ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Bo Fan,Wenzhi Li,Zhongkuan Luo,Xianghua Zhang,Hongli Ma,Ping Fan,Bai Xue
Using solid–liquid hybrid electrolytes is an effective strategy to overcome the large solid/solid interfacial resistance in all-solid-state batteries and the safety problems in liquid batteries. The properties of the solid/liquid electrolyte interphase layer (SLEI) are essential for the performance of solid–liquid hybrid electrolytes. In this work, the solvation reactions between Li2S–P2S5 glass-ceramic solid electrolytes (SEs) and ether electrolytes were studied, and their influence on the SLEI was examined. Although 1,2-dimethoxyethane (DME) reacted with the Li2S–P2S5 glass-ceramic SE to form a dense SLEI, 1,3-dioxolane (DOL) severely corroded the SE, resulting in a loose SLEI. Consequently, a stable SLEI formed with DME. Using a combination of the Li2S–P2S5 glass-ceramic SE and the DME-based liquid electrolyte (LE), stable lithium plating/stripping cycles over 1000 h and a hybrid Li–S battery that retained a specific capacity of 730 mAh g–1 after 200 cycles were demonstrated. The knowledge of the reactions between the sulfide electrolytes and the organic LEs is instructive for the design of stable sulfide–liquid hybrid electrolytes for advanced batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Hong Liu,Peng Zeng,Hao Yu,Xi Zhou,Zhi Li,Manfang Chen,Changqing Miao,Gairong Chen,Tianjing Wu,Xianyou Wang
The significantly-high theoretical energy density and eco-sustainability of lithium sulfur batteries (LSBs) arouses a rapid surge of interest in recent years. However, some key issues of cathode, for instance, the polysulfides confinement, low ion/electrons transfer and etc., hinder the practical utilization of LSBs. Herein, such issues could be carefully handled by using the conductive polypyrrole as polysulfides wrapper. The polypyrrole with pyrrole rings can efficiently confine polysulfides inside cathode for redox. Meanwhile, the conductive polypyrrole with delocalized π-electron cloud can facilitate electrons transfer. Besides, the addition of carbon nanotube (CNT) and oxidized graphene (GO) can enhance the conductivity of cathode material. As a result, the Li 2 S/CNT/GO/PPy cathode delivers a cycling capacity of 525 mAh g −1 with a low-capacity decay rate of 0.065 % cycle −1 after 400 cycles. Therefore, the lithium-sulfur battery with Li 2 S-based and PPy-wrapped cathode could reasonably be counted as a potential alternative of long-cycling Li-ion cells.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Advanced Science
·
2022
·Vol. 9
·期 33
·2204192
·
IF 17.521
Jiongwei Shan,Wei Wang,Bing Zhang,Xinying Wang,Weiliang Zhou,Liguo Yue,Yunyong Li
Designing dense thick sulfur cathodes to gain high-volumetric/areal-capacity lithium–sulfur batteries (LSBs) in lean electrolytes is extremely desired. Nevertheless, the severe Li 2 S clogging and unclear mechanism seriously hinder its development. Herein, an integrated strategy is developed to manipulate Li 2 S redox kinetics of CoP/MXene catalyst via electron-donor Cu doping. Meanwhile a dense S/Cu 0.1 Co 0.9 P/MXene cathode (density = 1.95 g cm −3 ) is constructed, which presents a large volumetric capacity of 1664 Ah L −1 (routine electrolyte) and a high areal capacity of ≈8.3 mAh cm −2 (lean electrolyte of 5.0 µL mg s −1 ) at 0.1 C. Systematical thermodynamics, kinetics, and theoretical simulation confirm that electron-donor Cu doping induces the charge accumulation of Co atoms to form more chemical bonding with polysulfides, whereas weakens Co S bonding energy and generates abundant lattice vacancies and active sites to facilitate the diffusion and catalysis of polysulfides/Li 2 S on electrocatalyst surface, thereby decreasing the diffusion energy barrier and activation energy of Li 2 S nucleation and dissolution, boosting Li 2 S redox kinetics, and inhibiting shuttling in the dense thick sulfur cathode. This work deeply understands the atomic-level manipulation mechanism of Li 2 S redox kinetics and provides dependable principles for designing high-volumetric-energy-density, lean-electrolyte LSBs through integrating bidirectional electro-catalysts with manipulated Li 2 S redox and dense-sulfur engineering.
研究领域:
材料化学
·
电化学
·
能源存储
·
纳米催化
·
固态离子学
·
先进电池技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Lei Zhou,Muhammad Khurram Tufail,Niaz Ahmad,Tinglu Song,Renjie Chen,Wen Yang
The extrinsic cathode interface between the sulfide electrolyte and the Li2S electrode is always ignored in all-solid-state lithium–sulfur batteries. However, the aggregation of the Li2S cathode is still observed during cycling. The gradually lost extrinsic contact interface between the cathode and the electrolyte would result in considerable interface resistance and severe capacity decay in the cell due to the lack of efficient electron and ionic conduction at the interface. Herein, a facile dual-doping strategy demonstrates the synthesis of a functional inorganic electrolyte. The obtained Li7P2.9Ce0.2S10.9Cl0.3 glass–ceramic electrolyte shows a higher-lithium-ionic conductivity of 3.2 mS cm–1 at room temperature. Further, UV–vis absorption and ex situ scanning electron microscopy studies confirm robust interfacial adhesion between the functional inorganic electrolyte, Li7P2.9Ce0.2S10.9Cl0.3, and the Li2S cathode. Thus, a stable extrinsic cathode interface is unprecedently built. Finally, the all-solid-state lithium–sulfur battery based on the Li7P2.9Ce0.2S10.9Cl0.3 electrolyte delivers a higher reversible initial capacity of 617 mA h g–1, a lower interface resistance of 25 Ω cm2 and much better cycling stability (with a high capacity retention of 89% after 100 cycles) than the pristine Li7P3S11 electrolyte.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2018
·Vol. 14
·期 17
·1703871
·
IF 9.598
Fangmin Ye,Meinan Liu,Xue Yan,Jia Li,Zhenghui Pan,Hongfei Li,Yuegang Zhang
High-capacity Li 2 S cathode (1166 mAh g −1 ) is regarded as a promising candidate for the next-generation lithium ion batteries. However, its high potential barrier upon the initial activation process leads to a low utilization of Li 2 S. In this work, a Li 2 S/graphite full cell with the zero activation potential barrier is achieved through an in situ electrochemical conversion of Li 2 S 8 catholyte into the amorphous Li 2 S. Theoretical calculations indicate that the zero activation potential for amorphous Li 2 S can be ascribed to its lower Li extraction energy than that of the crystalline Li 2 S. The constructed Li 2 S/graphite full cell delivers a high discharge capacity of 1006 mAh g −1 , indicating a high utilization of the amorphous Li 2 S as a cathode. Moreover, a long cycle life with 500 cycles for this Li 2 S/graphite full cell is realized. This in situ electrochemical conversion strategy designed here is inspired for developing high energy Li 2 S-based full cells in future.
研究领域:
电化学
·
储能
·
锂离子电池
·
材料科学
✓ 已验证
DOI
高影响因子
Small
·
2023
·Vol. 20
·期 14
·2307950
·
IF 13.3
Fengfeng Han,Liwen Fan,Zhiguo Zhang,Xitian Zhang,Lili Wu
The development of lithium–sulfur batteries (LSBs) is impeded by the shuttle effect of polysulfides (LiPSs) and the sluggish nucleation of Li 2 S. To address these challenges, incorporating electrocatalysts into sulfur host materials represents an effective strategy for promoting polysulfide conversion, in tandem with the rational design of multifunctional sulfur host materials. In this study, Pt nanoparticles are integrated into biomass-derived carbon materials by solution deposition method. Pt, as an electrocatalyst, not only enhances the electrical conductivity of sulfur cathodes and effectively immobilizes LiPSs but also catalyzes the redox reactions of sulfur species bidirectionally. Additionally, Pt helps regulate the 3D deposition and growth of Li 2 S while reducing the reaction energy barrier. Consequently, this accelerates the conversion of LiPSs in LSBs. Furthermore, the catalytic ability of Pt for the redox reactions of sulfur species, along with its influence on the 3D deposition and growth of Li 2 S, is elucidated using electrochemical kinetic analyses and classical models of electrochemical deposition. The cathodes exhibit a high initial specific capacity of 1019.1 mAh g −1 at 1 C and a low decay rate of 0.045% over 1500 cycles. This study presents an effective strategy to regulate Li 2 S nucleation and enhance the kinetics of polysulfide conversion in LSBs.
研究领域:
储能
·
电化学
·
纳米材料
·
催化
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Ning Wang,Naiqin Zhao,Chunsheng Shi,Enzuo Liu,Chunnian He,Fang He,Liying Ma
Lithium-sulfur (Li-S) batteries have been recognized as one of the promising next-generation energy storage devices owing to their high energy density, low cost and eco-friendliness. As for cathode’s performance, the main challenges for developing highly-efficient and long-life Li-S batteries are to retard the polysulfides diffusion into electrolyte and the reaction with metallic lithium (Li). Especially, the safety issues, derived from metallic Li in anode, must be overcome. Herein, we fabricated lithium sulfide@porous carbon composites (Li 2 S@PC) by an in-situ reaction between the lithium sulfate (Li 2 SO 4 ) and the pyrolytic carbon from glucose. The nanosized Li 2 S particles were uniformly distributed in the carbon matrix, which not only significantly improve electronic conductivity of the electrode but also effectively trap the dissolved polysulfides. Furthermore, on the basis of the graphite’s electrochemical features in ether-based electrolyte, we assembled graphite-Li 2 S@PC full cells using the obtained Li 2 S@PC composites as the cathode, graphite as the anode and the DOL/DME with LiNO 3 additive as the electrolyte. A unique strategy was proposed to activate the full-cells in descending order using constant voltage and current to charge the cut-off voltage. This Li-S full cell exhibits stable cycling performance at 0.5 C over 100 cycles. Because graphite-Li 2 S batteries are suitable to the lithium-ion batteries industry, our preliminary results here will shed a new light on the cell design and industrial production.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Donghao Wang,Yuqi Wu,Xuefan Zheng,Shijun Tang,Zhengliang Gong,Yong Yang
All-solid-state Li–S batteries (ASSLSBs) offer an opportunity to realize both high energy density , safety and reliability, via eliminating the polysulfides shuttle effect and flammable liquid electrolyte. However, the sluggish kinetics of S and Li 2 S solid conversion results in low discharge capacity at high active material loading, which is critical for ASSLSBs to implement the high energy density potential. Herein, nitrogen doped-carbon (NC) coated Li 2 S (Li 2 S@NC composite) is developed for ASSLSBs that highly improves electrochemical performance. A thin and uniform nitrogen doped-carbon layer is coated on Li 2 S via pyrolysis deposition approach to prepare Li 2 S@NC. The as obtained Li 2 S@NC composite exhibits greatly enhanced electrochemical performance with high reversible capacity, high coulombic efficiency of ~100%, good rate capability and cycling stability. Particularly, outstanding electrochemical performance with high capacity of 931 mAh g −1 can also be obtained at both high Li 2 S content (43%) and high areal Li 2 S loading (10.4 mg cm −2 ).
研究领域:
材料科学
·
电化学
·
能源存储
·
固态电池
·
纳米材料
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Jinxue Peng,Xuefan Zheng,Yuqi Wu,Cheng Li,Zhongwei Lv,Chenxi Zheng,Jun Liu,Haoyue Zhong,Zhengliang Gong,Yong Yang
All-solid-state lithium–sulfur batteries (ASSLSBs) are considered to be a promising solution for the next generation of energy storage systems due to their high theoretical energy density and improved safety. However, the practical application of ASSLSBs is hindered by several critical challenges, including the poor electrode/electrolyte interface, sluggish electrochemical kinetics of solid–solid conversion between S and Li2S in the cathode, and big volume changes during cycling. Herein, the 85(92Li2S-8P2S5)-15AB composite cathode featuring an integrated structure of a Li2S active material and Li3PS4 solid electrolyte is developed by in situ generating a Li3PS4 glassy electrolyte on Li2S active materials, resulting from a reaction between Li2S and P2S5. The well-established composite cathode structure with an enhanced electrode/electrolyte interfacial contact and highly efficient ion/electron transport networks enables a significant enhancement of redox kinetics and an areal Li2S loading for ASSLSBs. The 85(92Li2S-8P2S5)-15AB composite demonstrates superior electrochemical performance, exhibiting 98% high utilization of Li2S (1141.7 mAh g(Li2S)–1) with both a high Li2S active material content of 44 wt % and corresponding areal loading of 6 mg cm–2. Moreover, the excellent electrochemical activity can be maintained even at an ultrahigh areal Li2S loading of 12 mg cm–2 with a high reversible capacity of 880.3 mAh g–1, corresponding to an areal capacity of 10.6 mAh cm–2. This study provides a simple and facile strategy to a rational design for the composite cathode structure achieving fast Li–S reaction kinetics for high-performance ASSLSBs.
研究领域:
材料科学
·
储能技术
·
电化学
·
固态电池
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Zongzhe Liu,Shaobo Ma,Xue Mu,Renlong Li,Geping Yin,Pengjian Zuo
A silicon anode with ultra-high specific capacity has motivated tremendous exploration for high-energy-density lithium ion batteries while it still faces serious issues of irreversible lithium loss, unstable electrode electrolyte interface (SEI), and huge volume expansion. Prelithiation is a crucial technology to alleviate the harm of active lithium loss of silicon-based full-cell systems. Herein, we reported a cathode prelithiation method using Li2S-PAN as a lithium “donor”, which was synthesized via chemical reaction between sulfurized polyacrylonitrile and Li-biphenyl complex. The Li2S-PAN with an initial charging capacity of 668 mAh g–1 (2.5–4.0 V) is loaded on the LiFePO4 electrode, and the LiFePO4/Li2S-PAN composite electrode displays a high initial charge capacity of 206 mAh g–1, which is 22.3% higher than the pristine LiFePO4. With a silicon/graphite/carbon (Si/G/C) composite anode, the Si/G/C||LiFePO4/Li2S-PAN full cell exhibits a reversible capacity of 123 and 107 mAh g–1 in the 1st and 10th cycle, which is 15.5 and 24.5% higher than the Si/G/C||LiFePO4 battery, respectively. The SEI layer of the silicon anode in the Si/G/C||LiFePO4/Li2S-PAN cell contains abundant conductive LiF species, which can enhance the interfacial stability and reaction kinetics of the cells. The proposed cathode prelithiation process is compatible with the industrial roll-to-roll electrode preparation process, exhibiting a promising application prospect.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2020
·
IF 14.588
Feng Ma,Yangyang Wan,Xiaoming Wang,Xinchao Wang,Jiashun Liang,Zhengpei Miao,Tanyuan Wang,Cheng Ma,Gang Lu,Jiantao Han,Yunhui Huang,Qing Li
The sluggish kinetics of lithium polysulfides (LiPS) transformation is recognized as the main obstacle against the practical applications of the lithium–sulfur (Li–S) battery. Inspired by molybdoenzymes in biological catalysis with stable Mo–S bonds, porous Mo–N–C nanosheets with atomically dispersed Mo–N2/C sites are developed as a S cathode to boost the LiPS adsorption and conversion for Li–S batteries. Thanks to its high intrinsic activity and the Mo–N2/C coordination structure, the rate capability and cycling stability of S/Mo–N–C are greatly improved compared with S/N–C due to the accelerated kinetics and suppressed shuttle effect. The S/Mo–N–C delivers a high reversible capacity of 743.9 mAh g–1 at 5 C rate and an extremely low capacity decay rate of 0.018% per cycle after 550 cycles at 2 C rate, outperforming most of the reported cathode materials. Density functional theory calculations suggest that the Mo–N2/C sites can bifunctionally lower the activation energy for Li2S4 to Li2S conversion and the decomposition barrier of Li2S, accounting for its inherently high activity toward LiPS transformation.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Batteries-Basel
·
2026
·Vol. 12
·期 4
·128
·
IF 6.3
Xinyi Wang,Sha Li,Lingwen Zhang,Jun Li,Dan Guo,Qizhao Hu,Gang Tang,Hongxu Li
Lithium sulfide (Li2S) is indispensable for lithium–sulfur batteries and sulfide solid-state batteries. However, its high preparation cost and strict process conditions represent core bottlenecks restricting large-scale commercial application. To address this issue, a novel process featuring a low-cost, high-safety, and controllable reaction is proposed in this work. Compared with the commercial H2S-based route for Li2S production, the developed process presents distinct advantages, including accessible raw materials, high safety, low overall cost, and low environmental load. Using Li2SO4·H2O as the raw material and Ti as the reducing agent, high-purity T-Li2S (>99.9%) is successfully synthesized via solid-state sintering and purification, yielding a higher purity level than that of commercial C-Li2S (>99.7%). Furthermore, sulfide all-solid-state electrolytes T-Li5.3PS4.3ClBr0.7and C-Li5.3PS4.3ClBr0.7are prepared using the as-obtained T-Li2S and commercial C-Li2S as precursors, respectively. The room-temperature Li-ion conductivities are determined to be 14.5 mS/cm and 11.0 mS/cm, revealing faster ion migration and efficient ion transport in T-Li5.3PS4.3ClBr0.7without high-temperature assistance, which fully validates the feasibility of the proposed strategy. Overall, this work provides a new technical route for the preparation of high-purity Li2S, showing promising application prospects.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）