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Energy Storage Materials · 2017 · IF 0

Engineering layer structure of MoS2-graphene composites with robust and fast lithium storage for high-performance Li-ion capacitors

Rutao Wang,Shijie Wang,Dongdong Jin,Yabin Zhang,Yaojun Cai,Jianmin Ma,Li Zhang

Two dimensional layered MoS 2 has demonstrated great promise as an ideal alternative to graphite-based anodes for hybrid Li-ion capacitors and Li-ion batteries. Research effort on this material has focused mainly on synthesizing highly nanostructured MoS 2 that allows reducing the dimensions into nanoscale to cross over the sluggish kinetics of Li-ion charge storage. Herein, we engineer the layer structure of MoS 2 to preferentially expand the interlayer distance to increase atomic interface contact/interaction by successfully inserting amorphous carbon layer into adjacent MoS 2 monolayers. This interlayer modified MoS 2 is demonstrated to have the predominantly pseudocapacitive characteristics and can get further gains in Li-ion storage properties through incorporating reduced graphene oxide (RGO). Thus, a novel hybrid Li-ion capacitor is fabricated by employing this MoS 2 -RGO composite as the anode and activated carbon as the cathode, which exhibits an ultrahigh specific energy density of 188   Wh   kg -1 at 200   W   kg -1 and remains 45.3   Wh   kg -1 even at a high specific power density of 40,000   W   kg -1 as well as long cycle life. This work shows that engineering interlayer structure and introducing conductive graphene can significantly impact the Li-ion storage properties, enabling new opportunities for designing newly advanced MoS 2 anodes for next-generation energy storage devices.

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ADVANCED MATERIALS · 2024 ·Vol. 36 ·期 25 ·2400656 · IF 27.4

The Potential Regulation of Working Anode for Long-Term Zero-Volt Storage at 37 °C in Li-Ion Batteries

Hanchen Wang,Yingtian Liu,Mingze Jiang,Yu-Xing Yao,Chunhua Hu,Chong Yan,Qiang Zhang,Luming Li

The advanced lithium-ion batteries that can tolerate zero-volt storage (ZVS) are in high demand for implantable medical devices and spacecraft. However, ZVS can raise the anode potential, leading to Cu current collector dissolution and solid-electrolyte interphase (SEI) degradation, especially at 37 °C. In this contribution, by quantitatively regulating the dosage of Li 6 CoO 4 cathode additives, controllable potential of the working anode under abusive-discharge conditions is demonstrated. The addition of Li 6 CoO 4 keeps zero-crossing potential (ZCP) and the potential of ZVS below 2.0 V (vs Li/Li + ) for LiCoO 2 |mesocarbon microbead cells at 37 °C. The capacity retention ratio (CRR) increases from 69.1% and 35.9% to 98.6% and 90.8% after 10 and 20 days of ZVS, respectively. The Cu dissolution and SEI degradation are effectively suppressed, while the over-lithiated cathode exhibits high reversible capacity after ZVS. The limiting conditions of long-term ZVS are further explored and a corresponding guide map is designed. When quantitatively regulating ZCP and the potential in ZVS, Cu dissolution, SEI degradation, and irreversible conversion of the cathode constitute the limiting conditions. This contribution designs the most reasonable potential range for ZVS protection at 37 °C, and realizes the best CRR record through precise potential regulation for the first time.

CAS / MDL: 1307-96-6 12057-24-8
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NEW JOURNAL OF CHEMISTRY · 2024 · IF 2.7

Recycling of Li and Co from spent LiCoO2 cathode materials through a low-temperature urea-assisted sulfation roasting approach

Yichuan Kong,Yongzhi Duan,Yuezhi Zhang,Yulin Min,Hongxiu Lu,Penghui Shi

The lithium-ion battery industry is experiencing explosive growth. Efficiently and greenly recycling Li, Co and other valuable metals is extremely important to alleviate the scarcity of resources and protect the environment. In this study, an improved recycling strategy is proposed to convert spent LiCoO2 batteries into water-soluble sulfate below 350 °C using the auxiliary effect of urea on sulfation roasting. This strategy not only allows for the direct synthesis of precursors for regeneration after selective recovery of lithium and cobalt but also further reduces the roasting temperature requirement compared to the conventional salt-thermal method. After roasting, Li and Co can be recovered from the solution by simple aqueous leaching. Under optimal conditions, the leaching rates of Li and Co were 94.94% and 95.47%, respectively. Subsequently, the Li and Co compounds that could be used as battery precursors were obtained by the addition of CO32−. Characterized by high efficiency, low energy consumption, absence of secondary pollution, and utilization of inexpensive and readily accessible raw materials, this approach offers a novel concept in the domain of lithium-ion battery recycling via salt-thermal methods.

CAS / MDL: 12190-79-3
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APPLIED SURFACE SCIENCE · 2025 · IF 6.9

Amorphous FePx nanoparticles embedded in N, P-codoped carbon nanofibers for high capacity and long cycle Li-ion batteries

Xuxu Wang,Wenbo Wang,Jinhui Li,Shuang Gao,Ping Nie,Fen Yao,Limin Chang

Transition metal phosphides (TMPs) are ideal anodes for lithium-ion batteries (LIBs) due to their high theoretical specific capacity and suitable lithiation potential. However, transition metal phosphides suffer from the shortcomings of large volume change and low electrical conductivity, resulting in poor rate performance and short cycle life. In this paper, nanofibers consisting of amorphous FeP x nanoparticles and N, P-codoped carbon substrate are synthesized by electrospinning and in-situ phosphidation to address these challenges. The amorphous structure with no grain boundary and isotropy can provide more Li + transport channels and Li + storage sites. Moreover, the N, P-codoped carbon substrate can effectively improve the electronic conductivity of the electrodes and the structural robustness of the nanofibers. Due to the unique structure and composition, the FeP x /C nanofibers exhibit excellent electrochemical performance when used as anodes for LIBs (stable cycling over 2200 cycles at 1 A g −1 ). It is suggested that the large pseudo-capacitance and fast Li + diffusion resulting from the amorphous structure are important reasons for the excellent electrochemical performance of FeP x /C nanofibers. This work provides a new idea to optimize the electrochemical performance of TMPs, which is expected to be used in other conversion anode materials.

CAS / MDL: 7705-08-0 83-86-3
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Energy Storage Materials · 2025 · IF 20.2

Precise Ni/Co separation from spent Li-Ion batteries: Revealing the pivotal role of H2O in deep eutectic solvents

Xingyu Hu,Hui Shi,Yilei Zheng,Penghui Shao,Liming Yang,Xubiao Luo

The sustainable recovery of valuable metals from end-of-life lithium-ion batteries (LIBs) has become essential for relieving the supply-demand contradiction of key resources. However, the high similarity in physicochemical properties of transition metals poses a fundamental challenge for the selective recycling. Here we proposed a facile strategy for defining the demarcation line of precipitation/dissolution behavior for precise Ni/Co separation. A malonic acid-based deep eutectic solvent (DES) is developed, emphasizing the H 2 O-mediated competitive coordination and differentiated solubility. We discovered the distinctive formation of [Ni(H 2 O) 6 ] 2+ and [CoCl 4 ] 2- in the DES-20 % H 2 O system. Furthermore, the K sp differences of the Ni-complex and Co-complex in the C 3 H 2 O 4 2- -rich environment was effectively magnified. These significant differences synergistically enable the generation of C 3 H 2 NiO 4 ·2H 2 O precipitation (∼ 99.9 % purity), achieving a remarkable Ni/Co separation factor of 125, which guarantees sequential separation of all metals. This universal methodology along with in-depth mechanism understanding provides a guideline toward value-added recovery of LIBs.

CAS / MDL: 110-94-1 144-62-7
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

A prelithiation pathway with high-release efficiency and self-enhanced interface chemistry to achieve stable Li-ion full cells

Jiabao Lai,Jiao You,Jianhui Zhu,Ming Yang,Yanyi Wang,Shengkui Zhong,Hongwei Mi,Chuanxin He,Dingtao Ma,Peixin Zhang

First-cycle irreversible lithium loss critically limits lithium-ion battery capacity. This study proposes the design of unique cathode prelithiation material, carbon sphere-composited lithium squarate (FSL-CS). Among them, the three-dimensional conductive network fabricated through chemical precipitation significantly enhances both electronic conductivity and structural stability. Electrochemical characterization reveals that FSL-CS delivers a compensation capacity of 390.8 mAh·g −1 during initial charging, achieving 92 % efficiency in lithium release, which have high-release efficiency. Compared to unmodified one, the composite demonstrates reduced kinetic barriers with a lowered delithiation plateau voltage of 3.97 V (vs. 4.16 V for pristine material). In situ/ex situ analyses confirm the carbon sphere composite strategy establishes self-enhanced interface chemistry. This optimizes interfacial charge transfer, boosting the Li + diffusion coefficient by an order of magnitude and continuously inducing in-situ formation of a gradient organic-inorganic composite cathode electrolyte interphase. Full-cell evaluations show that NCM811||Graphite batteries with 5 % FSL-CS maintain 87.3 % capacity retention after 400 cycles at 1C, while pouch cells retain 70.2 % capacity after 1000 cycles. Theoretical calculation reveals that FSL-CS exhibits a lower lithium migration energy barrier (0.65 eV) compared to conventional Li 2 NiO 2 (1.00 eV). This work provides new design principles for stable organic prelithiation systems featuring high-release efficiency, self-enhanced interfaces, and low-voltage operation.

CAS / MDL: 2892-51-5 554-13-2
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ACS Nano · 2023 · IF 17.1

Interfacial Manipulation via In Situ Constructed Fast Ion Transport Channels toward an Ultrahigh Rate and Practical Li Metal Anode

Shuixin Xia,Fengguang Li,Xun Zhang,Lingli Luo,Yue Zhang,Tao Yuan,Yuepeng Pang,Junhe Yang,Wei Liu,Zaiping Guo,Shiyou Zheng

The successful substitution of Li metal for the conventional intercalation anode can promote a significant increase in the cell energy density. However, the practical application of the Li metal anode has long been fettered by the unstable solid electrolyte interface (SEI) layer on the Li metal surface and notorious dendritic Li growth. Herein, a stabilized SEI layer with in situ constructed fast ion transport channels has successfully been achieved by a robust In2S3-cemented poly(vinyl alcohol) coating. The modified Li metal demonstrates significantly enhanced Coulombic efficiency, high rate performance (10 mA cm–2), and ultralong life cycling stability (∼4900 cycles). The Li|LiCoO2 (LCO) cell presents an ultralong-term stable operation over 500 cycles at 1 C with an extremely low capacity decay rate (∼0.018% per cycle). And the Li|LCO full cell with the ultrahigh loading cathode (∼25 mg cm–2) and ultrathin Li foil (∼40 μm) also reveals a prolonged cycling performance under the low negative-to-positive capacity ratio of 2.2. Furthermore, the Li|LCO pouch cell with a commercial cathode and ultrathin Li foil still manifests excellent cycling performance even under the harsh conditions of limited Li metal and lean electrolyte. This work provides a cost-effective and scalable strategy toward high performance practical Li metal batteries.

✓ 已验证 DOI PubMed 高影响因子
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MICROCHEMICAL JOURNAL · 2025 · IF 5.1

Ultrasensitive niclosamide electrochemical sensor based on chitosan-encapsulated and Super P Li carbon black-embedded whisker carbon nanotubes networks

Hongyuan Zhao,Mengyuan Zhao,Zetan Zhang,Xinya Xu,Wenwen Cao,Zirong Li

A novel niclosamide (NA) electrochemical sensor was constructed by modifying glassy carbon electrode (GCE) with chitosan (CTS)-encapsulated and Super P Li carbon black (Super P)-embedded whisker carbon nanotubes (w-CNTs) networks. The incorporation of w-CNTs and Super P formed an integrated carbon-based conductive networks that dramatically boosted the conductivity property. Moreover, CTS prevented the agglomeration of carbon materials and anchored zero-dimensional Super P and one-dimensional w-CNTs, constructing the “point-to-line” conductive carbon networks. The good film-forming ability of CTS enhanced the stability of the fabricated sensor. By harnessing the synergistic interplay of CTS/Super P/w-CNTs, the CTS/Super P/w-CNTs/GCE sensor achieved the remarkably sensitive NA detection (LOD: 10.5 nM) within an acceptable NA concentration range (0.01–25 μM). For the practical application of NA detection in water samples, the designed sensor exhibited outstanding reliability, as confirmed by relative standard deviations (RSD) ranging from 1.07 % to 3.48 %, and recovery rates ranging from 97.30 % to 102.80 %.

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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Nanofiltration membrane with crown ether as exclusive Li+ transport channels achieving efficient extraction of lithium from salt lake brine

Hongwei Li,Ying Wang,Tingyu Li,Xiang-Kui Ren,Jixiao Wang,Zhi Wang,Song Zhao

Lithium extraction from salt lake brines with high Mg 2+ /Li + ratios represents an effective alternative for tackling the scarcity of lithium resources. In this work, nanofiltration (NF) membrane with exclusive Li + transport channels was designed and prepared through facile interfacial polymerization, in which polyethyleneimine (PEI) bonded with 15-crown-5 ether (15C5) through hydrogen interaction was selected as the aqueous monomer ( [email protected] ) and reacted with trimesoyl chloride (TMC). The channels generated by 15C5 molecules could facilitate Li + transport owing to their affinity to Li + . Molecular dynamics simulation was conducted to further confirm the Li + transport through [email protected] membrane with exclusive Li + transport channels provided by 15C5. The [email protected] membrane displayed a permeability of 8.0 L·m −2 ·h −1 ·bar −1 and stable separation factor ( S Li,Mg ) of 14, which could reduce Mg 2+ /Li + mass ratio of a simulated brine from 20 to 1.7. Furthermore, a three-stage NF process was designed and performed using a [email protected] membrane to separate a simulated salt lake brine, containing multiple ions and Mg 2+ /Li + mass ratio of 50. After the treatment, the ultimate permeate solution of the third stage contained 24 ppm of Li + and 2.7 ppm of Mg 2+ with Mg 2+ /Li + mass ratio of 0.1. Therefore, this process could be applied to obtain Li 2 CO 3 products with high purity. Our investigation highlights the highly efficient Mg 2+ /Li + separation through NF membranes with exclusive Li + transport channels, potentially applicable to lithium extraction from salt lake brines with high Mg 2+ /Li + mass ratios.

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ACS Applied Energy Materials · 2025 · IF 5.5

Suppressing the Redox Shuttling Effect Based on the Anion Trapping Composite Separator Enhances the Performance of Li-O2 Batteries

Azhagar Samy,Raja Palani,Yi-Shiuan Wu,She-Huang Wu,Jeng-Kuei Chang,Arshid Numan,Rajan Jose,Chun-Chen Yang

Rechargeable lithium-oxygen (Li-O2) batteries are at the forefront of energy storage technology. Yet, they face critical challenges, including poor capacity, high overpotential at the oxygen cathode, inefficient lithium utilization, oxygen crossover, and the troublesome growth of lithium dendrites. This study provides an innovative solution using a graphene nanosheet (GNS) composite nickel ferrite (NiFe2O4) (NiFe2O4@GNS) catalyst and ZIF-8 particles decorated glass fiber (GF) (ZIF-8@GF) separator. Remarkably, the in situ grown ZIF-8@GF composite separator boosts higher ionic conductivity (∼2.87 × 10–3 S cm–1) and transport number (tLi+ ∼ 0.58). The modified catalyst and separator performed significantly better than the unmodified analogs in terms of specific capacity and cycling stability. In short, the device using the ZIF-8@GF separator and NiFe2O4@GNS catalyst goes up to 500 cycles without any charge polarization at 300 mA·g–1 and 500 mAh·g–1. In contrast, the corresponding cycle number for the cell with an unmodified separator even using the modified catalyst is ∼209 cycles with high charge polarization. These studies reveal that the modified separator effectively minimizes oxygen and I–/I3– redox crossover, captures anions, accelerates lithium-ion transport, and prevents the harmful intermediates (like O2– or LiO2), which can drastically degrade the organic electrolyte. Furthermore, the insulating characteristics of the ZIF-8@GF membrane deter direct electron transport to ZIF-8 nanoparticles during lithium peroxide formation, thus ensuring uninterrupted access to catalytic anion trapping sites.

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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Ni/Mg Dual Concentration-Gradient Surface Modification to Enhance Structural Stability and Electrochemical Performance of Li-Rich Layered Oxides

Guanghui Cong,Lujun Huang,Guobo Yang,Jinpeng Song,Shaoshuai Liu,Yating Huang,Xin Zhang,Zheyuan Liu,Lin Geng

Li-rich layered oxides (LRLOs), with the advantages of high specific capacity and low cost, are considered as candidates for the next-generation cathode of lithium-ion batteries (LIBs). Unfortunately, sluggish kinetics and interfacial degradation lead to capacity loss and voltage decay of the material during cycling. To address these issues, we propose a Ni/Mg dual concentration-gradient modification strategy for LRLOs. From the center to the surface of the modified materials, the contents of Ni and Mg are gradually increased while the content of Mn is decreased. The high Ni content on the surface increases the proportion of cationic redox, elevating the operating voltage and accelerating reaction kinetics. Moreover, the doped Mg on the surface of the material acting as a stabilizing pillar suppresses the migration of transition metals, stabilizing the layered structure. Therefore, the material with the Ni/Mg dual concentration-gradients delivers a superior electrochemical performance, exhibiting a suppressed voltage decay of 2.8 mV per cycle during 200 cycles (1 C, 2–4.8 V) and an excellent rate capability of 94.84 mAh/g at 7C. This study demonstrates a synergic design to construct high-performance LRLO cathode materials for LIBs.

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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Inhibition of Discharge Side Reactions by Promoting Solution-Mediated Oxygen Reduction Reaction with Stable Quinone in Li–O2 Batteries

Xiao Liu,Peng Zhang,Liangliang Liu,Jianwen Feng,Xiaofeng He,Xiaosheng Song,Qing Han,Hua Wang,Zhangquan Peng,Yong Zhao

Aprotic lithium–oxygen (Li–O2) batteries with an ultrahigh theoretical energy density have great potential in rechargeable power supply, while their application still faces several challenges, especially poor cycle stability. To solve the problems, one of the effective strategies is to inhibit the generation of the LiO2 intermediate produced via a surface-mediated oxygen reduction reaction (ORR) pathway, which is an important species inducing byproduct generation and low cell cyclic stability. Herein, a series of quinones and solid materials serve as the solution-mediated and surface-mediated ORR catalysts, and it was found that the generation of LiO2 and byproducts from solid catalysts was inhibited by quinones. Among the studied quinones, benzo[1,2-b:4,5-b′]dithiophene-4,8-dione, a quinone molecule with the advantage of a highly symmetrical planar and conjugated structure and without α-H, exhibits high redox potential, diffusion coefficient, and electrochemical stability, and consequently the best ORR activities and the capability to inhibit byproduct generation. It indicated that the increase of the solution-mediated ORR pathway plays an important role in restraining the discharging side reaction, substantially improving cell cycle stability and capacity. This study provides the theoretical and experimental basis for better understanding the ORR process of Li–O2 batteries.

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