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ELECTROCHIMICA ACTA · 2024 · IF 5.5

Entropy enhancement drived high initial Coulombic efficiency and capacity integrated SnS2 nanosheets for lithium-ion batteries

Rongzhang Yang,Hao Liang,Meiran Chen,Fengqi Lu

Layer SnS 2 has been garnered significant attention for next-generation lithium-ion batteries (LIBs), due to its abundant resources and high theoretical capacity. However, the low initial Coulombic efficiency, large volume expansion and structural degradation have significantly hindered its application in LIBs. Herein, the layer Sn 0.7 (MoFeCoNiV) 0.3 S 2 nanosheets (HE3-SnS 2 ) grown on the conductive substrate carbon cloth (CC) is synthesized by one-step hydrothermal method. Multiple elements doping strategy not only increases the conformational entropy which will improve the structural stability of during cycling, but also enlarges the interlayer spacing which benefits for lithium-ion transfer. As a result, the additive-free integrated CC@HE3-SnS 2 electrode achieves a high reversible specific capacity of 1204.9 mAh g −1 with a high initial Coulombic efficiency of 94.7 % at 1C, and maintains 1011.4 mAh g −1 after 100 cycles. Specifically, the CC@HE3-SnS 2 anode exhibits excellent rate capability of 670.8 mAh g −1 at 10C. Moreover, the full cell based on CC@HE3-SnS 2 anode and commercial LiCoO 2 cathode displays a stable capacity retention of 862.7 mAh g −1 after 100 cycles at 1C. The entropy-stabilized SnS 2 -based anode with high initial Coulombic efficiency and rate capability has a competitive candidate for LIBs.

CAS / MDL: 7803-55-6
研究领域: 材料科学 · 能源存储
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Energy Storage Materials · 2017 · IF 0

An ultra-stable and enhanced reversibility lithium metal anode with a sufficient O2 design for Li-O2 battery

Feilong Qiu,Xiaoyu Zhang,Yu Qiao,Xueping Zhang,Han Deng,Tianrui Shi,Ping He,Haoshen Zhou

Li metal is used as anode for Li–O 2 batteries because of its high specific capacity and low negative electrochemical potential. However, Li metal exhibits low Coulombic efficiency and limited cycle life, which hinder its practical use. In this study, we demonstrate that the performance of the Li metal anode was significantly improved by cycling in O 2 -rich electrolyte. In the presence of sufficient O 2 , the growth of Li dendrites was suppressed by the formation of flexible and mechanical strong solid electrolyte interphase layers. Consequently, Li metal anode remained stable over 800 cycles with 98.7% Coulombic efficiency. The origination of the superior performance was further analyzed through ion etching-assisted XPS and in situ electrochemical Raman spectroscopy . Our research provides a distinct and effective approach used to improve the stability and reversibility of Li metal anodes and reveal the superiority of Li metal systems in the presence of sufficient O 2 for Li-O 2 battery.

CAS / MDL: 110-71-4 7782-99-2
研究领域: 材料科学 · 电化学
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ADVANCED FUNCTIONAL MATERIALS · 2022 ·Vol. 32 ·期 40 ·2206615 · IF 19.924

Engineering Prelithiation of Polyacrylic Acid Binder: A Universal Strategy to Boost Initial Coulombic Efficiency for High-Areal-Capacity Si-Based Anodes

Zeheng Li,Weiting Tang,Yajun Yang,Guoyong Lai,Zheng Lin,Huayan Xiao,Juncheng Qiu,Xiujuan Wei,Shuxing Wu,Zhan Lin

The low initial Coulombic efficiency (ICE) and insufficient cycling lives of silicon (Si)-based anodes seriously hinder their eventual introduction into next-generation high-energy-density lithium–ion batteries (LIBs). Herein, an engineering prelithiation binder strategy based on polyacrylic acid (Li x PAA) is proposed for representative SiO x anodes. The ICEs and cycling lives of SiO x anodes are significantly improved by precisely controlling the lithiation degree of PAA binder. The ICE of the high-loading (3.0 mg cm −2 ) SiO x electrode increases by 10.9% when the Li 0.75 PAA binder replaces the PAA binder. Moreover, the working mechanism of the lithiation binder strategy to improve the electrochemical performances (especially for ICE) is systematically investigated, which is universally applied to other Si anodes such as Si nanoparticles and Si/graphite. This universal binder strategy and proposed working mechanism provide enlightenment on constructing high-ICE, high-energy-density, and long-life Si-based anodes.

CAS / MDL: 1310-66-3
研究领域: 材料科学 · 电化学
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CARBON · 2023 · IF 10.9

MOF-derived crystalline carbon with graphite-like crystal: A high initial coulombic efficiency, low potential and large capacity anode for Na-ion batteries

Xianwei Li,Zhenqian Wu,Xudong Ma,Ling Xin,Xiao Yu,Yong Liu

Carbonaceous materials , such as hard carbon and porous carbon , have gained great attentions as the anode materials for Na-ion batteries (NIBs). However, their defects and disordered structure cause the low initial coulombic efficiency (ICE), high-potential slope region and small charge capacity below 0.5 V. Herein, a structurally stable MOF contained 1,3,5-triazine-2,4,6-triamine moieties, belonging to the tetragonal space group I 4/m, is synthesized. On this basis, MOF-derived crystalline carbon with graphite-like crystal, instead of amorphous porous carbon, can be obtained due to slow pyrolysis of MOF framework along with timely and sufficient reassembly of the pyrolyzed carbon atoms into graphite-like crystal under graphite-induced condition. The graphite-like crystal has a geometrically similar unit cell to graphite crystal but with a magnification ratio of 1.25, yielding proportionally expanded d-spacing of (002) plane (4.2 Å), which enables the reversible Na + intercalation/de-intercalation. When applied in NIBs, it exhibits a very high ICE of 96.0% and reversible charge capacity of 356.2 mAh g −1 , reaching the advanced level of graphite applied in LIBs . More importantly, its charge capacity below 0.5 V can account for 90% of the total charge capacity, which is also the key parameter to effectively increase the energy density of full batteries.

研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

NaF-rich interphase and high initial coulombic efficiency of red phosphorus anode for sodium-ion batteries by chemical presodiation

Jiangping Song,Mengjun Wu,Kan Fang,Tian Tian,Rui Wang,Haolin Tang

Red phosphorus/carbon (P/C) materials have been extensively studied as promising anodes for sodium-ion batteries (SIBs) owing to their high capacities and moderate working potentials. However, the low initial Coulombic efficiency (ICE) and unstable solid-electrolyte interphase (SEI) of P/C composites limit their widespread applications. In this study, we develop an effective presodiation method to compensate for the irreversible sodium loss of the S-doped P/C (P/C@S) anode and yield a thin, uniform, and NaF-rich SEI layer on the presodiated P/C@S (pNa-P/C@S) anode during cycling. Consequently, the pNa-P/C@S anode exhibits a remarkable ICE of 98.7% as well as superior cycling performance and rate capability in the half cell. When pNa-P/C@S anode is coupled with conventional Na 3 V 2 (PO 4 ) 2 F 3 , Na 3 V 2 (PO 4 ) 3 , and NaCu 0.12 Ni 0.23 Fe 0.33 Mn 0.33 cathodes, all the full cells demonstrate desirable ICEs (>98%), high energy densities, and excellent cycling performance. The proposed method has been extended to another anode (SnO 2 ) to demonstrate its applicability in fabricating anodes with a high ICE and stable NaF-rich SEI layer.

研究领域: 材料科学 · 电化学
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Energy & Environmental Materials · 2020 ·Vol. 5 ·期 1 ·245-252 · IF 0

Carbon Supported MoO2 Spheres Boosting Ultra-Stable Lithium Storage with High Volumetric Density

Chunli Wang,Lianshan Sun,Bingbing Tian,Yong Cheng,Limin Wang

As important ingredients in lithium-ion battery, the Coulombic efficiency and power density greatly impact the electrochemical performances. Although recent literatures have reported nano-porous materials to enhance the specific capacities, intrinsic drawbacks such as poor initial Coulombic efficiency and low volumetric capacity could not be avoided. Herein, we propose a strategy to prepare carbon supported MoO 2 spheres used for lithium-ion battery with high volumetric capacity density. A high initial Coulombic efficiency of 76.5% is obtained due to limited solid electrolyte interface film formed on the exposed surface. Meantime, the sample with an optimal carbon content and a proper structural strength reveals a higher reversible capacity of 956 mA h g −1 than the theoretical capacity of crystalline MoO 2 (838 mA h g −1 ) and a high capacity retention ratio of 96.4% after 100 cycles at 0.5 A g −1 . And an effective compaction capacity density (under 5 MPa) of 670 mA h cm −3 of the spheres proves its potential value in practical applications.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 电池技术
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Nano Research · 2023 ·Vol. 16 ·期 6 ·8448-8456 · IF 9.9

Constructing a lithiophilic polyaniline coating via in situ polymerization for dendrite-free lithium metal anode

Xiong Xiaosong,Qiao Qiao,Zhou Qi,Cheng Xinbing,Liu Lili,Fu Lijun,Chen Yuhui,Wang Bin,Wu Xiongwei,Wu Yuping

Metallic lithium is regarded as one of the most promising electrode materials to break through the energy density bottleneck of current commercial lithium-ion batteries. However, the practical implementation of lithium metal anode is limited by the unstable electrode interface significantly, which directly induces a low Coulombic efficiency, short cycling lifespan, and dendritic lithium growth behavior. In this study, via in situ electropolymerization, lithiophilic and conformal polyaniline layer is developed to improve the initial lithium nucleation and plating process, reducing the interface charge transfer resistance and promoting uniform lithium plating/stripping behavior. Meanwhile, the polyaniline layer exhibits good adhesion to the substrate. As a result, the Li/Cu half cell delivers a high Coulombic efficiency of 99.1% for 400 cycles at 1.0 mA·cm −2 with polyaniline layer. In addition, long-term stable cycling at a current density of 1.0 mA·cm −2 for 1300 h has been achieved for lithium metal anode. This strategy provides a new perspective for the practical lithium metal batteries.

研究领域: 材料科学 · 电化学 · 电池技术
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Advanced Energy Materials · 2025 · IF 26

Repair Surface Defects on Biomass Derived Hard Carbon Anodes with N-Doped Soft Carbon to Boost Performance for Sodium-Ion Batteries

Jian Cui,Wenxiu Li,Panpan Su,Xuefen Song,Wendong Ye,Yongguang Zhang,Zhongwei Chen

Biomass-derived hard carbon (HC), a promising anode material for sodium-ion batteries with low cost and good cycling ability, has high surface activity that easily reacts with the electrolyte, causing low initial coulombic efficiency (ICE) and poor stability. This article proposes a facile synthesis of pine wood-derived HC material with N-doped soft carbon (SC) coating strategy to improve electrochemical performance, especially for the ICE. The optimized anode material exhibits higher reversible capacity of 314.0 mAh g −1 at 30 mA·g −1 with greatly enhanced ICE of 85.2%, and high rate performance of 260.0 mAh g −1 at 5.0 C. Combined with in situ/ex situ characterizations, SC coating greatly increased closed pores that is beneficial for improving sodium storage and the anode material is explored as a adsorption-filling sodium storage behavior, favoring the high-rate performance. Density functional theory (DFT) calculations further revealed that nitrogen doping in SC greatly enhanced the sodium adsorption kinetics and provides more adsorption sites for Na + storage, increasing sodium storage capacity. This work provides in-depth insights into the surface modification of hard carbon, and offers new opportunities for the design of efficient HC anodes.

CAS / MDL: 62-31-7 77-86-1
研究领域: 材料科学 · 电化学 · 能源存储
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Materials Today Chemistry · 2025 · IF 6.7

A polymeric three-dimensional adhesive network for a high initial Coulombic efficiency silicon anode

Siying Li,Zhengwei Wan,Zhuoying Wu,Dan Qian,Kun Wang,Xingyu Sun,Chuhan Zhou,Min Ling,Chengdu Liang

The inevitable side reactions during the cycling of silicon electrodes lead to the low initial Coulombic efficiencies. Binders play a vital role as a crucial component of electrodes in enhancing the initial Coulombic efficiencies in the cycling process. The water-soluble grafted CMC/PAA binder can form a three-dimensional adhesion network to cover Si particles. A large proportion of hydroxyl and carboxyl groups in the binder can generate a strong interaction with Si–OH bond to attach to the surface of Si particles. The dynamic cross-linked network helps to maintain the structural integrity of the electrodes while simultaneously enhancing the kinetics of lithium ion transportation. The Si@CMC/PAA electrode achieves a high initial Coulombic efficiency of 90.61 %, stable cycling performance and high rate capacity of 880 mAh·g −1 at 2 C.

研究领域: 材料科学 · 能源存储
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JOURNAL OF MEMBRANE SCIENCE · 2019 · IF 7.015

An interface-strengthened cross-linked graphene oxide/Nafion212 composite membrane for vanadium flow batteries

Daishuang Zhang,Qian Wang,Sangshan Peng,Xiaoming Yan,Xuemei Wu,Gaohong He

An interface-strengthened cross-linked graphene oxide/Nafion212 (CLGO/Nafion212) composite membrane was successfully fabricated and served as ion conducting membrane for vanadium flow batteries (VFBs). Firstly, the surface of Nafion212 was endowed with plenty of amino groups via in situ sol-gel chemistry approach of 3-aminopropyltriethoxysilane. Subsequently, a thin layer of m -xylylenediamino-crosslinked GO was formed using the spin-coating method. The composite membrane demonstrated much lower vanadium ion permeability (0.30 × 10 −6  cm 2  min −1 ) than pristine Nafion212 (1.88 × 10 −6  cm 2  min −1 ), mainly due to the presence of a cross-linked GO layer with angstrom-scale channels. The cell assembled with CLGO/Nafion212 exhibited enhanced coulombic efficiencies ( CE s, 93.0–97.2% vs. 68.0–91.6%) and energy efficiencies ( EE s, 88.9–85.2% vs. 65.7–82.2%) compared with the one with Nafion212 at 20–100 mA cm −2 . At a constant current density of 80 mA cm −2 , the long-term cycling tests showed that the discharge capacity fading of the flow cell equipped with CLGO/Nafion212 reached 0.25% per cycle, which was much smaller than that of Nafion212 (0.47% per cycle). The above findings proved that the cell equipped with CLGO/Nafion212 displayed superior electrochemical performances than that with Nafion212, therefore CLGO/Nafion212 composite membrane showed a great potential in VFBs.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Sol/Antisolvent Coating for High Initial Coulombic Efficiency and Ultra-stable Mechanical Integrity of Ni-Rich Cathode Materials

Xiaoqing Zhang,Jianwei Xiong,Fengzhen Chang,Zhuijun Xu,Zheng Wang,Philip Hall,Ya-Jun Cheng,Yonggao Xia

The Ni-rich cathode holds great promise for high energy density lithium-ion batteries because of its high capacity and operating voltage. However, crucial problems such as cation disorder, structural degradation, side reactions, and microcracks become serious with increasing nickel content. Herein, a novel and facile sol/antisolvent coating modification of Ni-rich layered oxide LiNi0.85Co0.1Mn0.05O2 (NCM) is developed where we use ethanol to disperse the nanosized LiBO2 to form the sol and adopt tetrahydrofuran (THF) as antisolvent to prepare the cluster of nanoparticles to be coated on the surface of NCM. The coating thickness can be tuned through the THF addition amount. The LiBO2 nanorod deposition is formed as well over the crack of the NCM cathode, likely acting as a patch to repair the original defect of the intrinsic crack. The uniform LiBO2 nanospherical particle coating together with LiBO2 nanorod wrapping provides a double protection against electrolytes. Compared with the raw material, LiBO2-coated LiNi0.85Co0.1Mn0.05O2 (LiBO2-coated NCM) exhibits a high initial Coulombic efficiency of 90.3% at 0.2 C between 2.8 and 4.3 V vs Li+/Li, a superior rate capability, enhanced fast charge property at 3 C, and restricted microcrack formation. This simple in-site modification and repairing technology guarantees a good mechanical integrity of the polycrystalline Ni-rich cathode.

CAS / MDL: 13453-69-5
研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

An ultra stable rice husk-based hard carbon using solid-electrolyte-binder containing sodium ion

Zhiqing Ge,Zhaoyong Chen,Huali Zhu,Yan Ji,Junfei Duan,Guang Zeng,Maohui Bai

Biomass-based hard carbon is a promising anode material for sodium-ion batteries (SIBs) because of its renewability, low cost and abundant porous structure. However, irreversible electrolyte consumption caused by hard carbon due to its large specific surface area and abundant structural defects is accompanied by a thick and uneven solid-electrolyte interphase (SEI), resulting in a low initial Coulombic efficiency (ICE) and rate performance of hard carbon anode. Therefore, an advanced sodium ion contained solid-electrolyte-binder (SSEB) with abundant hydrophilic functional groups is designed. The SSEB can uniformly cover the electrode surface by connecting oxygen-containing functional groups on the hard carbon surface, and the added polyethylene oxide (PEO) can construct ion diffusion paths to promote Na + transport. As a result, a SEI with a thickness of 9 nm has been obtained, and rice husk-based hard carbon with the SSEB provided high ICE (90.7 %) and capacity retention rate of 89.7 % after 2000 cycles at 3000 mA g −1 . The new design of Na  +  contained solid-electrolyte-binder open a door for the understand and application of hard carbon for sodium-ion batteries.

研究领域: 材料科学 · 能源技术
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