary battery technology that can reduce the risk of commercial lithium-ion batteries by replacing flammable organic liquid electrolytes with non-flammable solid electrolytes. The practical application of ASSLBs requires developing robust solid electrolytes that possess ionic conductivity at room temperature on a par with that of organic liquids. These solid electrolytes must also be thermally and chemically stable, as well as compatible with electrode materials. Inorganic solid electrolytes, including oxide and sulfide-based compounds, are being studied as promising future candidates for ASSLBs due to their higher ionic conductivity and thermal stability than polymer electrolytes. Here, we present the challenges currently facing the development of oxide and sulfide-based solid electrolytes, as well as the research efforts underway aiming to resolve these challenges.

This study prepares highly porous carbon (c-fPI) for lithium-ion battery anode that starts from the synthesis of fluorinated polyimide (fPI) via a step polymerization, followed by carbonization. During the carbonization of fPI, the decomposition of fPI releases gases which are particularly from fluorine-containing moiety (–CF3) of fPI, creating well-defined microporous structure with small graphitic regions and a high specific surface area of 934.35 m2 g− 1. In particular, the graphitic region of c-fPI enables lithiation–delithiation processes and the high surface area can accommodate charges at electrolyte/electrode interface during charge–discharge, both of which contribute electrochemical performances. As a result, c-fPI shows high specific capacity of 248 mAh g− 1 at 25 mA g− 1, good rate-retention performance, and considerable cycle stability for at least 300 charge–discharge cycles. The concept of using a polymeric precursor (fPI), capable of forming considerable pores during carbonization is suitable for the use in various applications, particularly in energy storage systems, advancing materials science and energy technologies.

In recent years, the energy storage sector has experienced a notable transition toward the use of organic electrodes. This shift is largely attributed to their superior energy density, cost-effectiveness, and eco-friendliness. However, there is a main drawback that the organic molecules oftentimes suffer shuttle phenomenon across the separator due to their high solubility in the organic electrolyte. In addition, the low electrical conductivity of organic materials is also detrimental, thereby requiring a large amount of carbon additives (up to 40 wt. %) in the electrode. In this perspective, addition of carbon additives with the desirable amount, which can prevent organic molecules from being dissolved into the liquid phase as well as provide the electrical conductivity. While N,Nʹ-dimethylphenazine (DMPZ) was investigated as a model material, we compared two carbon additives with different surface areas and functional groups. We carefully scrutinized the structural effect of carbon additives on the cycle-life performance of the organic electrode.

Disposable masks manufactured in response to the COVID-19 pandemic have caused environmental problems due to improper disposal methods such as landfilling or incineration. To mitigate environmental pollution, we suggest a new process for recycling these disposable masks for ultimate application as a conductive material in lithium-ion batteries (LIBs). In our work, the masks were chemically processed via amine functionalization and sulfonation, followed by carbonization in a tube furnace in the Ar atmosphere. The residual weight percentages, as evaluated by thermogravimetric analysis (TGA), of the chemically modified masks were 30.6% (600 °C, C-600), 24.5% (750 °C, C-750), and 24.1% (900 °C, C-900), respectively, thereby demonstrating the possibility of using our proposed method to recycle masks intended for disposal. The electrochemical performance of the fabricated carbonized materials was assessed by fabricating silicon/graphite (20:80) anodes incorporating these materials as additives for use in LIBs. Using a coin-type half-cell system, cells with the aforementioned carbonized materials exhibited initial capacities of 553 mAh/g, 607 mAh/g, and 571 mAh/g, respectively, which are comparable to those of commercial Super P (591 mAh/g). Cell cycled at the rate of 0.33 C with C-600, C-750, and C-900 as additives demonstrated capacity retention of 53.2%, 47.4%, and 51.1%, respectively, compared with that of Super P (48.3%). In addition, when cycled at rates from 0.2 to 5 C, the cells with anodes containing the respective additives exhibited rate capabilities similar to those of Super P. These results might be attributable to the unique surface properties and morphologies of the carbonized materials derived from the new recycling procedure, such as the size and number of heteroatoms on the surface.

Highly safe lithium-ion batteries (LIBs) are required for large-scale applications such as electrical vehicles and energy storage systems. A highly stable cathode is essential for the development of safe LIBs. LiFePO4 is one of the most stable cathodes because of its stable structure and strong bonding between P and O. However, it has a lower energy density than lithium transition metal oxides. To investigate the high energy density of phosphate materials, vanadium phosphates were investigated. Vanadium enables multiple redox reactions as well as high redox potentials. LiVPO4O has two redox reactions (V5+/V4+/V3+) but low electrochemical activity. In this study, LiVPO4O is doped with fluorine to improve its electrochemical activity and increase its operational redox potential. With increasing fluorine content in LiVPO4O1-xFx, the local vanadium structure changed as the vanadium oxidation state changed. In addition, the operating potential increased with increasing fluorine content. Thus, it was confirmed that fluorine doping leads to a strong inductive effect and high operating voltage, which helps improve the energy density of the cathode materials.

Refined structured tin dioxide gets the amount of attraction because of its low cost and stability. The C@SnO2 nanospheres with mesoporous structures were produced using the hard template method in this work. The C@SnO2 is primarily gained attributed to the dehydration condensation of C6H12O6 and the hydrolysis of SnCl4 ·5H2O. The morphology of the C@SnO2 was analyzed by physical characterization and the diameter of the obtained C@SnO2 was around 138 nm. When C@SnO2 was applied to lithium-ion batteries as anode material, it performed outstanding electrochemical properties, with a capacity of 735 and 539 mA h g− 1 maintained at 1000 and 2000 mA g− 1, respectively. Furthermore, it exhibits favorable discharge/ charge cycle stability. This is probably because of the more chemically redox active sites provided by C@SnO2 nanocomposites and it also allows fast ion diffusion and electron migration.

The development of functional carbon materials using waste biomass as raw materials is one of the research hotspots of lithium-sulfur batteries in recent years. In this work, used a natural high-quality carbon source—coffee grounds, which contain more than 58% carbon and less than 1% ash. Honeycomb-like S and N dual-doped graded porous carbon (SNHPC) was successfully prepared by hydrothermal carbonization and chemical activation, and the amount of thiourea used in the activation process was investigated. The prepared SNHPC showed excellent electrochemical energy storage characteristics. For example, SNHPC-2 has a large pore volume (1.85 cm3·g− 1), a high mesoporous ratio (36.76%), and a synergistic effect (S, N interaction). As the cathode material of lithium-sulfur batteries, SNHPC-2/S (sulfur content is 71.61%) has the highest specific capacity. Its initial discharge-specific capacity at 0.2 C is 1106.7 mAh·g−1, and its discharge-specific capacity after 200 cycles is still as high as 636.5 mAh·g−1.

In this study, we investigate the opportunity of using waste tire char as a cathode material for lithium-ion primary batteries (LPBs). The char obtained by carbonizing waste tires was washed with acid and thermally fluorinated to produce CFX. The structural and chemical properties of the char and CFX were analyzed to evaluate the effect of thermal fluorination. The carbon structure of the char was increasingly converted to CFX structure as the fluorination temperature increased. In addition, the manufactured CFX- based LPBs were evaluated through electrochemical analysis. The discharge capacity of the CFX reached a maximum of 800 mAh/g, which is comparable to that of CFX- based LPBs manufactured from other carbon sources. On the basis of these results, the use of waste tire char-based CFX as a cathode material for LPBs is presented as a new opportunity in the field of waste tire recycling.

전고체 전지는 전기 자동차의 안정성을 향상시키기 위해 기존의 리튬 이온 전지를 대체할 주요 후보로 간주되고 있 습니다. 그러나 전고체 전지에 사용되는 황화물계 고체 전해질은 산화 환원 안정성이 부족하며 양극복합전극과 표면 에서 부반응을 이르켜 문제를 야기시킵니다. 때문에 양극 표면 코팅법이 제안되었고 이는 충방전 사이클 안정성 및 속도 특성의 개선에 유용한 효과를 나타낼 수 있습니다. 본 논문에서는 결정학적 분석을 통하여 신규 Li-Zr-O 조성 탐색을 하였고, 다양한 양극 소재 코팅소재 후보군 중 리튬 이온 전도체인 Li6Zr2O7 구조가 매우 유망하다는 연구 결 과를 확인했습니다. 본 논문은 기존에 사용되는 LiNbO3, Li4Ti5O12가 아닌 새로운 다양한 구조 및 조성의 양극 코팅 소 재개발에 대한 필요성 및 가능성을 시사합니다.

With a rapid expansion in electric vehicles, a huge amount of the spent Li-ion batteries (LIBs) could be discharged in near future. And thus, the proper handling of the spent LIBs is essential to sustainable development in the industry of electrical vehicles. Among various approaches such as pyrometallurgy, hydrometallurgy, and direct recycling, the hydrometallurgical manner has gained interest in recycling the spent LIBs due to its high effectiveness in recycling raw materials (e.g., lithium, nickel, cobalt, and manganese). However, the hydrometallurgical process not only requires the use of large amounts of acids and water resources but also produces toxic gases and wastewater leading to environmental and economic problems, considering potential economic and environmental problems. Thus, this review aims to provide an overview of conventional and state-of-the-art hydrometallurgical processes to recover valuable metals from spent LIBs. First, we briefly introduce the basic principle and materials of LIBs. Then, we briefly introduce the operations and pros-and cons- of hydrometallurgical processes. Finally, this review proposes future research directions in hydrometallurgy, and its potential opportunities in the fundamental and practical challenges regarding its deployment going forward.