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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Selectively Leaching Li from Anode Materials of Spent Lithium-Ion Battery by Using Water

Tingyan Ren,Keyi Lin,Man Zhao,Bozhang Lai,Jujun Ruan

Selective extraction of Li from spent lithium-ion batteries (LIBs) is currently a hot topic. However, current research techniques focus on selectively extracting Li from cathode materials, and there are problems with high energy consumption, complex processes, and high difficulty in technical application. And Li in the anode material was ignored. Therefore, this study proposes a technique for selectively extracting Li from anode materials using aqueous solutions. The experimental results show that there is 4.15% Li in the anode material carbon black powder. Under acidic, alkaline, and pure water conditions, the extraction rate of Li from anode materials is greater than 90.00%. Acidic and alkaline conditions can leach heavy metals such as Ni/Co/Mn/Cu, requiring secondary treatment of wastewater, while the concentration of heavy metals leached from water can be directly discharged. When ultrasonic leaching is used for 5–10 min, the leaching rate is greater than 90.00%. When shaking leaching is used for 30–60 min, the leaching rate is greater than 90.00%. When standing leaching is used for 60–120 min, the leaching rate is greater than 90.00%. In the actual production process, suitable enhanced leaching methods can be selected according to different needs. This article may be the first study to propose the selective extraction of Li from anode materials using aqueous solutions.

✓ 已验证 DOI 高影响因子
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WATER RESEARCH · 2025 · IF 12.4

Surfactant-regulated electrospray printing PEI-TMC nanofiltration membrane for efficient separation of Mg2+/Li+

Huijun Yu,Xieyang Xu,Yingsong Liu,Chenshuo Wang,Linxuan Gao,Jianbing Wang

Nanofiltration (NF) offers an energy-efficient approach for lithium recovery from brines. Conventional NF membranes rely on the positively charged polyamide layer formed via interfacial polymerization (IP) of polyethyleneimine (PEI) and trimesoyl chloride (TMC) to repel Mg 2+ more strongly than Li + , but their Mg 2+ /Li + selectivity remains constrained by limited control over pore size distribution. Here, we develop polyamide (PA) layers using amphiphilic dioctyl sulfosuccinate sodium (DOSS)-mediated electrospray interfacial polymerization (DEIP). Electrospray-assisted polymerization at the interfaces of abundant immiscible microdroplets produces thinner PA layers with reduced transport resistance and accelerates monomer diffusion in a non-selective manner. Molecular dynamics (MD) simulation and density function theory (DFT) calculations further reveal that DOSS selectively regulates the diffusion behavior of PEI and TMC within microdroplets, enabling the formation of PA layers with uniform pore structures and a positively charged surface. These structural advantages deliver precise ion sieving for lithium extraction, achieving a Mg 2+ /Li + selectivity of 142 and water permeance of 13.45 L·m −2 ·h −1 ·bar −1 . The DEIP membrane also demonstrates stable Mg 2+ /Li + separation over seven days of continuous NF operation. This work underscores the promise of DEIP membranes for high-efficiency lithium extraction and highlighted their potential for practical brine-based lithium recovery.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Polymers · 2025 ·Vol. 17 ·期 17 ·2369 · IF 4.9

Three-Dimensional-Printed Polymer–Polymer Composite Electrolytes for All-Solid-State Li Metal Batteries

Hao Wang,Xin Xiong,Huie Hu,Sijie Liu

High-performance batteries for military and extreme environment applications require alternatives to conventional liquid lithium-ion batteries (LIBs), which suffer from poor low-temperature performance and safety risks. All-solid-state lithium batteries (ASSLBs) offer enhanced safety and superior low-temperature capability. In this work, we designed and fabricated composite solid-state electrolytes using polyvinylidene fluoride (PVDF) and polyacrylic acid (PAA) as polymer matrices, N,N-dimethylformamide (DMF) as the solvent, and lithium bis(trifluoromethane sulfonimide) (LiTFSI) as the lithium salt. Composite solutions with varying PAA mass ratios were prepared. Advanced three-dimensional (3D) printing technology enabled the rapid and precise fabrication of electrolyte membranes. An ionic conductivity of about 2.71 × 10−4S cm−1at 25 °C, high mechanical strength, and good thermal properties can be achieved through component and 3D printing process optimization. Assembled LiCoO2||PVDF@PAA||Li ASSLBs delivered an initial discharge capacity of 165.3 mAh/g at 0.1 mA cm−2(room temperature), maintaining 98% capacity retention after 300 cycles. At 0 °C, these cells provided 157.4 mAh/g initial capacity with 85% retention over 100 cycles at 0.1 mA cm−2. This work identifies the optimal PAA ratio for enhanced electrochemical performance and demonstrates the viability of 3D printing for advanced ASSLB manufacturing.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Small · 2023 ·Vol. 19 ·期 33 ·2301275 · IF 13.3

Interfacial Interaction of Multifunctional GQDs Reinforcing Polymer Electrolytes For All-Solid-State Li Battery

Huaxin Liu,Laiqiang Xu,Hanyu Tu,Zheng Luo,Fangjun Zhu,Wentao Deng,Guoqiang Zou,Hongshuai Hou,Xiaobo Ji

Solid-state polymer electrolytes are highly anticipated for next generation lithium ion batteries with enhanced safety and energy density. However, a major disadvantage of polymer electrolytes is their low ionic conductivity at room temperature. In order to enhance the ionic conductivity, here, graphene quantum dots (GQDs) are employed to improve the poly (ethylene oxide) (PEO) based electrolyte. Owing to the increased amorphous areas of PEO and mobility of Li + , GQDs modified composite polymer electrolytes achieved high ionic conductivity and favorable lithium ion transference numbers. Significantly, the abundant hydroxyl groups and amino groups originated from GQDs can serve as Lewis base sites and interact with lithium ions, thus promoting the dissociation of lithium salts and providing more ion pathways. Moreover, lithium dendrite is suppressed, associated with high transference number, enhanced mechanical properties and steady interface stability. It is further observed that all solid-state lithium batteries assembled with GQDs modified composite polymer electrolytes display excellent rate performance and cycling stability.

✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Enabling stable cobalt-free Li-rich cathodes through a one-step dual-modified strategy

Peilin Ran,Xiaoqing Li,Kang Wu,Na Li,Kesheng Gao,Chenzhang Gu,Jinkui Zhao,Enyue Zhao,Zhimin Wu,Fangwei Wang

Cobalt-free Lithium-rich layered oxides (LRLOs) are promising cathodes for low-cost and high-energy-density Li-ion batteries. However, their remarkable capacity comes with challenges including structural degradation, irreversible oxygen release and sluggish kinetics. Herein, we conduct a one-step dual-modified strategy by yttrium doping and Li 3 PO 4 surface modification. Combining density-functional theory calculations with in-situ X-ray diffraction and in-situ differential electrochemical mass spectrometry, the Y 3+ doping and Li 3 PO 4 nano coating modified LRLOs is demonstrated has an excellent structural stability with enhanced Li⁺ diffusion kinetics and stabilized oxygen lattice. Excellent rate performance and thermal stability are achieved: high discharge specific capacity of 221 mAh·g −1 at room temperature (96.5 % at 1 C after 100 cycles) and incredible discharge specific capacity of 210 mAh·g −1 at 55 °C (91.8 % at 2 C after 100 cycles). This work resolves the safety and stability issues and provides a feasible strategy for Co-free LRLOs.

✓ 已验证 DOI 高影响因子
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Journal of Energy Chemistry · 2020 · IF 7.216

A three-dimensional crosslinked chitosan sulfate network binder for high-performance Li–S batteries

Jianwen Feng,Huan Yi,Zhiwen Lei,Jun Wang,Hongbo Zeng,Yonghong Deng,Chaoyang Wang

Poor cycling performance caused by the shuttle effect of polysulfides is the main obstacle in the development of advanced lithium–sulfur (Li–S) batteries. Functional polymer binders with polar groups can effectively adsorb polysulfides chemically, thereby suppressing the shuttle effect. Herein, a robust three-dimensional crosslinked polymer network, which demonstrates excellent mechanical property and strong affinity for polysulfides , is prepared by the aldimine condensation and coordination reactions. The crosslinked chitosan sulfate network (CCSN) significantly enhances the cycling performance and rate capability of the sulfur cathode. The CCSN-based sulfur cathode exhibits a high initial discharge capacity of 824 mAh g −1 with only 0.082% average capacity loss per cycle at 1 C. At a high rate of 4 C, the cathode exhibits a high capacity retention of 84.8% after 300 cycles. Moreover, the CCSN-based sulfur cathode exhibits an excellent cycling performance at a high sulfur loading of 2.5 mg cm −2 , which indicates the excellent mechanical strength and binding performance of the CCSN binder for high-energy density Li–S batteries. This study demonstrates a viable approach for developing high-performance Li–S batteries for practical application.

✓ 已验证 DOI 高影响因子
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ACS Omega · 2021 · IF 3.512

One-Pot Synthesis of High-Performance Tin Chalcogenides/C Anodes for Li-Ion Batteries

Xianyu Liu,Tayyaba Najam,Ghulam Yasin,Mohan Kumar,Miao Wang

Tin chalcogenides are considered as promising anode materials for lithium-ion batteries (LIBs) due to their high theoretical lithium-storage capacity. Herein, we have successfully synthesized the composites of tin chalcogenides and graphite, that is, SnS/C, SnSe/C, and SnS0.5Se0.5/C, via a simple one-pot solid-state method. During the electrochemical test, they exhibit excellent lithium-storage ability and cyclic performance as the anode electrodes of LIBs due to the introduction of carbon. In particular, (i) SnS/C displayed a high specific capacity of 875 mAh g–1 at 0.2 A g–1 over 200 cycles; (ii) SnSe/C presents 734 mAh g–1 at 0.2 A g–1 after 100 cycles, and it delivers 690 mAh g–1 at 1.0 A g–1 over 300 cycles; and (iii) the SnS0.5Se0.5/C composite electrode delivers a specific capacity of 643 mAh g–1 at 0.5 A g–1 over 150 cycles. Furthermore, another series of tin-based composites have also been successfully fabricated (i.e., Sn/C, SnS2/C, SnSe2/C, and SnTe/C), showing the general applicability of the synthetic route applied here. Our synthetic approach demonstrates a promising route for the large-scale production of high-performance tin chalcogenides/C anode materials for LIBs and other battery systems (e.g., Na-ion and K-ion batteries).

✓ 已验证 DOI 高影响因子
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ELECTROCHIMICA ACTA · 2020 · IF 6.215

Efficacious nitrogen introduction into MoS2 as bifunctional electrocatalysts for long-life Li-O2 batteries

Xiaoping Fan,Youguo Huang,Hongqiang Wang,Fenghua Zheng,Chunlei Tan,Yu Li,Xifei Lu,Zhaoling Ma,Qingyu Li

Defect engineering has been an efficient means to govern the electrocatalytic performances of oxygen electrode in Li-O 2 batteries. Herein, we introduce N atoms into MoS 2 for manufacturing sulfur vacancies to improve the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) kinetics of rechargeable Li-O 2 batteries. The obtained results show that N doping opened the crystal distance space of N-MoS 2 , reduced the charge transfer resistance and simultaneously induces Mo-N bonds and a large number of sulfur vacancies. The assembled Li-O 2 batteries with N-MoS 2 as the cathode electrocatalyst deliver discharge specific capacity of 5205.5 mAh g −1 at the current density of 100 mA g −1 , which is much higher than the MoS 2 (2600.3 mAh g −1 ). It also shows excellent cyclic performance with 224 cycles at the current density of 200 mA g −1 within a capacity limitation of 1000 mAh g −1 . Overall, the as-developed N-MoS 2 could be regarded as a promising cathode electrocatalyst for Li-O 2 batteries.

✓ 已验证 DOI 高影响因子
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Heterostructured CuCo2S4-Co9S8 Nanosheets as Freestanding Cathodes for Flexible Fiber-Shaped Li-CO2 Batteries

Xiaoqi Zhu,Lin Chen,Qisheng Fang,Jianli Cheng,Yuefeng Su,Paula Ratajczak,Francois Beguin,Bin Wang

Li-CO2 batteries with attractive characteristics of high energy density power supply and carbon dioxide fixation have attracted widespread attention. However, the lack of suitable cathode catalysts and their unsatisfactory electrochemical performance have impeded their development as promising Li-CO2 batteries for energy storage. Constructing heterojunctions by interfacial engineering to improve performance is considered one of the effective strategies. Herein, heterostructured CuCo2S4-Co9S8 nanosheets are fabricated by a facile hydrothermal method and employed as efficient cathode catalysts for Li-CO2 batteries. The construction of heterojunctions by interfacial engineering has proved as an effective strategy to enhance the electrochemical performance of the Li-CO2 batteries. The delocalized electrons between CuCo2S4 and Co9S8 contribute to a low median charge potential (∼3.6 V), small polarization (0.62 V), high energy efficiency of up to 83%, and outstanding cycle life (480 h) of the CuCo2S4-Co9S8 cathodes. Meanwhile, as a proof of concept, flexible fiber-shaped Li-CO2 batteries based on these cathodes are fabricated and demonstrate boosted flexibility adaptability and provide a stable power supply at various bending conditions.

✓ 已验证 DOI 高影响因子
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ACS Applied Energy Materials · 2022 · IF 6.959

Li2CO3: Insights into Its Blocking Effect on Li-Ion Transfer in Garnet Composite Electrolytes

Yixuan Guo,Jun Cheng,Zhen Zeng,Yuanyuan Li,Hongqiang Zhang,Deping Li,Lijie Ci

Garnet-type Li7La3Zr2O12 (LLZO) has been widely used as a filler in composite solid electrolytes (CSEs) to achieve high-performance solid-state batteries (SSBs). Unfortunately, moisture-sensitive LLZO suffers from surface Li2CO3 passivation when being exposed to an ambient atmosphere. The insulated Li2CO3 layer is thought to reduce the Li+ transportability of CSEs. However, further studies are still needed to find out the underlying mechanism, which helps to guide future filler modification and electrolyte design. Herein, the role of the Li2CO3 layer in CSEs is elucidated from different perspectives. The passivate Li2CO3 layer is verified to prohibit the formation of the high conductive interlayer, change the Li+ transport pathway, and decrease the carrier concentration in CSEs. Also, the Li2CO3 layer would reduce the electropositivity of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) particles, which therefore weakens the anchoring effect toward bis(trifluoromethanesulfonyl)imide (TFSI)−. Accordingly, without Li2CO3, the electrolyte of polyethylene oxide/LiTFSI/IL (ionic liquid) with LLZTO-AT (PLILA) displays 2 times higher ionic conductivity and an improved Li+ transference number of 0.49. Additionally, an excellent cycling performance is presented in Li symmetric cells and full cells with PLLA. This work provides a novel perspective for future research on lithium-ion transport mechanisms and inspires designing better-performance SSBs.

✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Processing mechanism synergizing surface and intercalation pseudocapacitance engineering fast-charging Li-based anode materials

Zhuo Chen,Qiming Wang,Shuai Bai,Xi Wang,Wenlie Lin,Yining Zhang

Pseudocapacitive material can achieve rapid charge and discharge response. In this study, a vanadium-based conductive network hydrate (Na 0.13 Mg 0.02 )V 2 O 5 ·0.98H 2 O (NMVO) was designed. The Na + and Mg 2+ in NMVO are sandwiched between two layers of vacancy-ordered prisms and monoclinic nanonetwork V 3 O 7 (VO 2 :V 2 O 5  = 1:1) to form a conductive network with a layer spacing of up to 11.67 Å, this structure facilitates rapid interlayer diffusion of cations and enhanced conductivity. Reduction-NMVO (r-NMVO) with hierarchical heterostructures was prepared via an in-situ electrochemical process to generate interlayer vanadium-based active sites (LiV 3 O 8 , LiV 2 O 5 , Na 3 V 3 O 8 , MgVO 3 ) with multi-electron reaction, which enhanced the generation of surface redox pseudocapacitance. The interlayer heterostructure is integrated with the core of the precursor V 3 O 7 to form an active site-rich conductive network with strong pulse impact resistance, which promotes the generation of intercalated pseudocapacitance and increases the cycle stability of the electrode. This intercalation-surface redox pseudocapacitive mechanism was confirmed by first-principles, in-situ, and ex-situ characterization analysis. The r-NMVO|Li battery still maintains a capacity of 95.5 % after 65,500 cycles at a current density of 50 A g −1 . These results contribute directly to the realization of stable, fast charge and discharge material design.

✓ 已验证 DOI 高影响因子
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Materials Chemistry Frontiers · 2021 ·Vol. 5 ·期 6 ·2715-2723 · IF 6.482

A(NH3)xFePS3 (A = Li, K): intercalated Fe thiophosphate via the liquid ammonia method

Xiaojing Feng,Zhongnan Guo,Xiaoxiao Yan,Jun Deng,Dan Wu,Zijing Zhang,Fan Sun,Wenxia Yuan

Metal phosphorus trichalcogenides (MPX3) are of great interest since these layered materials exhibit wide applications in optical, electrical and magnetic fields. An effective chemical intercalation route for MPX3 which could regulate their physical properties, however, is still lacking. In this work, we show that the liquid ammonia method is an efficient route to co-intercalate alkali metals and NH3 molecules into the gaps in FePS3. After intercalation, the interlayer distance is significantly enlarged by ∼3 Å while the monoclinic lattice (C2/m space group) is still maintained. The structure refinement and EDS measurement suggest that intercalation does not induce any Fe vacancy, thus leading to electron transfer from the alkali metal to [FePS3] layers. Interestingly, magnetic susceptibility shows that the intrinsic anti-ferromagnetic transition in the FePS3 matrix is completely suppressed by this intercalation, whereas a spin-glass state is observed in A(NH3)xFePS3 (A = Li, K) in the lower temperature range (<50 K). The intercalation described in this work is reversible: the alkali metal can be easily de-intercalated using a two-step route and the anti-ferromagnetism reappears accordingly. Meanwhile, the liquid ammonia method is also shown to be efficient at intercalating other MPS3 materials (M = Mn, Co, Ni). Our work not only enriches the intercalation chemistry in the MPX3 system but also provides an excellent route to regulate the magnetic properties of these layered materials.

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