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1.
Angew Chem Int Ed Engl ; : e202404738, 2024 Apr 18.
Article in English | MEDLINE | ID: mdl-38634674

ABSTRACT

Electrocatalytic carbon dioxide reduction reaction (CO2RR) to produce ethylene (C2H4) is conducive to sustainable development of energy and environment. At present, most electrocatalysts for C2H4 production are limited to the heavy metal copper, meanwhile, achieving metal-free catalysis remains a challenge. Noted piperazine with sp3 N hybridization is beneficial to CO2 capture, but CO2RR performance and mechanism have been lacking. Herein, based on linkage engineering, we construct a novel high-density sp3 N catalytic array via introducing piperazine into the crystalline and microporous aminal-linked covalent organic frameworks (COFs). Thanks to its high sp3 N density, strong CO2 capture capacity and great hydrophilicity, aminal-linked COF successfully achieves the conversion of CO2 to C2H4 with a Faraday efficiency up to 19.1%, which is stand out in all reported metal-free COF electrocatalysts. In addition, a series of imine-linked COFs are synthesized and combined with DFT calculations to demonstrate the critical role of sp3 N in enhancing the kinetics of CO2RR. Therefore, this work reveals the extraordinary potential of linkage engineering in COFs to break through some catalytic bottlenecks.

2.
ACS Appl Mater Interfaces ; 16(14): 17637-17648, 2024 Apr 10.
Article in English | MEDLINE | ID: mdl-38549247

ABSTRACT

Aqueous zinc-ion batteries (ZIBs) are competitive among the elective candidates for electrochemical energy storage systems, but the intrinsic drawbacks of zinc metal anodes such as dendrites and corrosion severely hinder their large-scale application. Developing alternative anode materials capable of high reversibility and stability for storing Zn2+ ions is a feasible approach to circumvent the challenge. Herein, a sulfur-defect-induced TiS1.94 (D-TiS1.94) as a promising intercalation anode material for ZIBs is designed. The abundant Zn2+-storage active sites and lower Zn2+ migration barrier induced by sulfur defects endow D-TiS1.94 with a high capacity for Zn2+-storage (219.1 mA h g-1 at 0.05 A g-1) and outstanding rate capability (107.3 mA h g-1 at 5 A g-1). In addition, a slight volume change of 8.1% is identified upon Zn2+ storage, which favors a prolonged cycling life (50.3% capacity remaining in 1500 cycles). More significantly, the D-TiS1.94||ZnxMnO2 full battery demonstrates a high discharge capacity of 155.7 mA h g-1 with a capacity retention of 59.8% in 400 cycles. It has been estimated that the high-capacity, low-operation voltage, and long-life D-TiS1.94 can be a promising component of the ZIB anode material family, and the strategy proposed in this work will provide guidance to the defect engineering of high-performance electrode materials toward energy storage applications.

3.
ACS Nano ; 2024 Feb 09.
Article in English | MEDLINE | ID: mdl-38334264

ABSTRACT

Multivalent cation batteries are attracting increasing attention in energy-storage applications, but reversible storage of highly polarizing multivalent cations is a major difficulty for the electrode materials. In the present study, charge-delocalizing Mo3S13 cluster-based materials (crystalline (NH4)2Mo3S13 and amorphous MoSx) are designed and investigated as cathodes for rechargeable magnesium batteries. Both of the cathodes show high magnesium storage capacities (296 and 302 mAh g-1 at 100 mA g-1) and superior rate performances (76 and 80 mAh g-1 at 15 A g-1). A high area loading of 3.0 mg cm-2 could be achieved. These performances are of the highest level compared with those of reported magnesium storage materials. Further mechanism study and theoretical computation demonstrate the magnesium storage active sites are the bridging disulfur groups of the Mo3S13 cluster. The valence state of bridging disulfur decreases/increases largely during magnesiation/demagnesiation along with breaking/formation of the sulfur-sulfur bond, which makes the Mg-association/dissociation highly reversible. The sulfur-sulfur bond breaking and formation provides high reversible capacities. Prominently, the valence state increase and sulfur-sulfur bond formation of the bridging disulfur during charge weakens the bonding with Mg2+, significantly assisting the magnesium dissociation. The present study not only develops high-performance magnesium storage cathode materials but also demonstrates the importance of constructing favorable magnesium storage active sites in the high-performance cathode materials design. The findings presented herein are of great significance for the development of electrode materials for the storage of multivalent cations.

4.
Angew Chem Int Ed Engl ; 63(10): e202316966, 2024 Mar 04.
Article in English | MEDLINE | ID: mdl-38217483

ABSTRACT

LiPF6 as a dominant lithium salt of electrolyte is widely used in commercial rechargeable lithium-ion batteries due to its well-balanced properties, including high solubility in organic solvents, good electrochemical stability, and high ionic conductivity. However, it suffers from several undesirable properties, such as high moisture sensitivity, thermal instability, and high cost. To address these issues, herein, we propose an electron-donation modulation (EDM) rule for the development of low-cost, sustainable, and electrochemically compatible LiNO3 -based electrolytes. We employ high donor-number solvents (HDNSs) with strong electron-donation ability to dissolve LiNO3 , while low donor-number solvents (LDNSs) with weak electron-donation ability are used to regulate the solvation structure to stabilize the electrolytes. As an example, we design the LiNO3 -DMSO@PC electrolyte, where DMSO acts as an HDNS and PC serves as an LDNS. This electrolyte exhibits excellent electrochemical compatibility with graphite anodes, as well as the LiFePO4 and LiCoO2 cathodes, leading to stable cycling over 200 cycles. Through spectroscopy analyses and theoretical calculation, we uncover the underlying mechanism responsible for the stabilization of these electrolytes. Our findings provide valuable insights into the preparation of LiNO3 -based electrolytes using the EDM rule, opening new avenues for the development of advanced electrolytes with versatile functions for sustainable rechargeable batteries.

5.
Angew Chem Int Ed Engl ; 63(10): e202317439, 2024 Mar 04.
Article in English | MEDLINE | ID: mdl-38251812

ABSTRACT

Chemical presodiation (CP) is an effective strategy to enhance energy density of sodium ion batteries. However, the sodiation reagents reported so far are basically polycyclic aromatic hydrocarbons (PAHs) wth low reductive potential (~0.1 V vs. Na+ /Na), which could easily cause over-sodiation and structural deterioration of the presodiated cathodes. In this work, Aromatic ketones (AKs) are rationally designed as mild presodiating reagents by introducing a carbonyl group (C=O) into PAHs to balance the conjugated and inductive effect. As the representatives, two compounds 9-Fluorenoneb (9-FN) and Benzophenone (BP) manifest favorable equilibrium potential of 1.55 V and 1.07 V (vs. Na+ /Na), respectively. Note that 9-FN demonstrates versatile presodiating capability toward multiple Na uptake hosts (tunneled Na0.44 MnO2 , layered Na0.67 Ni0.33 Mn0.67 O2 , polyanionic Na4 Fe2.91 (PO4 )2 P2 O7 , Na3 V2 (PO4 )3 and Na3 V2 (PO4 )2 F3 ), enabling greatly improved initial charging capacity of the cathode to balance the irrevisible capacity of the anode. Our results indicate that the Aromatic ketones are competitive presodiating cathodic reagents for high-performance sodium-ion batteries, and will inspire more studies and application attempts in the future.

6.
Adv Mater ; 36(5): e2308881, 2024 Feb.
Article in English | MEDLINE | ID: mdl-37921499

ABSTRACT

Low-temperature performance of lithium-ion batteries (LIBs) has always posed a significant challenge, limiting their wide application in cold environments. In this work, the high-performance LIBs working under ultralow-temperature conditions, which is achieved by employing the weak-solvation and low-viscosity isobutyronitrile as a cosolvent to tame the affinity between solvents and lithium ions, is reported. The as-prepared electrolytes exhibit a sufficiently high conductivity (1.152 mS cm-1 ) at -70 °C. The electrolytes enable LiCoO2 cathode and graphite anode to achieve high Coulombic efficiency of >99.9% during long-term cycling at room temperature, and to respectively achieve 75.8% and 100.0% of their room-temperature capacities at -40 °C. Even the LiCoO2 //graphite pouch cells can retain 68.7% of the room-temperature capacity when discharged at -70 °C, and present stable cycling performance at -40 and 60 °C. This work provides a solution for the development of advanced electrolytes to enable LIBs working at wide-temperatures range.

7.
Angew Chem Int Ed Engl ; 62(47): e202312373, 2023 Nov 20.
Article in English | MEDLINE | ID: mdl-37806968

ABSTRACT

The solvation structure of Li+ plays a significant role in determining the physicochemical properties of electrolytes. However, to date, there is still no clear definition of the solvating power of different electrolyte solvents, and even the solvents that preferentially participate in the solvation structure remain controversial. In this study, we comprehensively discuss the solvating power and solvation process of Li+ ions using both experimental characterizations and theoretical calculations. Our findings reveal that the solvating power is dependent on the strength of the Li+ -solvent (ion-dipole) interaction. Additionally, we uncover that the anions tend to enter the solvation sheath in most electrolyte systems through Li+ -anion (ion-ion) interaction, which is weakened by the shielding effect of solvents. The competition between the Li+ -solvent and Li+ -anion interactions ultimately determines the final solvation structures. This insight into the fundamental understanding of the solvation structure of Li+ provides inspiration for the design of multifunctional mixed-solvent electrolytes for advanced batteries.

8.
Chem Sci ; 14(30): 8206-8213, 2023 Aug 02.
Article in English | MEDLINE | ID: mdl-37538828

ABSTRACT

Aqueous zinc-ion batteries (AZIBs) with excellent safety, low-cost and environmental friendliness have great application potential in large-scale energy storage systems and thus have received extensive research interest. Layered oxovanadium phosphate dihydrate (VOPO4·2H2O) is an appealing cathode for AZIBs due to the unique layered framework and desirable discharge plateau, but bottlenecked by low operation voltage and unstable cycling. Herein, we propose delta-oxovanadium phosphate (δ-VOPO4) without conventional pre-embedding of metal elements or organics into the structure and paired it into AZIBs for the first time. Consequently, superior to the layered counterpart, δ-VOPO4 exhibits better performance with a prominent discharge voltage of 1.46 V and a higher specific capacity of 122.6 mA h g-1 at 1C (1C = 330 mA g-1), as well as an impressive capacity retention of 90.88 mA h g-1 after 1000 cycles under 10C. By investigation of structure resolution and theoretical calculation, this work well elucidates the structure-function relationship in vanadyl phosphates, offering more chances for exploration of new cathode materials to construct high performance AZIBs.

9.
Sci Bull (Beijing) ; 68(17): 1894-1903, 2023 Sep 15.
Article in English | MEDLINE | ID: mdl-37544880

ABSTRACT

Fe-based polyanionic sulfate materials are one of the most promising candidates for large-scale applications in sodium-ion batteries due to their low cost and excellent electrochemical performance. Although great achievements have been gained on a series of Na6-2xFex(SO4)3 (NFSO-x, 1.5 ≤ x ≤ 2.0) materials such as Na2Fe2(SO4)3, Na2Fe1.5(SO4)3, and Na2.4Fe1.8(SO4)3 for sodium storage, the phase and structure characteristics on these NFSO-x are still controversial, making it difficult to achieve phase-pure materials with optimal electrochemical properties. Herein, six NFSO-x samples with varied x are investigated via both experimental methods and density functional theory calculations to analyze the phase and structure properties. It reveals that a pure phase exists in the 1.6 ≤ x ≤ 1.7 region of the NFSO-x, and part of Na ions tend to occupy Fe sites to form more stable frameworks. The NFSO-1.7 exhibits the best electrochemical performance among the NFSO-x samples, delivering a high discharge capacity (104.5 mAh g-1 at 0.1 C, close to its theoretical capacity of 105 mAh g-1), excellent rate performance (81.5 mAh g-1 at 30 C), and remarkable cycle stability over 10,000 cycles with high-capacity retention of 72.4%. We believe that the results are useful to clarify the phase and structure characteristics of polyanionic materials to promote their application for large-scale energy storage.

10.
Phys Chem Chem Phys ; 25(33): 22497-22504, 2023 Aug 23.
Article in English | MEDLINE | ID: mdl-37581354

ABSTRACT

Hybrid Mg2+/A+ (A = Li, K, or Na) batteries are promising energy-storage devices combining the merits of a metallic Mg anode and A+ intercalation cathodes. Mg2+/Li+ co-intercalations into the cathodes have been reported, and it is believed that Li-intercalation would reduce the activation energy of the Mg-intercalation and improve the kinetics. Herein, a new understanding of the Mg2+/Li+ and Mg2+/Na+ co-intercalations is revealed for layered TiS2 from the point of view of the thermodynamics and kinetics. In addition to Li-, Na- and Mg-intercalations, Mg-Li (Mg-Na) mixed and Mg-Li (Mg-Na) interlaced intercalations can also be observed. The Mg-Li (Mg-Na) mixed intercalation is co-intercalation of Mg2+ and Li+ (Na+) into the same TiS2 layer, whereas the Mg-Li (Mg-Na) interlaced intercalation means Mg2+ and Li+ (Na+), respectively, intercalate into the adjacent TiS2 layers. The Li- (Na-) intercalation has faster kinetics, whereas the Mg-Li (Mg-Na) interlaced intercalation structure is more stable thermodynamically. The Mg-Li and Mg-Na interlaced intercalations would gradually become the predominant principles of the TiS2-based hybrid Mg2+/Li+ and Mg2+/Na+ batteries, respectively. With this stabilization, both of the hybrid Mg2+/Li+ and Mg2+/Na+ batteries show high capacities, good rate capabilities and stable cycling.

11.
bioRxiv ; 2023 Jun 29.
Article in English | MEDLINE | ID: mdl-37425795

ABSTRACT

Epithelial-to-mesenchymal transition (EMT) contributes significantly to chemotherapy resistance and remains a critical challenge in treating advanced breast cancer. The complexity of EMT, involving redundant pro-EMT signaling pathways and its paradox reversal process, mesenchymal-to-epithelial transition (MET), has hindered the development of effective treatments. In this study, we utilized a Tri-PyMT EMT lineage-tracing model and single-cell RNA sequencing (scRNA-seq) to comprehensively analyze the EMT status of tumor cells. Our findings revealed elevated ribosome biogenesis (RiBi) during the transitioning phases of both EMT and MET processes. RiBi and its subsequent nascent protein synthesis mediated by ERK and mTOR signalings are essential for EMT/MET completion. Importantly, inhibiting excessive RiBi genetically or pharmacologically impaired the EMT/MET capability of tumor cells. Combining RiBi inhibition with chemotherapy drugs synergistically reduced metastatic outgrowth of epithelial and mesenchymal tumor cells under chemotherapies. Our study suggests that targeting the RiBi pathway presents a promising strategy for treating patients with advanced breast cancer. Significance: This study uncovers the crucial involvement of ribosome biogenesis (RiBi) in the regulation of epithelial and mesenchymal state oscillations in breast cancer cells, which plays a major role in the development of chemoresistant metastasis. By proposing a novel therapeutic strategy targeting the RiBi pathway, the study offers significant potential to enhance treatment efficacy and outcomes for patients with advanced breast cancer. This approach could help overcome the limitations of current chemotherapy options and address the complex challenges posed by EMT-mediated chemoresistance.

12.
Nanoscale ; 15(12): 5655-5664, 2023 Mar 23.
Article in English | MEDLINE | ID: mdl-36880871

ABSTRACT

Transition metal selenides are a research hotspot in sodium-ion batteries (SIBs). However, slow kinetics and rapid capacity decay due to volume changes during cycling limit their commercial applications. Heterostructures have the ability to accelerate charge transport and are widely used in energy storage devices due to their abundant active sites and lattice interfaces. A rational design of heterojunction electrode materials with excellent electrochemical performance is essential for SIBs. Herein, a novel anode material heterostructured FeSe2/MoSe2 (FMSe) nanoflower for SIBs was successfully prepared through a facile co-precipitation and hydrothermal route. The as-prepared FMSe heterojunction exhibits excellent electrochemical performance, including a high invertible capacity (493.7 mA h g-1 after 150 cycles at 0.2 A g-1), long-term cycling stability (352.2 mA h g-1 even after 4200 cycles at 5.0 A g-1) and competitive rate capability (361.2 mA h g-1 at 20 A g-1). By matching with a Na3V2(PO4)3 cathode, it can even exhibit ideal cycling stability (123.5 mA h g-1 at 0.5 A g-1 after 200 cycles). Furthermore, the sodium storage mechanism of the FMSe electrodes was systematically determined by ex situ electrochemical techniques. Theoretical calculation also reveals that the heterostructure on the FMSe interface enhances charge transport and promotes reaction kinetics.

13.
ACS Nano ; 16(12): 20510-20520, 2022 Dec 27.
Article in English | MEDLINE | ID: mdl-36410730

ABSTRACT

Rechargeable magnesium batteries (RMBs) are a promising large-scale energy-storage technology with low cost and high reliability. However, developing high-performance cathode materials remains the most prominent obstacle because of the insufficient magnesium-storage active sites and unfavorable magnesium cation transport paths, as well as the strong interaction between the cathode material and the bivalent magnesium cation. Herein, ammonium tetrathiomolybdate is demonstrated to be a high-performance RMB cathode material. Ammonium tetrathiomolybdate exhibits a high capacity of 333 mAh g-1 at 50 mA g-1 and a good rate performance of 129 mAh g-1 at 5.0 A g-1 (∼15 C). An amorphous structure with plenty of efficient magnesium-storage active sites and open magnesium transport paths is in situ formed during the first cycle via ammonium extraction. The covalent-like bond between the molybdenum and sulfur delocalizes the negative charge, weakening the interaction with the bivalent magnesium cation and accelerating the kinetics. The covalent-like molybdenum-sulfur bond also promotes the simultaneous redox of molybdenum and sulfur, leading to a high specific capacity. The present work introduces a high-capacity and high-power RMB cathode material, elucidates the origin of the high performance, and provides insights for the design and optimization of RMB cathode materials.

14.
ACS Appl Mater Interfaces ; 14(38): 43387-43396, 2022 Sep 28.
Article in English | MEDLINE | ID: mdl-36098664

ABSTRACT

Sodium metal is a promising anode for high-energy-density sodium rechargeable batteries (RSBs). However, the low Coulombic efficiency (CE) of the Na plating/stripping process and the problem of safety hinder their practical application. Herein, we report a facile strategy for employing the fluorinated phosphate solvents to realize highly reversible Na plating/stripping and improve the safety performance. The fluorinated phosphate molecules reduce the polarity of the solvent and lower the coordination number to Na+, which makes it possible to form the anion-induced ion-solvent-coordinated (AI-ISC) structures with high reduction tolerance. Moreover, the fluorination treatment enhances the oxidation resistance of the phosphate solvent, enabling compatibility with the high-voltage Na3V2(PO4)2F3 (NVPF) cathode. As expected, the Na@Al//NVPF full cell with the as-prepared 0.9 M NaFSI/tris(2,2,2-trifluoroethyl) phosphate (TFEP) demonstrates a capacity retention of 83.4% after 200 cycles with an average CE of 99.6%. This work opens a new avenue for designing high-energy-density RSBs with improved safety performance.

15.
Adv Mater ; 34(47): e2206039, 2022 Nov.
Article in English | MEDLINE | ID: mdl-36165216

ABSTRACT

The anionic redox reaction (ARR) has attracted extensive attention due to its potential to enhance the reversible capacity of cathode materials in Li/Na-ion batteries (LIBs/SIBs). However, the understanding of its activation mechanism is still limited by the insufficient mastering of the underlying thermodynamics and kinetics. Herein, a series of Mg/Li/Zn-substituted Nax MnO2 and Lix MnO2 cathode materials are designed to investigate their ARR behaviors. It is found that the ARR can be activated in only Li-substituted Lix MnO2 and not for Mg- and Zn-substituted ones, while all Mg/Li/Zn-substituted Nax MnO2 cathode materials exhibit ARR activities. Combining theoretical calculations with experimental results, such a huge difference between Li and Na cathodes is closely related to the migration of substitution ions from the transition metal layer to the alkali metal layer in a kinetic aspect, which generates unique Li(Na)-O-□TM and/or □Li/ Na -O-□TM configurations and reducing reaction activation energy to trigger the ARR. Based on these findings, an ion-migration mechanism is proposed to explain the different ARR behaviors between the Nax MnO2 and Lix MnO2 , which can not only reveal the origin of ARR in the kinetic aspect, but also provide a new insight for the development of high-capacity metal oxide cathode materials for LIBs/SIBs.

16.
ChemSusChem ; 15(12): e202200479, 2022 Jun 22.
Article in English | MEDLINE | ID: mdl-35384327

ABSTRACT

Metal-ion batteries have emerged as promising candidates for energy storage system due to their unlimited resources and competitive price/performance ratio. Vanadium-based compounds have diverse oxidation states rendering various open-frameworks for ions storage. To date, some vanadium-based polyanionic compounds have shown great potential as high-performance electrode materials. However, there has been a growing concern regarding the cost and environmental risk of vanadium. In this Review, all links in the industry chain of vanadium-based electrodes were comprehensively summarized, starting with an analysis of the resources, applications, and price fluctuation of vanadium. The manufacturing processes of the vanadium extraction and recovery technologies were discussed. Moreover, the commercial potentials of some typical electrode materials were critically appraised. Finally, the environmental impact and sustainability of the industry chain were evaluated. This critical Review will provide a clear vision of the prospects and challenges of developing vanadium-based electrode materials.

17.
Small ; 18(11): e2104876, 2022 Mar.
Article in English | MEDLINE | ID: mdl-35119209

ABSTRACT

Lithium (Li) metal is an excellent anode of Li ion batteries because of its high theoretical capacity and the low redox potential compared to other anodes. However, the uncontrollable growth of Li dendrites still incurs serious safety issues and poor electrochemical performances, leading to its limited practical application. An oxygen and boron codoped honeycomb carbon skeleton (OBHcCs) is reported and a stable Li metal-based anode is realized. It can be coated on a copper foil substrate to be used as a current collector for a dendrite-free Li metal anode. OBHcCs effectively reduces the local current density owing to the high surface area and inhibits Li dendrite growth, which is explored by scanning electron microscopy and an X-ray photoelectron spectra depth profile. The abundant lithiophilic oxygen and boron-containing functional groups reduce the potential barrier of nucleation and lead to the homogeneous Li ions flux as confirmed by the density functional theories. Therefore, the Li metal anode based on OBHcCs (OBHcCs@Li) stably runs for 700 h in a symmetric cell with a Li stripping capacity of 1 mAh cm-2 at 1 mA cm-2 . Furthermore, the OBHcCs@Li|LiFePO4 full cell shows a good capacity retention of 84.6% with a high coulombic efficiency of 99.6% at 0.5 C for 500 cycles.

18.
Small ; 18(10): e2106144, 2022 Mar.
Article in English | MEDLINE | ID: mdl-35038220

ABSTRACT

Solid phase conversion sulfur cathode is an effective strategy for eliminating soluble polysulfide intermediates (LiPSs) and improving cyclability of Li-S batteries. However, realizing such a sulfur cathode with high sulfur loading and high capacity utilization is very challenging due to the insulating nature of sulfur. In this work, a strategy is proposed for fabricating solid phase conversion sulfur cathode by encapsulating sulfur in the mesoporous channels of CMK-3 carbon to form a coaxially assembled sulfur/carbon (CA-S/C) composite. Vinyl carbonate (VC) is simultaneously utilized as the electrolyte cosolvent to in-situ form a dense solid electrolyte interface (SEI) on the CA-S/C composite surface through its nucleophilic reaction with the freshly generated polysulfides at the beginning of initial discharge, thus separating the direct contact of interior sulfur with the outer electrolyte. As expected, such a CA-S/C cathode can operate in a solid phase conversion manner in the VC-ether cosolvent electrolyte to exhibit a full capacity utilization (1667 mA h g-1 , ≈100%), a high rate capability of 2.0 A g-1 and excellent long-term cyclability over 500 cycles even at a high sulfur loading (75%, based on the weight of CA-S/C composite), demonstrating great promise for constructing high-energy-density and cycle-stable Li-S batteries.

19.
ACS Appl Mater Interfaces ; 14(1): 574-580, 2022 Jan 12.
Article in English | MEDLINE | ID: mdl-34936327

ABSTRACT

Propylene carbonate (PC)-based electrolytes have many attractive advantages over the commercially used ethylene carbonate (EC)-based electrolytes like a wider operating temperature and higher oxidation stability. Therefore, PC-based electrolytes become the potential candidate for lithium-ion batteries with higher energy density, longer lifespan, and better low- and high-temperature performance. In spite of the superiority, PC is incompatible with the graphite anode because PC fails to passivate the graphite anode, leading to severe decomposition and gas evolution, which seriously restrict the development of the PC-based electrolytes. Nevertheless, it is recently found that the usage of diethyl carbonate (DEC) as a cosolvent will greatly improve the anodic tolerance of PC to realize the reversible lithiation/delithiation of the graphite anode in the PC-based electrolyte. It is because DEC induces anions into the solvation shell of Li+ to form an anion-induced ion-solvent-coordinated (AI-ISC) structure with higher reduction stability. In this work, we fabricated 4.4 V pouch cells to assess in detail the practical viability of the PC-based electrolyte in a commercial battery system. In comparison to conventionally used EC-based cells, the pouch cells with the PC-based electrolyte exhibit more excellent high-voltage tolerance and electrochemical performance at all temperature ranges (-40 to 85 °C), demonstrating the wide application prospect of the PC-based electrolyte.

20.
Small Methods ; 5(8): e2100372, 2021 Aug.
Article in English | MEDLINE | ID: mdl-34927871

ABSTRACT

Sodium-ion battery has been considered as one of the most promising power sources for large-scale energy storage systems due to its similar electrochemistry to the lithium-ion battery and the crust abundance of Na resources. Essentially, developing low-cost electrode materials along with a facile and economical synthesis procedure is critically important to promote the commercialization of sodium-ion batteries. However, applicable cathode materials capable of being massively produced are still scarcely reported to date. Herein, a green and scalable synthesis approach is developed to obtain Na3 Fe2 (PO4 )P2 O7 (NFPP)/rGO composite by using FePO4 and Na3 PO4 as the resources, during which all the atoms present in the starting materials end up in the product. The prepared Na3 Fe2 (PO4 )P2 O7 /rGO cathode exhibits an ultralong cycle life (capacity retention of 72.4% after 8000 cycles at 20 C) and outstanding rate capability (42.4 mAh g-1 at 100 C). In particular, the NFPP/rGO-HC full battery assembled by the Na3 Fe2 (PO4 )P2 O7 /rGO cathode and hard carbon anode demonstrates an energy density of 192 Wh kg-1 and superior cycling performance (capacity retention of 85.2% after 500 cycles). These results will contribute to the development of sodium-ion batteries from applicable Na3 Fe2 (PO4 )P2 O7 /rGO cathode material.

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