ACS Applied Energy Materials
·
2024
·
IF 5.4
Jiazhen Du,Xianxian Zhou,Yue Ma,Huazhao Yang,Xiaoxiao Liu,Donghong Duan,Qinbo Yuan,Shibin Liu
Accelerating Li2S2/Li2S reduction through catalysis to enhance the apparent conversion kinetics has emerged as an innovative paradigm for a highly efficient lithium–sulfur battery. Nonetheless, the sluggish kinetics of the solid–solid conversion from solid-state intermediate product Li2S2 to the final discharge product Li2S (corresponding to the last 50% of the theoretical capacity) leads to the premature end of discharge and low discharge capacity output and sulfur utilization. Here, we add 1-butyl-1-methylpyrrolidine trifluoromethanesulfonate ([P14][OTf]) to a typical ether electrolyte, which in turn promotes the slow Li2S2/Li2S conversion kinetics by increasing the solubility of Li2S/Li2S2. The three-electrode experimental and characterization studies disclose that the exchange current densities of Li2S2 reduction, Li2S oxidation, and Li2S2 oxidation are up to 2.28 times, 4.6 times, and 1.04 times than those of the control electrolyte, respectively. Furthermore, the modified electrolyte could activate “dead Li2S”, thus providing more reactive sites and inducing small particle Li2S/Li2S2 deposition. Accordingly, the LSBs containing the Control/5 wt % [P14][OTf] electrolyte exhibit a significantly improved capacity rate of 40% compared with the traditional electrolyte at 0.5 C for 500 cycles (corresponding to a fading rate 0.1% per cycle). We believe that increasing Li2S2/Li2S solubility via electrolyte modification provides practical opportunities toward long-life batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Bo Fan,Yuexin Fang,Bai Xue,Qixing Wu,Zhongkuan Luo,Xianghua Zhang,Laurent Calvez,Lilin Wu
Flexible solid-state batteries fabricated by printing techniques are promising integrated power supplies for miniaturized and customized electronic devices. While typically these batteries use polymer solid electrolytes, a flexible Li2S cathode with sulfide solid electrolyte is spray-printed in this work, by using solvated Li3PS4 nanoparticles as inorganic ion-conductive binder. This benefits from a novel low-temperature-sintering property of these nanoparticles, which can be pressure-free densified, along with the desolvation process, and thus bind the cathode at 250 °C. The battery can be stably charged and discharged for 300 cycles with no stacking pressure, and the capacity maintains at 840 mA h gLi2 S–1. We believe this low-temperature-sintering phenomenon of solid electrolyte nanoparticles will open a new path toward the application of sulfide solid electrolytes in printed solid-state 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
Nanoscale
·
2025
·
IF 5.1
Na Yang,Jiarui Xue,Yuanxiao Ji,Jiyuan Zhang,Weiye Zhang,Xuexia He,Qi Li,zhibin lei,Zonghuai Liu,Jie Sun
Lithium Sulfur (Li-S) batteries have attracted great attention in recent years due to their high theoretical energy density (2600 Wh kg-1) and specific capacity (1675 mAh g-1), abundant reserves and environmental friendly. However, the well-known poor electrical conductivity of sulfur/Li2S, shuttle effect of Lithium Polysulfides (LiPSs) and the in-situ formation of lithium dendrites during cycling process extremely hinders the large fabrication of Li-S batteries. In this work, we have designed and prepared a Poly (3,4-ethylenedioxythiophene) (PEDOT) and Fe3C nanoparticles co-decorated Carbon Nanofibers (CNFs) membrane as a self-supporting Li2S host to enhance the electrochemical performance of Li-S batteries. The PEDOT coating layer can tightly connect Fe3C nanoparticles with the CNFs to form a conductive network, which significantly enhancing the conductivity of the cathode. At the same time, the strong chemical adsorption of PEDOT and the catalytic effect of Fe3C can effectively accelerate the conversion kinetics of LiPSs, thereby improving the battery performance. As a result, the optimized PEDOT@CNFs@Fe3C-16wt%/Li2S composite cathode can achieve a high initial specific capacity of 816 mAh g-1 at the current density of 0.1 C. While such cathode also exhibits only 0.033% capacity decay per cycle at 0.5 C after 1000 cycles, showing its advantages as a high-performance self-supporting flexible Li-S composite cathode.
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
·
2022
·
IF 7.336
Sheng Liang,Ranlin Dong,Shaohua Lu,Lei Hu,Lingli Liu,Qiang Dong,Chonghai Deng,Guangchao Qin,Mao Xu,Chu Liang
Lithium sulfide (Li 2 S) is considered as a promising alternative for the intercalation–type cathode materials because of its high theoretical specific capacity (1166 mAh g –1 ). However, the large–scale application of Li 2 S is limited by its intrinsic low electronic/ionic conductivity and severe shuttle effect of polysulfides. Herein, we report a facile and green method to the in–situ synthesis of Li 2 S–molybdenum (Mo) nanocomposites at room temperature by mechanochemical reaction of lithium hydride with molybdenum sulfide. The fig–like carbon coated Li 2 S–Mo (Li 2 S–Mo@C) nanocomposite with core–shell structure exhibits a low initial activation barrier of 2.51 V, high reversible capacity of 742 mAh g − 1 after 70 cycles at 0.2 A g − 1 and excellent cycling stability over 500 cycles at 1.0 A g − 1 . According to density functional theory calculation and experimental studies, the excellent electrochemical performance of fig–like Li 2 S–Mo@C nanocomposite can be attributed to the increased electronic/ionic conductivity, strong adsorption ability and catalytic conversion of lithium polysulfides, resulting from the synergistic effects of Mo nanodots and, carbon shell and their nanostructure. This work provides a new idea for developing large–scale applications of Li 2 S–based electrodes.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Hong Liu,Peng Zeng,Yongfang Li,Hao Yu,Manfang Chen,Sidra Jamil,Changqing Miao,Gairong Chen,Qi-Cheng Liu,Zhigao Luo,Xianyou Wang
The merit of high energy density endows the lithium sulfide (Li2S)-based lithium–sulfur batteries (LSBs) as a promising candidate for next-generation energy storage batteries. In this work, Li2S is chemically anchored onto the surface of two-dimensional graphene oxide (GO), which is then tangled and connected by one-dimensional carbon nanotube (CNT) to promote electron transfer, and finally further embedded with PANI-derived carbon (PDC) to suppress a polysulfide shuttle. The deliberately designed carbon matrix offers a fast electron and ion transfer route, suitable surface area, void volume, and pore size for redox reactions and polysulfide confinement. Furthermore, PDC could synergistically immobilize polysulfides inside the cathode by means of chemisorption so as to restrain the shuttle effect in LSBs. Last but not least, PDC with a quinone-based structure could function as a redox mediator (RM) to facilitate Li2S oxidation with minimized polarization. Benefited from the aforementioned advantages, the as-fabricated Li2S-GO/CNT/PDC composite, which is coupled with a lithium metal as the anode, delivers initially a high specific capacity of 925 mAh g–1 at 0.1 C and good retention capability of 550 mAh g–1 after 400 cycles at 2 C. Therefore, the good electrochemical behavior of the Li2S-GO/CNT/PDC composite suggests its promising prospects for the commercial application of LSBs in high-energy storage devices.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
Small Methods
·
2020
·Vol. 4
·期 9
·2000353
·
IF 12.13
Mingshan Wang,Hua Yang,Kangqi Shen,Hao Xu,Wenjie Wang,Zhenliang Yang,Lei Zhang,Junchen Chen,Yun Huang,Mingyang Chen,David Mitlin,Xing Li
A stable lean-electrolyte operating lithium–sulfur (Li–S) battery based on a cathode of Li 2 S in situ electrocatalytically deposited from L 2 S 8 catholyte onto a support of metallic molybdenum disulfide (1T-MoS 2 ) on carbon cloth (CC) is created. The 1T-MoS 2 significantly accelerates the conversion Li 2 S 8 catholyte to Li 2 S, chemically adsorbs lithium polysulfide (LiPSs) from solution, and suppresses crossover of the LiPSs to the anode. These experimental findings are explained by density functional theory calculations that show that 1T-MoS 2 gives rise to strong adsorption of polysulfides on its surface and is electrocatalytic for the targeted reversible Li–S conversion reactions. The CC/1T-MoS 2 electrode in a Li–S battery delivers an initial capacity of 1238 mAh g −1 , with a low capacity fade of only 0.051% per cycle over 500 cycles at 0.5 C . Even at a high sulfur loading (4.4 mg cm −2 ) and low electrolyte/S (E/S) ratio of 3.7 µL mg −1 , the battery achieves an initial reversible capacity of 1176 mA h g −1 at 0.5 C , with 87% capacity retention after 160 cycles. The post 500 cycles Li metal opposing 1T-MoS 2 is substantially smoother than the Li opposing CC, with XPS supporting the role of 1T-MoS 2 in inhibiting LiPSs crossover.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
2D Materials
·
2022
·Vol. 9
·期 2
·025028
·
IF 6.861
Meng Yuan,Haodong Shi,Cong Dong,Shuanghao Zheng,Kai Wang,Shaoxu Wang,Zhong-Shuai Wu
Some vital challenges are main obstacles for further development of lithium–sulfur (Li–S) batteries such as low capacity and poor cycle stability resulted from polysulfide shuttling behavior, the physical/chemical entrapment is regarded as an effective method to inhibit and catalyze polysulfides. Herein we design a cross-linked framework of reduced graphene oxide anchored with Cu2−xSe nanoparticles (Cu2−xSe@rGO) by building an electrolyte/Cu2−xSe/graphene triple-phase interface to be a high-efficiency electrocatalyst for Li–S batteries. Importantly, this three-dimensional conductive network possesses a large specific surface area with high ion transport capability, meanwhile providing strong physical constraint for efficient adsorption of soluble polysulfides. Further, this triple-phase catalytic interface provides strong chemical adsorption and abundant Cu2−xSe nanoparticle sulfiphilic active sites, effectively inhibiting the dissolution of polysulfides and guaranteeing the efficient polysulfide adsorption catalysis as well as rapidly uniform Li2S nucleation. Consequently, with the Cu2−xSe@rGO separator, a lower capacity decay rate about 0.059% per cycle after 500 cycles at 2 C is obtained. What's more, with a higher areal sulfur loading of 3.0 mg cm−2, the capacity is still maintained at 805 mAh g−1 over 100 cycles. Therefore, this work will open new avenue to construct 2D transition metal selenide for superior performance Li–S batteries.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
He Wang,Hongling Guo,Zihao Huang,Weiliang Liu,Mei Li,Jinshui Yao,Jiaxi Cui,Yuanhao Wang,Manman Ren
The high activity barriers of Li 2 S nucleation and deposition limit the redox reaction kinetics of lithium polysulfides (LiPSs), meanwhile, the significant shuttle effect of LiPSs hampers the advancement of Li-S batteries (LSBs). In this work, a NiSe 2 /CoSe 2 -rGO (NiSe 2 /CoSe 2 -G) sulfur host with bifunctional catalytic activity was prepared through a hard template method. Electrochemical experiment results confirm that the combination of NiSe 2 and CoSe 2 not only facilitates the bidirectional catalytic function during charge and discharge processes, but also increases the active sites toward LiPSs adsorption. Simultaneously, the highly conductive rGO network enhances the electronic conductivity of NiSe 2 /CoSe 2 -G/S and provides convenience for loading NiSe 2 /CoSe 2 catalysts. Benefitting from the exceptional catalytic-adsorption capability of NiSe 2 /CoSe 2 and the presence of rGO, the NiSe 2 /CoSe 2 -G/S electrode exhibits excellent electrochemical properties . At 1C, it demonstrates a low capacity attenuation of 0.087 % per cycle during 500 cycles. The electrode can maintain a discharge capacity of 927 mAh/g at a sulfur loading of 3.3 mg cm −2 . The bidirectional catalytic activity of NiSe 2 /CoSe 2 -G offers a prospective approach to expedite the redox reactions of active S, meanwhile, this work also offers an ideal approach for designing efficient S hosts for LSBs.
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
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Pengcheng Shi,Xin Liang,Kun Xu,Yi Sun,Sheng Cheng,Chunhua Chen,Hongfa Xiang
Li 2 S is highly desired for high energy-density lithium sulfur batteries since it allows to be matched with Li metal-free anodes and alleviates the volume expansion of S cathode. However, Li + extraction from Li 2 S usually suffers from a huge voltage barrier due to its poor electron conductivity and sluggish Li + ion diffusion during activation. In this work, trace sulfone-assisted-NH 4 I is adopted as an electrolyte additive with synergistic dissolution and catalysis effects to alleviate the voltage barrier of Li 2 S. On one hand, the intercalation between sulfone-NH 4 + and Li 2 S turns solid Li 2 S into liquid phase, which significantly speeding up the transport of electrons and Li + ions during activation. On the other hand, I − works as a redox mediator, which further facilitates the oxidation of Li 2 S to polysulfides. By taking the advantages of synergistic dissolution and catalysis effects from sulfone-NH 4 + and I − , the Li 2 S cathode can be activated at ~3.0 V with a very flat plateau. Finally, the Li 2 S cathode cycled in the electrolyte with optimized 0.5% sulfone-assisted-NH 4 I additive shows a high initial discharge capacity of 1160 mAh g −1 at 0.05C, along with enhanced cycling performances and rate capabilities.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Chinese Physics B
·
2022
·Vol. 31
·期 9
·098203
·
IF 1.652
Jieru Xu,Qiuchen Wang,Wenlin Yan,Liquan Chen,Hong Li,Fan Wu
Sulfide solid electrolytes are widely regarded as one of the most promising technical routes to realize all-solid-state batteries (ASSBs) due to their high ionic conductivity and favorable deformability. However, the relatively high price of the crucial starting material, Li2S, results in high costs of sulfide solid electrolytes, limiting their practical application in ASSBs. To solve this problem, we develop a new synthesis route of Li2S via liquid-phase synthesis method, employing lithium and biphenyl in 1, 2-dimethoxyethane (DME) ether solvent to form a lithium solution as the lithium precursor. Because of the comparatively strong reducibility of the lithium solution, its reaction with sulfur proceeds effectively even at room temperature. This new synthesis route of Li2S starts with cheap precursors of lithium, sulfur, biphenyl and DME solvent, and the only remaining byproduct (DME solution of biphenyl) after the collection of Li2S product can be recycled and reused. Besides, the reaction can proceed effectively at room temperature with mild condition, reducing energy cost to a great extent. The as-synthesized Li2S owns uniform and extremely small particle size, proved to be feasible in synthesizing sulfide solid electrolytes (such as the solid-state synthesis of Li6PS5Cl). Spontaneously, this lithium solution can be directly employed in the synthesis of Li3PS4 solid electrolytes via liquid-phase synthesis method, in which the centrifugation and heat treatment processes of Li2S are not necessary, providing simplified production process. The as-synthesized Li3PS4 exhibits typical Li+ conductivity of 1.85×10−4 S⋅cm−1 at 30 °C.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 27
·2208095
·
IF 13.3
Rui Zhang,Biao Chen,Chunsheng Shi,Junwei Sha,Liying Ma,Enzuo Liu,Naiqin Zhao
Constructing a 3D composite Li metal anode (LMA) along with the engineering of artificial solid electrolyte interphase (SEI) is a promising strategy for achieving dendrite-free Li deposition and high cycling stability. The nanostructure of artificial SEI is closely related to the performance of the LMA. Herein, the self-grown process and morphology of in situ formed Li 2 S during lithiation of Cu x S is studied systematically, and a large-sized sheet-like Li 2 S layer as an artificial SEI is in situ generated on the inner surface of a 3D continuous porous Cu skeleton (3DCu@Li 2 S-S). The sheet-like Li 2 S layer with few interfacial pitfalls (Cu/Li 2 S heterogeneous interface) possesses enhanced diffusion of Li ions. And the continuous porous structure provides transport channels for lithium-ion transport. As a result, the 3DCu@Li 2 S-S presents a high Coulombic efficiency (99.3%), long cycle life (500 cycles), and high-rate performance (10 mA cm −2 ). Furthermore, Li/3DCu@Li 2 S anode fabricated by thermal infusion method inherits the synergistic advantages of sheet-like Li 2 S and continuous porous structure. The Li/3DCu@Li 2 S anode shows significantly enhanced cycling life in both liquid and solid electrolytes. This work provides a new concept to design artificial SEI for LMA with high safe and high performance.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Small
·
2024
·
IF 13
Jing Gao,Yuan Gao,Jinghua Hao,Xiaolin Sun,Fuhua Zhao,Yuan Zhang,Wenyan Si,Jianfei Wu
All-solid-state lithium sulfide-based batteries (ASSLSBs) have drawn much attention due to their intrinsic safety and excellent performance in overcoming the polysulfide shuttle effect. However, the sluggish kinetics of Li 2 S cathode severely impede commercial utilization. Here, a Cu + , I − co-doping strategy is employed to activate the kinetics of Li 2 S to construct high-performance ASSLSBs. The electronic conductivity and Li-ion diffusion coefficient of the co-doped Li 2 S are increased by five and two orders of magnitude, respectively. Cu + as a redox medium greatly improves the reaction kinetics, which is supported by ex situ X-ray photoelectron spectroscopy. Density functional theory calculation (DFT) shows that Cu + , I − co-doping reduces the Li-ions diffusion energy barrier. The co-doped Li 2 S exhibits a remarkable improvement in capacity (1165.23 mAh g −1 (6.65 times that of pristine Li 2 S) at 0.02 C and 592.75 mAh g −1 at 2 C), and excellent cycling stability (84.58% capacity retention after 6200 cycles at 2 C) at room temperature. Moreover, an ASSLSB, fabricated with a lithium-free (Si─C) anode, obtains a high specific capacity of 1082.7 mAh g −1 at 0.05 C and 97% capacity retention after 400 cycles at 0.5 C. This work provides a broad prospect for the development of ASSLSBs with practical energy density exceeding that of traditional lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）