GREEN CHEMISTRY
·
2026
·
IF 10.6
Lei You,Chen Cheng,Shaoqing Liu,Siwei Kuang,Dongming Cai,Danyun Lei,Ying Zheng,Jianwen Liu
The practical deployment of lithium–sulfur (Li–S) batteries is severely hampered by the polysulfide shuttle effect, significant volume changes during sulfur conversion reactions, and dendrite growth on the Li anode. While modifying diaphragms with polar materials like Co3O4 offers a promising solution, their conventional synthesis relies on costly virgin materials and complex processes, raising economic and environmental concerns. Concurrently, the escalating pile of spent lithium-ion batteries (LIBs) presents a critical waste challenge. Hence, a sustainable “waste-to-wealth” strategy is proposed to address both issues simultaneously through the upcycling of spent LiCoO2 (LCO) batteries into a high-value Co3O4-N-doped reduced graphene oxide (Co3O4-rGO) composite, which is employed as a multifunctional diaphragm modifier. The Co3O4 nanoparticles, derived from the spent cathode, are designed to anchor and convert lithium polysulfides (LiPSs), while the N-doped rGO, regenerated from the discarded anode, provides a conductive network and facilitates Li+ transport. This synergistic effect effectively suppresses the polysulfide shuttle, accelerates reaction kinetics, and promotes uniform lithium deposition. Consequently, Li–S batteries equipped with the Co3O4-rGO-0.5 modified diaphragm exhibit exceptional cycling stability and rate capability, retaining a high capacity of 502.9 mAh g−1 after 600 cycles at 3C with an ultra-low capacity decay rate of 0.0437% per cycle, markedly outperforming batteries with conventional diaphragms. This work establishes a scalable, eco-friendly protocol for repurposing battery waste into advanced materials, paving the way for the development of sustainable energy storage systems.
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高影响因子
ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 34
·46235-46246
·
IF 7.8
Wang Tiansheng,Lin Yixin,Zheng Zeqiang,Gao Chaochao,Xu Jie,Yu Wen,Zhang Jiaheng
The increasing volume of spent lithium-ion batteries (LIBs) has triggered severe resource and environmental issues, making the environmentally friendly, high-value regeneration of spent LiCoO 2 (SLCO) imperative in the new energy field. Upcycling SLCO into high-voltage lithium cobalt oxide (LCO) potentiates its high-value-added utilization; however, single-functional lithium sources in existing regeneration processes only achieve basic lithium compensation and fail to simultaneously address the bottlenecks of bulk structural degradation and uncontrolled interfacial side reactions under 4.6 V high-voltage cycling, which hinders the stable upcycling of SLCO into high-voltage LCO. Herein, a bulk-interface and dual-domain stabilization strategy is proposed via one-step solid-state sintering with lithium cysteinate (Li-Cys). The preferential cleavage of Li–S bonds in Li-Cys first enables targeted lithium compensation for spent LiCoO 2 , followed by the introduction of NaOH to provide a mild alkaline environment, thereby simultaneously achieving Na/S co-doping in the bulk and the in situ construction of a Li 2 SO 4 /LiN x O y coating at the interface. Na + stabilized the layered structure as an interlayer pillar, S enhanced the lattice oxygen stability, and the coating suppressed interfacial side reactions, jointly improving the structural stability and ion transport kinetics. The regenerated NS-RLCO cathode delivered an initial capacity of 205 mAh/g at 0.1C, 91.9% capacity retention after 100 cycles at 1C, and 158.9 mAh/g reversible capacity at 3C. Economic and life-cycle analyses confirmed its superior cost and environmental benefits over traditional recycling processes, providing a novel route for environmentally friendly, high-value regeneration of spent LCO.
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PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Qiujun Wang,Yifei Wang,Nana Bai,Xiaomeng Jia,Zhaojin Li,Qujiang Sun,Ranran Li,Fei Yuan,Bo Wang
LiCoO 2 (LCO) stands as one of the dominant cathode materials in commercial lithium-ion batteries due to its high energy density and extended cycle life. However, irreversible structural phase transitions (O3 to H1–3) are triggered when the LCO is charged beyond 4.4 V, accompanied by lattice oxygen release and cobalt dissolution. These phenomena aggravate cathode electrolyte interfacial side reactions, ultimately resulting in progressive capacity decay and coulombic efficiency deterioration. Herein, capitalizing on the high solubility of LiNO 3 in sulfolane (SUL), a novel carbonate-based composite polymer electrolyte (CPE) was engineered to in-situ construct cathode electrolyte interface (CEI) layer enriched with Li 3 N, Li 2 O, Li 2 SO 4 , Li 2 SO 3 , and RSO 3 Li through LiNO 3 decomposition, effectively suppressing cobalt dissolution. Remarkably, capacity retention of 73.93 % was reached after 100 cycles under 4.6 V. This work highlights a synergistic SUL-LiNO 3 interfacial modulation strategy, offering a pioneering electrolyte design paradigm for 4.6 V-class LCO batteries.
研究领域:
材料科学
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电化学
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能源存储
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高影响因子
Energy Storage Materials
·
2024
·
IF 18.9
Meng Wang,Xiaolang Liu,Wen Zhang,Hongwei Niu,Leimin Xu,Jiantao Han,Yuhao Lu
For the first time, this work investigates the synergetic impact of yttrium (Y) and aluminium (Al) co-doping on the electrochemical properties of 4.6 V LiCoO 2 (LCO) cathode for high energy density lithium-ion batteries. The optimized LCO demonstrates an impressive initial discharge capacity of 208.6 mAh g −1 in the voltage range of 3–4.6 V, along with superior structural stability , retaining over 86 % of its initial capacity even after 125 cycles at the current of 100 mA g −1 that is far higher than the capacity retention of 40 % for the pristine LCO under the same condition. Thanks to the synergistic effect , Al in Co layers enhances the bonds of Al/Co-O to stabilize oxygen in the LCO crystal structure while Y serves “pillar” in Li layers, migrated from the initial Co layers during cycling process, effectively curtail the formation and expansion of interlayer cracking, which contributes to the long-term cycle stability of LCO under high voltage. Most importantly, Al/Y co-doping is a facile process compatible with the existing industrial infrastructure for LCO mass production, and thus it can be scaled up readily for commercial applications. Al/Y co-doped LCO is assembled into commercial-level pouch cells with graphite anode, achieves an extremely high energy density of 750 Wh/L, and exhibits a superior cycling stability and obtains a capacity retention of 88.2 % at 25 °C after 800 cycles with the high cutoff voltage of 4.55 V.
研究领域:
材料科学
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电化学
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储能
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电池技术
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高影响因子
Small
·
2020
·Vol. 16
·期 13
·1907163
·
IF 11.459
Rongxiang Hu,Huayu Qiu,Huanrui Zhang,Peng Wang,Xiaofan Du,Jun Ma,Tianyuan Wu,Chenglong Lu,Xinhong Zhou,Guanglei Cui
Lithium (Li) metal batteries (LMBs) are enjoying a renaissance due to the high energy densities. However, they still suffer from the problem of uncontrollable Li dendrite and pulverization caused by continuous cracking of solid electrolyte interphase (SEI) layers. To address these issues, developing spontaneously built robust polymer-reinforced SEI layers during electrochemical conditioning can be a simple yet effective solution. Herein, a robust homopolymer of cyclic carbonate urethane methacrylate is presented as the polymer matrix through an in situ polymerization method, in which cyclic carbonate units can participate in building a stable polymer-integrated SEI layer during cycling. The as-investigated gel polymer electrolyte (GPE) assembled LiCoO 2 /Li metal batteries exhibit a fantastic cyclability with a capacity retention of 92% after 200 cycles at 0.5 C (1 C = 180 mAh g −1 ), evidently exceeding that of the counterpart using liquid electrolytes. It is noted that the anionic ring-opening polymerization of the cyclic carbonate units on the polymer close to the Li metal anodes enables a mechanically reinforced SEI layer, thus rendering excellent compatibility with Li anodes. The in situ formed polymer-reinforced SEI layers afford a splendid strategy for developing high voltage resistant GPEs compatible with Li metal anodes toward high energy LMBs.
研究领域:
材料科学
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能源存储
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DOI
PubMed
高影响因子
Energy Storage Materials
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2018
·
IF 0
Gaozhan Liu,Dongjiu Xie,Xuelong Wang,Xiayin Yao,Shaojie Chen,Ruijuan Xiao,Hong Li,Xiaoxiong Xu
A series of new solid electrolytes of Li 3+3 x P 1- x Zn x S 4- x O x ( x = 0.01, 0.02, 0.03, 0.04, 0.05, 0.06) are synthesized successfully via Zn, O co-doping the Li 3 PS 4 glass-ceramic for the first time. The result shows that Li 3 PS 4 aliovalent substitution of 2 mol% ZnO (Li 3.06 P 0.98 Zn 0.02 S 3.98 O 0.02 ) presents the highest conductivity of 1.12×10 −3 S cm −1 at room temperature, which is twice that of the pristine Li 3 PS 4 . Besides, Li 3.06 P 0.98 Zn 0.02 S 3.98 O 0.02 exhibits excellent stability against humid air , lithium metal and chlorobenzene solvent. The mechanisms of the enhancement of conductivity and air-stability are well understood by conducting first-principles density functional theory (DFT) calculation and Bond-Valence (BV) analysis, and the results well demonstrate that the conductivity and air-stability of Li 3 PS 4 could be improved via Zn, O dual-doping, in which partial P 5+ could be substituted by Zn 2+ , and a part of S 2- could be replaced by O 2- . Finally, the all-solid-state lithium battery (ASSLB) with bi-layer electrolytes of LiCoO 2 /Li 10 GeP 2 S 12 /Li 3.06 P 0.98 Zn 0.02 S 3.98 O 0.02 /Li is assembled, and it delivers an initial discharge capacity of 139.1 mAh g −1 at 0.1 C and a capacity retention of 81.0% after 100 cycles at room temperature. This work combines systematical experimental characterizations and sufficient theoretical calculations to develop a new promising sulfide electrolyte with superior lithium ion conductivity and high air-stability for ASSLBs application.
研究领域:
材料科学
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电化学
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能源存储
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DOI
Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 22
·11930-11939
·
IF 7.443
Shaojie Han,Yonggao Xia,Zhen Wei,Bao Qiu,Lingchao Pan,Qingwen Gu,Zhaoping Liu,Zhiyong Guo
The Li-rich layered oxides are attractive electrode materials due to their high reversible specific capacity (>250 mA h g−1); however, the origin of their abnormal capacity is still ambiguous. In order to elucidate this curious anomaly, we compare the lattice oxygen oxidation states among the Li-rich layered oxide Li1.14Ni0.136Co0.136Mn0.544O2, Li2MnO3 and LiNi0.5Co0.2Mn0.3O2, the two components in Li-rich layered oxides, and the most common layered oxide LiCoO2 before and after initial charge–discharge. For simplicity, we employ chemical treatments of NO2BF4 and LiI acetonitrile solutions to simulate the electrochemical delithiation and lithiation processes. X-ray photoelectron spectroscopy (XPS) studies reveal that part of lattice oxygen in Li1.14Ni0.136Co0.136Mn0.544O2 and Li2MnO3 undergoes a reversible redox process (possibly O2− ↔ O22−), while this does not occur in LiNi0.5Co0.2Mn0.3O2 and LiCoO2. This indicates that the extra capacity of Li-rich layered oxides can be attributed to the reversible redox processes of oxygen in the Li2MnO3 component. Thermogravimetric analysis (TGA) further suggests that the formed O22− species in the delithiated Li1.14Ni0.136Co0.136Mn0.544O2 can decompose into O2 at about 210 °C. This phenomenon demonstrates a competitive relationship between extra capacity and thermal stability, which presents a big challenge for the practical applications of these materials.
研究领域:
材料科学
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电化学
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储能
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电池材料
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固态化学
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Xiaojian Liao,Maoyou Ye,Jialin Liang,Zhijie Guan,Shoupeng Li,Yanghong Deng,Qiaowei Gan,Zihang Liu,Xiaodi Fang,Shuiyu Sun
The recovery of metals from spent LiCoO 2 batteries (SLBs) is essential to avoid resource wastage and the production of hazardous waste . However, the major challenge in regard to recovering metals from SLBs using traditional bioleaching is the low Co yield. To overcome this issue, a mixed culture of Acidithiobacillus caldus and Sulfobacillus thermosulfidooxidans was designed for use in SLBs leaching in this study. With the assistance of Fe 2+ as a reductant, 99% of Co and 100% of Li were leached using the above mixed-culture bioleaching (MCB) process, thus solving the problem of low metal leaching efficiency from SLBs. Analysis of the underlying mechanism revealed that the effective extraction of metals from SLBs by the Fe 2+ -MCB process relied on Fe 2+ -releasing electrons to reduce refractory Co(III) to Co(II) that can be easily bioleached. Finally, the hazardous SLBs was transformed into a non-toxic material after treatment utilizing the Fe 2+ -MCB process. However, effective SLBs leaching was not achieved by the addition of Fe 0 to the MCB system. Only 25% Co and 31% Li yields were obtained, as the addition of Fe 0 caused acid consumption and bacterial apoptosis. Overall, this study revealed that reductants that cause acid consumption and harm bacteria should be ruled out for use in reductant-assisted bioleaching processes for extracting metals from SLBs.
研究领域:
环境科学
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微生物学
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高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 12
·6801-6808
·
IF 10.733
Lei Zhang,Shi Wang,Jingyu Li,Xu Liu,Pingping Chen,Tong Zhao,Liaoyun Zhang
Polyether-based materials, especially poly(ethylene oxide) (PEO) and derivatives thereof, have been extensively studied as Li-conducting all-solid-state polymer electrolytes (SPEs) for Li-based batteries due to their specific advantages such as easy fabrication, high safety, and outstanding compatibility with lithium salts. However, PEO-based polymers usually have too strong complexation ability with lithium ions and high crystallinity, resulting in a low lithium-ion transference number and room temperature ionic conductivity. In this study, we choose hyperbranched polyethylenimine (HPEI) as the core of a SPE matrix, while polyester segments as the arms through sequential ring-open polymerization (ROP) of glycolide (GC) and ε-caprolactone (CL). Specifically, the HPEI core containing N atoms can promote the dissociation of lithium salts, while the polyester segments can effectively dissolve lithium salts and transport ions. Furthermore, the SPE (HPEI–PGC–PCL/LiTFSI) is cast onto a ceramic film containing ceramic nanowires to prepare a composite SPE (CSPE), which can further construct ion transport channels at the interface of the polymer and nanowires. Synergizing the advantages of HPEI–PGC–PCL and ceramic nanowires, the CSPE exhibits superior electrochemical performance. Especially, the LiFePO4/CSPE/Li cell exhibits a discharge capacity of 162 mA h g−1 at the C-rates of 0.2, 0.5 and 1C, and an average discharge capacity of 158 mA h g−1 with an average coulombic efficiency of 99.8% over 200 cycles at 0.5C. More importantly, the LiCoO2/CSPE/Li cell also shows very good cycling performance (reaches 130 mA h g−1 at a current density of 0.06 mA cm−2) and rate capacity (reaches 80 mA h g−1 at a current density of 0.3 mA cm−2). This work highlights a new and novel host material that has the potential to be used as a high performance all-solid-state electrolyte for solid-state batteries.
研究领域:
材料科学
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电化学
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电池技术
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DOI
高影响因子
ACS Nano
·
2024
·
IF 15.8
Yu Ye,Jiazhong Geng,Daxian Zuo,Kangdi Niu,Diancheng Chen,Junhao Lin,Xihan Chen,Haw Jiunn Woo,Yizhou Zhu,Jiayu Wan
All-solid-state batteries (ASSBs) have garnered considerable attention as promising candidates for next-generation energy storage systems due to their potentially simultaneously enhanced safety capacities and improved energy densities. However, the solid future still calls for materials with high ionic conductivity, electrochemical stability, and favorable interfacial compatibility. In this study, we present a series of halide solid-state electrolytes (SSEs) utilizing a doping strategy with highly valent elements, demonstrating an outstanding combination of enhanced ionic conductivity and oxidation stability. Among these, Li2.6In0.8Ta0.2Cl6 emerges as the standout performer, displaying a superionic conductivity of up to 4.47 mS cm–1 at 30 °C, along with a low activation energy barrier of 0.321 eV for Li+ migration. Additionally, it showcases an extensive oxidation onset of up to 5.13 V (vs Li+/Li), enabling high-voltage ASSBs with promising cycling performance. Particularly noteworthy are the ASSBs employing LiCoO2 cathode materials, which exhibit an extended cyclability of over 1400 cycles, with 70% capacity retention under 4.6 V (vs Li+/Li), and a capacity of up to 135 mA h g–1 at a 4 C rate, with the loading of active materials at 7.52 mg cm–2. This study demonstrates a feasible approach to designing desirable SSEs for energy-dense, highly stable ASSBs.
研究领域:
材料科学
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能源存储
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电池技术
·
电化学
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DOI
高影响因子
Science Advances
·
2022
·Vol. 8
·期 40
·
IF 14.957
Jing Xu,Yang Jin,Kai Liu,Nawei Lyu,Zili Zhang,Bin Sun,Qianzheng Jin,Hongfei Lu,Huajun Tian,Xin Guo,Devaraj Shanmukaraj,Hui Wu,Meicheng Li,Michel Armand,Guoxiu Wang
Recycling lithium from spent batteries is challenging because of problems with poor purity and contamination. Here, we propose a green and sustainable lithium recovery strategy for spent batteries containing LiFePO4, LiCoO2, and LiNi0.5Co0.2Mn0.3O2 electrodes. Our proposed configuration of “lithium-rich electrode || LLZTO@LiTFSI+P3HT || LiOH” system achieves double-side and roll-to-roll recycling of lithium-containing electrode without destroying its integrity. The LiTFSI+P3HT-modified LLZTO membrane also solves the H+/Li+ exchange problem and realizes a waterproof protection of bare LLZTO in the aqueous working environment. On the basis of these advantages, our system shows high Li selectivity (97%) and excellent Faradaic efficiency (≥97%), achieving high-purity (99%) LiOH along with the production of H2. The Li extraction processes for spent LiFePO4, LiNi0.5Co0.2Mn0.3O2, and LiCoO2 batteries is shown to be economically feasible. Therefore, this study provides a previously unexplored technology with low energy consumption as well as high economic and environmental benefits to realize sustainable lithium recycling from spent batteries.
研究领域:
材料科学
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环境科学
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可持续发展
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电池技术
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DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Minghao Zhang,Shaojian Zhang,Chenyu Liu,Zengqing Zhuo,Yuan Lei,Denghai Xiao,Chenghao Yao,Wei Fu,Chunni Jiang,Yiting Miao,Li Feng,Zhan Lin
All-solid-state lithium-ion batteries (ASSLIBs) with many advantages are excellent candidates for eVTOL batteries. However, a significant challenge arises from the incompatibility between cathode materials and sulfide solid-state electrolytes (S-SSEs). To overcome this, a sulphuration reduction interphase consisting of CoO/Li 2 SO 4 /Li 2 CO 3 is formed on the surface of the cathode through a simplified sulfur-induced thermal reduction process applied to lithium cobalt oxide (LCO) in this work. The introduction of sulfur transforms the LCO surface, enhancing compatibility with S-SSEs. Consequently, ASSLIBs exhibit a notable initial capacity of 143.3 mAh g −1 at 0.2 C, with 86.19 % capacity retention after 200 cycles. Furthermore, the batteries in this study demonstrate an outstanding rate capacity of 77 mAh g −1 at 2 C (pristine sample with 0 mAh g −1 at 2 C). This evidence strongly substantiates the remarkable efficacy of the sulphuration reduction interphase in effectively mitigating interfacial reactions and ensuring rate ability. Essentially, this study opens new avenues for fostering a stable cathode/SSEs interface, providing a novel framework for designing high-performance and safe eVTOL batteries.
研究领域:
材料科学
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电化学
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能源存储
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高影响因子
危险品化学品经营许可证（带存储）