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1.
Proc Natl Acad Sci U S A ; 120(31): e2301260120, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37487097

RESUMO

Lithium-sulfur (Li-S) batteries with high energy density and low cost are promising for next-generation energy storage. However, their cycling stability is plagued by the high solubility of lithium polysulfide (LiPS) intermediates, causing fast capacity decay and severe self-discharge. Exploring electrolytes with low LiPS solubility has shown promising results toward addressing these challenges. However, here, we report that electrolytes with moderate LiPS solubility are more effective for simultaneously limiting the shuttling effect and achieving good Li-S reaction kinetics. We explored a range of solubility from 37 to 1,100 mM (based on S atom, [S]) and found that a moderate solubility from 50 to 200 mM [S] performed the best. Using a series of electrolyte solvents with various degrees of fluorination, we formulated the Single-Solvent, Single-Salt, Standard Salt concentration with Moderate LiPSs solubility Electrolytes (termed S6MILE) for Li-S batteries. Among the designed electrolytes, Li-S cells using fluorinated-1,2-diethoxyethane S6MILE (F4DEE-S6MILE) showed the highest capacity of 1,160 mAh g-1 at 0.05 C at room temperature. At 60 °C, fluorinated-1,4-dimethoxybutane S6MILE (F4DMB-S6MILE) gave the highest capacity of 1,526 mAh g-1 at 0.05 C and an average CE of 99.89% for 150 cycles at 0.2 C under lean electrolyte conditions. This is a fivefold increase in cycle life compared with other conventional ether-based electrolytes. Moreover, we observed a long calendar aging life, with a capacity increase/recovery of 4.3% after resting for 30 d using F4DMB-S6MILE. Furthermore, the correlation between LiPS solubility, degree of fluorination of the electrolyte solvent, and battery performance was systematically investigated.

2.
Small ; : e2401587, 2024 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-38855999

RESUMO

Heterostructured materials commonly consist of bifunctions due to the different ingredients. For host material in the sulfur cathode of lithium-sulfur (Li-S) batteries, the chemical adsorption and catalytic activity for lithium polysulfides (LiPS) are important. This work obtains a Ni5P2-Ni nanoparticle (Ni5P2-NiNPs) heterostructure through a confined self-reduction method followed by an in situ phosphorization process using Al/Ni-MOF as precursors. The Ni5P2-Ni heterostructure not only has strong chemical adsorption, but also can effectively catalyze LiPS conversion. Furthermore, the synthetic route can keep Ni5P2-NiNPs inside of the nanocomposites, which have structural stability, high conductivity, and efficient adsorption/catalysis in LiPS conversion. These advantages make the assembled Li-S battery deliver a reversible specific capacity of 619.7 mAh g- 1 at 0.5 C after 200 cycles. The in situ ultraviolet-visible technique proves the catalytic effect of Ni5P2-Ni heterostructure on LiPS conversion during the discharge process.

3.
Small ; 20(1): e2304938, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37649198

RESUMO

Materials with various single-transition metal atoms dispersed in nitrogenated carbons (M─N─C, M = Fe, Co, and Ni) are synthesized as cathodes to investigate the electrocatalytic behaviors focusing on their enhancement mechanism for performance of Li-S batteries. Results indicate that the order of both electrocatalytic activity and rate capacity for the M─N─C catalysts is Co > Ni > Fe, and the Co─N─C delivers the highest capacity of 1100 mAh g-1 at 1 C and longtime stability at a decay rate of 0.05% per cycle for 1000 cycles, demonstrating excellent battery performance. Theoretical calculations for the first time reveal that M─N─N─C catalysts enable direct conversion of Li2 S6 to Li2 S rather than Li2 S4 to Li2 S by stronger adsorption with Li2 S6 , which also has an order of Co > Ni > Fe. And Co─N─C has the strongest adsorption energy, not only rendering the highest electrocatalytic activity, but also depressing the polysulfides' dissolution into electrolyte for the longest cycle life. This work offers an avenue to design the next generation of highly efficient sulfur cathodes for high-performance Li-S batteries, while shedding light on the fundamental insight of single metal atomic catalytic effects on Li-S batteries.

4.
Small ; 20(16): e2308603, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38009482

RESUMO

The shuttle effect of lithium polysulfides (LiPSs) severely hinders the development and commercialization of lithium-sulfur batteries, and the design of high-conductive carbon fiber-host material has become a key solution to suppress the shuttle effect. In this work, a unique Co/CoN-carbon nanocages@TiO2-carbon nanotubes structure (NC@TiO2-CNTs) is constructed using an electrospinning and nitriding process. Lithium-sulfur batteries using NC@TiO2-CNTs as cathode host materials exhibit high sulfur utilization (1527 mAh g-1 at 0.2 C) and can still maintain a discharge capacity of 663 mAh g-1 at a high current density of 5 C, and the capacity loss is only 0.056% per cycle during 500 cycles at 1 C. It is worth noting that even under extreme conditions (sulfur-loading = 90%, surface-loading = 5.0 mg cm-2 (S), and E/S = 6.63 µL mg-1), the lithium-sulfur batteries can still provide a reversible capacity of 4 mAh cm-2. Throughdensity functional theory calculations, it has been found that the Co/CoN heterostructures can adsorb and catalyze LiPSs conversion effectively. Simultaneously, the TiO2 can adsorb LiPSs and transfer Li+ selectively, achieving dual confinement for the shuttle effect of LiPSs (nanocages and nanotubes). The new findings provide a new performance enhancement strategy for the commercialization of lithium-sulfur batteries.

5.
Small ; 20(12): e2306928, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37953415

RESUMO

The development of lithium-sulfur batteries is seriously hindered by the shuttle effect of lithium polysulfides (LiPSs) and the low electrical conductivity of sulfur. To solve these problems, efficient catalysts can be used to improve the conversion rate of LiPSs and the conductivity of sulfur cathode. Herein, annealed melamine foam supported MoSe2 (NCF@MoSe2) is used as interlayer and the MoSe2/MoP heterojunction obtained by phosphating MoSe2 is further used as the catalyst material for metal fusion with a sulfur element. The interlayer can not only improve the electrical conductivity and effectively adsorb and catalyze LiPSs, but more importantly, the MoSe2/MoP heterojunction can also effectively adsorb and catalyze LiPSs, so that the batteries have a dual inhibition shuttling effect strategy. Furthermore, the rapid anchor-diffusion transition of LiPSs, and the suppression of shuttling effects by catalyst materials are elucidated using theoretical calculations and in situ Raman spectroscopy. The two-step catalytic strategy exhibits a high reversibility of 983 mAh g-1 after 200 cycles at 0.5 C and a high-rate capacity of 889 mAh g-1 at 5 C. This work provides a feasible solution for the rational design of interlayer and heterojunction materials and is also conducive to the development of more advanced Li-S batteries.

6.
Small ; 20(34): e2400068, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38593293

RESUMO

Lithium-sulfur (Li-S) batteries with high theoretical energy density (2600 Wh kg-1) are considered to be one of the most promising secondary batteries. However, the practical application of Li-S batteries is limited by the polysulfides shuttling and unstable lithium metal anodes. Herein, an asymmetric separator (CACNM@PP), composed of Co-Ni/MXene (CNM) on the cathode and Cu-Ag/MXene (CAM) on the anode for high-performance Li-S batteries is reported. For the cathode, CNM provides a synergistic effect by integrating Co, Ni, and MXene, resulting in strong chemical interactions and fast conversion kinetics for polysulfides. For the anode, CAM with abundant lithiophilicity active sites can lower the nucleation barrier of Li. Moreover, LiCl/LiF layers are generated in situ as an ion conductor layer during charging and discharging, inducing a uniform deposition of Li. Therefore, the assembled cells with the CACNM@PP separators harvest excellent electrochemical performance. This work provides novel insights into the development of commercially available high-energy density Li-S batteries with asymmetric separators.

7.
Small ; 20(31): e2311850, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38446091

RESUMO

Lithium-sulfur (Li-S) batteries hold immense promise as next-generation energy storage due to their high theoretical energy density (2600 Wh kg⁻¹), low cost, and non-toxic nature. However, practical implementation faces challenges, primarily from Li polysulfide (LiPS) shuttling within the cathode and Li dendrite growth at the anode. Optimized electrodes/electrolytes design effectively confines LiPS to the cathode, boosting cycling performance in coin cells to up to hundreds of cycles. Scaling up to larger pouch cells presents new obstacles, requiring further research for long-term stability. A 1.45 Ah pouch cell, with optimized sulfur loading and electrolyte/sulfur ratio is developed, which delivers an energy density of 151 Wh kg-1 with 70% capacity retention up to 100 cycles. Targeting higher energy density (180 Wh kg-1), the developed 1Ah pouch cell exhibits 68% capacity retention after 50 cycles. Morphological analysis reveals that pouch cell failure is primarily from Li metal powdering and resulting polarization, rather than LiPS shuttling. This occurs for continuous Li ion stripping/plating during cycling, leading to dendrite growth and formation of non-reactive Li powder, especially under high currents. These issues increase ion diffusion resistance and reduce coulombic efficiency over time. Therefore, the study highlights the importance of a protected Li metal anode for achieving high-energy-dense batteries.

8.
Small ; 20(40): e2402725, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-38837316

RESUMO

Unveiling the inherent link between polysulfide adsorption and catalytic activity is key to achieving optimal performance in Lithium-sulfur (Li-S) batteries. Current research on the sulfur reaction process mainly relies on the strong adsorption of catalysts to confine lithium polysulfides (LiPSs) to the cathode side, effectively suppressing the shuttle effect of polysulfides. However, is strong adsorption always correlated with high catalysis? The inherent relationship between adsorption and catalytic activity remains unclear, limiting the in-depth exploration and rational design of catalysts. Herein, the correlation between "d-band center-adsorption strength-catalytic activity" in porous carbon nanofiber catalysts embedded with different transition metals (M-PCNF-3, M = Fe, Co, Ni, Cu) is systematically investigated, combining the d-band center theory and the Sabatier principle. Theoretical calculations and experimental analysis results indicate that Co-PCNF-3 electrocatalyst with appropriate d-band center positions exhibits moderate adsorption capability and the highest catalytic conversion activity for LiPSs, validating the Sabatier relationship in Li-S battery electrocatalysts. These findings provide indispensable guidelines for the rational design of more durable cathode catalysts for Li-S batteries.

9.
Small ; 20(1): e2304847, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37658511

RESUMO

The "shuttle effect" and slow redox reactions of Li-S batteries limit their practical application. To solve these problems, a judicious catalyst design for improved battery cycle life and rate performance is essential. Herein, this issue is addressed by modifying the Li-S battery separator using a 2D Fe2 O3 -CoP heterostructure that combines the dual functions of polar Fe2 O3 and high-conductivity CoP. The synthesized ultrathin nanostructure exposes well-dispersed active sites and shortens the ion diffusion paths. Theoretical calculations, electrochemical tests, and in situ Raman spectroscopy measurements reveal that the heterostructure facilitates the inhibition of polysulfide shuttling and enhances the electrode kinetics. A sulfur cathode constructed using the Fe2 O3 -CoP-based separator provides an astonishing capacity of 1346 mAh g-1 at 0.2 C and a high capacity retention of ≈84.5%. Even at a high sulfur loading of 5.42 mg cm-2 , it shows an area capacity of 5.90 mAh cm-2 . This study provides useful insights into the design of new catalytic materials for Li-S batteries.

10.
Small ; 20(8): e2306159, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37840442

RESUMO

2D metal-organic frameworks (2D MOFs) with π conjugation have attracted widespread attention in the field of lithium storage due to their unique electron transfer units and structural characteristics. However, the periodic 2D planar extension structure hides some active sites, which is not conducive to the utilization of its structural advantages. In this work, a series of triptycene-based 2D conductive MOFs (M-DBH, M = Ni, Mn, and Co) with 3D extension structures are constructed by coordinating 9,10-dihydro-9,10-[1,2]benzenoanthracene-2,3,6,7,14,15-hexaol with metal ions to explore their potential applications in lithium-ion and lithium-sulfur batteries. This is the first study in which 2D conductive MOFs with the 3D extended molecule are used as electrode materials for lithium storage. The designed material generates rich active sites through staggered stacking layers and shows excellent performance in lithium-ion and lithium-sulfur batteries. The capacity retention rate of Ni-DBH can reach over 70% after 500 cycles at 0.2 C in lithium-ion batteries, while the capacity of S@Mn-DBH exceeds 305 mAh g-1 after 480 cycles at 0.5 C in lithium-sulfur batteries. Compared with the materials with 2D planar extended structures, the M-DBH electrodes with 3D extended structures in this work exhibit better performance in terms of cycle time and lithium storage capacity.

11.
Small ; : e2404917, 2024 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-39324285

RESUMO

Lithium-sulfur (Li-S) battery is a potential next-generation energy storage technology over lithium-ion batteries for high capacity, cost-effective, and environmentally friendly solutions. However, several issues including polysulfides shuttle, low conductivity and limited rate-capability have hampered its practical application. Herein, a new class of cathode active material with perfect core-shell structure is reported, in which sulfur is fully encapsulated by conductivity-enhancing FeS2 (named as S@FeS2), for high-rate application. Surface-stabilized S@FeS2 cathode exhibits a stable cycling performance under 2 - 20 times higher rates (1-2 C, charged in 30-60 min) than standard rates (e.g., 0.1-0.5 C, charged in 2-10 h), without polysulfides shuttle event. Surface analysis results reveal the unprecedented formation of a stable solid electrolyte interphase (SEI) layer on S@FeS2 cathode, which is distinguished from other sulfur-based cathodes that are not able to form the SEI layer. The data suggest that the prevention of polysulfides shuttling is owing to the surface protection effect of FeS2 shell and the SEI layer formation overlying core-shell S@FeS2. This unique and potential material concept proposed in the present study will give insight into designing a prospective fast charging Li-S battery.

12.
Chemphyschem ; : e202400415, 2024 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-39258451

RESUMO

In Lithium sulfur (Li-S) batteries the sulfur host material is a significant area of research that could impart enhanced conductivity and alleviate the shuttling of polysulfides. In the present study, graphene oxide- sulfur, GOS was synthesized in melt diffusion method by exploring the two different strategies: Ambient (G2-M) and Inert (G2-T) conditions. Within the cathode, efficient storage of S with sufficient space in GO interlayers was outperformed by G2-T method.  Further with PEDOT nanostructures enveloped by oxidative polymerisation proves to be a robust conductive layer and an adsorbing agent. It is evidenced physic chemically by XRD, FTIR, TGA, HR-SEM. Moreover, in addition to the supporting studies, high binding energies at 168.3 and 169.5 eV confirms the superior performance for PEDOT/GO-S (G3T) as best cathode within the system. The electrochemical behaviour of G3-T possess very low cell impedance with an excellent cyclic reversibility in CV during (de)lithiation process. At 0.1 C, an initial discharge capacity of 868 mAh g-1 has been achieved confirming a high catalytic activity with a low polarisation potential of (∆E=0.25) inducing fast reaction kinetics. Thus potential locking of sulfur under inert condition is explored with a proven OCV of 2.3 V with red LED glow.

13.
Nanotechnology ; 35(21)2024 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-38377620

RESUMO

Lithium-sulfur (Li-S) batteries exhibit a huge potential in energy storage devices for the thrilling theoretical energy density (2600 Wh kg-1). Nevertheless, the serious shuttle effect rooted in polysulfides and retardative hysteresis reaction kinetics results in inferior cycling and rate performances of Li-S batteries, impeding commercial applications. In order to further promote the energy storage abilities of Li-S batteries, a unique binder-free sulfur carrier consisting of SnS2-modified multi-hole carbon nanofibers (SnS2-MHCNFs) has been constructed, where MHCNFs can offer abundant space to accommodate high-level sulfur and SnS2can promote the adsorption and catalyst capability of polysulfides, synergistically promoting the lithium-ion storage performances of Li-S batteries. After sulfur loading (SnS2-MHCNFs@S), the material was directly applied as a cathode electrode of the Li-S battery. The SnS2-MHCNFs@S electrode maintained a good discharge capacity of 921 mAh g-1after 150 cycles when the current density was 0.1 C (1 C = 1675 mA g-1), outdistancing the MHCNFs@S (629 mAh g-1) and CNFs@S (249 mAh g-1) electrodes. Meanwhile, the SnS2-MHCNFs@S electrode still exhibited a discharge capacity of 444 mAh g-1at 2 C. The good performance of SnS2-MHCNFs@S electrode indicates that combining multihole structure designation and polar material modification are highly effective methods to boost the performances of Li-S batteries.

14.
Angew Chem Int Ed Engl ; : e202417624, 2024 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-39345165

RESUMO

Regulating the transformation of sulfur species is the key to improving the electrochemical performance of lithium-sulfur (Li-S) batteries, in particular, to accelerate the reversible conversion between solid phase Li2S2 and Li2S. Herein, we introduced Spidroin, which is a main protein in spider silk, as a dual functional separator coating in Li-S batteries to effectively adsorb polysulfides via the sequence of amino acids in its primary structure and regulate Li+ flux through the ß-sheet of its secondary structure, thus accelerating the reversible transformation between Li2S2 and Li2S. Spidroin-based Li-S cells exhibited an exceptional electrochemical performance with a high specific capacity of  744.1 mAh g-1 at 5C and a high areal capacity of 7.5 mAh cm-2 at a low electrolyte-to-sulfur (E/S) ratio of 6 µL mgs-1 and a sulfur loading of 8.6 mgs cm-2.

15.
Angew Chem Int Ed Engl ; : e202413670, 2024 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-39295281

RESUMO

All-solid-state Li-S batteries (ASSLSBs) due to high theoretical energy density and exceptional safety are highly desirable for electric aircraft. However, as the flight altitude rises, the low-temperature performance is hampered by inadequate practical capacity. Here, we discover that low-temperature sulfur utilization is constrained by the multi-step endothermic conversion reaction. By introducing multi-chalcogen to modulate the local entropy, a short-chain molecule cathode is designed to shorten the reduction pathways and enhance low-temperature discharge capacity. Furthermore, the mismatched lithiation lattice of the short-chain cathode reduces the decomposition energy barriers, thus enhancing low-temperature charge/discharge reversibility. The designed short-chain cathode exhibits high cathode utilization (99.4%) and cycling stability (400 cycles, 92.2% retention) at room temperature, as well as delivers excellent discharge capacity (579.6 mAh g-1, -40 °C) and cycling performance (100 cycles, 98.4% retention, 394.9 Wh kg-1electrode, -20 °C) at low temperature. This study presents new opportunities to stimulate the development of low-temperature ASSLSBs.

16.
Small ; 19(42): e2303266, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37292047

RESUMO

Lithium-sulfur (Li-S) batteries with high energy density and low cost are the most promising competitor in the next generation of new energy reserve devices. However, there are still many problems that hinder its commercialization, mainly including shuttle of soluble polysulfides, slow reaction kinetics, and growth of Li dendrites. In order to solve above issues, various explorations have been carried out for various configurations, such as electrodes, separators, and electrolytes. Among them, the separator in contact with both anode and cathode is in a particularly special position. Reasonable design-modified material of separator can solve above key problems. Heterostructure engineering as a promising modification method can combine characteristics of different materials to generate synergistic effect at heterogeneous interface that is conducive to Li-S electrochemical behavior. This review not only elaborates the role of heterostructure-modified separators in dealing with above problems, but also analyzes the improvement of wettability and thermal stability of separators by modification of heterostructure materials, systematically clarifies its advantages, and summarizes some related progress in recent years. Finally, future development direction of heterostructure-based separator in Li-S batteries is given.

17.
Small ; 19(48): e2303015, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37582643

RESUMO

Preparing MoS2 -based materials with reasonable structure and catalytic activity to enhance the sluggish kinetics of lithium polysulfides (LiPSs) conversion is of great significance for Li-S batteries (LSBs) but still remain a challenge. Hence, hollow nanotubes composed of N-doped ultrathin MoS2 nanosheets (N-MoS2 NHTs) are fabricated as efficient S hosts for LSBs by using CdS nanorods as a sacrifice template. Characterization and theoretical results show that the template effectively inhibits the excessive growth of MoS2 sheets, and N doping expands the interlayer spacing and modulates the electronic structure, thus accelerating the mass/electron transfer and enhancing the LiPSs adsorption and transformation. Benefiting from the merits, the N-MoS2 NHTs@S cathode exhibits an excellent initial capacity of 887.8 mAh g-1 and stable cycling performances with capacity fading of only 0.0436% per cycle at 1.0 C (500 cycles). Moreover, even at high S loading that of 7.5 mg cm-2 , the N-MoS2 NHTs@S cathode also presents initial excellent areal capacity of 7.80 mAh cm-2 at 0.2 C. This study offers feasible guidance for designing advanced MoS2 -based cathode materials in LSBs.

18.
Small ; 19(49): e2303784, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37612805

RESUMO

Li-S batteries are regarded as promising devices for energy storage systems owing to high energy density, low cost, and environmental friendliness. However, challenges of polysulfides shuttling in sulfur cathode and dendrite growth of lithium anode severely hinder the practical application. Developing advanced skeletons simultaneously regulating the cathode and anode is significant and challenging. Hence, a novel and scalable strategy combining spray drying and topological nitriding is proposed, and hierarchically assembled rGO hollow microspheres encapsulated highly porous nanospheres consisted of ultrafine Nb4 N5 -Nb2 O5 or Nb4 N5 nanoparticles as multifunctional skeletons for S and Li are designed. In such unique architecture, a 3D highly porous structure provides abundant void space for loading of S and Li, and accommodates volume change during cycling. Moreover, Nb4 N5 -Nb2 O5 heterostructured interface promotes adsorption-conversion process of polysulfides, while strong lithophilic Nb4 N5 induces the selective infiltration of Li into the void of the skeleton and regulates the uniform deposition and growth. More interestingly, in situ generated Li3 N@Nb ion/electron conducting interfaces induced by the reaction of Nb4 N5 and Li reduce the nucleation overpotential and induce selective deposition of Li into the cavity. Consequently, the Li-S full cell exhibits superior cycling stability and impressive rate performance with a low capacity ratio of negative/positive.

19.
Small ; 19(5): e2206616, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36440668

RESUMO

Anisotropically hybridized porous crystalline Li-S battery separators based on porous crystalline materials that can meet the multiple functionalities of both anodic and cathodic sides are much desired for Li-S battery yet still challenging in directional design. Here, an anisotropically hybridized separator (CPM) based on an ionic liquid-modified porphyrin-based covalent-organic framework (COF-366-OH-IL) and catalytically active metal-organic framework (Ni3 (HITP)2 ) that can integrate the lithium-polysulfides (LiPSs) adsorption/catalytic conversion and ion-conduction sites together to directionally meet the requirements of electrodes is reported. Remarkably, the-obtained separator exhibits an exceptional high Li+ transference-number (tLi+  = 0.8), ultralow polarization-voltage (<30 mV), high initial specific-capacity (921.38 mAh g-1 at 1 C), and stable cycling-performance, much superior to polypropylene and monolayer-modified separators. Moreover, theoretical calculations confirm the anisotropic effect of CPM on the anodic side (e.g., Li+ transfer, LiPSs adsorption, and anode-protection) and cathodic side (e.g., LiPSs adsorption/catalysis). This work might provide a new perspective for separator exploration.

20.
Small ; 19(5): e2205525, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36433827

RESUMO

Lithium-sulfur battery suffers from sluggish kinetics at low temperatures, resulting in serious polarization and reduced capacity. Here, this work introduces medium-entropy-alloy FeCoNi as catalysts and carbon nanofibers (CNFs) as hosts. FeCoNi nanoparticles are in suit synthesized in cotton-derived CNFs. FeCoNi with atomic-level mixing of each element can effectively modulate lithium polysulfides (LiPSs), multiple components making them promising to catalyze more LiPSs species. The higher configurational entropy endows FeCoNi@CNFs with extraordinary electrochemical activity, corrosion resistance, and mechanical properties. The fractal structure of CNFs provides a large specific surface area, leaving room for volume expansion and Li2 S accumulation, facilitating electrolyte wetting. The unique 3D conductive network structure can suppress the shuttle effect by physicochemical adsorption of LiPSs. This work systematically evaluates the performance of the obtained Li2 S6 /FeCoNi@CNFs electrode. The initial discharge capacity of Li2 S6 /FeCoNi@CNFs reaches 1670.8 mAh g-1 at 0.1 C under -20 °C. After 100 cycles at 0.2 C, the capacity decreases from 1462.3 to 1250.1 mAh g-1 . Notably, even under -40 °C at 0.1 C, the initial discharge capacity of Li2 S6 /FeCoNi@CNFs still reaches 1202.8 mAh g-1 . After 100 cycles at 0.2 C, the capacity retention rate is 50%. This work has important implications for the development of low-temperature Li-S batteries.

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