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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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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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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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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 16 ·7206-7220 · IF 9.931

A scalable ternary SnO2–Co–C composite as a high initial coulombic efficiency, large capacity and long lifetime anode for lithium ion batteries

Tao Liang,Renzong Hu,Houpo Zhang,Hanyin Zhang,Hui Wang,Yunpeng Ouyang,Jun Liu,Lichun Yang,Min Zhu

A new ternary SnO2–Co–C composite is produced using a facile and scalable ball milling method, which has a microstructure that includes refined SnO2–Co hybrids embedded in graphite. The Co additives dramatically inhibit Sn coarsening in the lithiated SnO2, which enables highly reversible conversion reactions in the SnO2-based ternary composite during cycling. The electrodes exhibit high ICEs with an average of 80.8% and a reversible capacity of 780 mA h g−1 at 0.2 A g−1 after 400 cycles when the composite was manufactured via small planetary ball milling, and they achieve 875 mA h g−1 after 250 cycles when the material is prepared on a large-scale with a roller mill. Even at a high rate of 2 A g−1, the composite has a long lifetime and delivers 610 mA h g−1 after 1000 cycles. Furthermore, a stable capacity of 410 mA h g−1 can be also retained in a full cell combined with a LiFePO4 cathode and SnO2–Co–C anode when cycling within 2.3–3.4 V at 0.2C. The new ternary SnO2–Co–C composite demonstrates excellent comprehensive electrochemical performances, and it is a promising candidate anode material for use in practical applications.

CAS / MDL: 7440-48-4 18282-10-5
研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2020 · IF 6.215

Good cycling stability and high initial efficiency demonstrated in full cells with limited lithium source for an advanced SnO2–Co–C composite anode

Gang Wen,Hui Liu,Tao Liang,Yunpeng Ouyang,Liang Tan,Renzong Hu,Jun Liu,Yao Zhang,Min Zhu

Despite there being many reports on SnO 2 -based anode materials, most of the electrode materials are tested in half cells using lithium metal with unlimited lithium-ion sources as the counter electrode, which may conceal the real properties of these composites to a certain extent. In this study, a ternary SnO 2 –Co–C composite was fabricated by a scalable ball milling strategy. The composite exhibited high initial Coulombic efficiency (ICE, >80%), a large capacity (∼900 mA h g −1 ) and superior cycling stability (capacity retention more than 99% after 100 cycles) in half cells. Furthermore, coin-type full cells in which the ternary SnO 2 –Co–C anodes were paired with different cathodes were demonstrated. A LiFePO 4 ||SnO 2 –Co–C full cell tested at 0.5–3.4 V exhibited an ICE of 75.1% and an initial discharge capacity of 906 mA h g −1 , which were close to those of the SnO 2 –Co–C||Li half cells. By analyzing the cycling performance and characteristics of the charge/discharge process for the full cells with different capacity ratios of cathode/anode, it was confirmed that the capacity decay of the full cells was due to the continuous consumption of Li + ions during cycling. Hence, the testing voltage windows were adjusted according to the lithiation/de-lithiation behavior of the SnO 2 . On this basis, the LiFePO 4 ||SnO 2 –Co–C full cells tested at 2.3–3.4 V and the LiCoO 2 ||SnO 2 –Co–C full cells tested at 2.60–3.75 V exhibited excellent cycling stability, demonstrating 80.3% and almost 100% capacity retention after 100 cycles, respectively, thereby laying a foundation for the practical application of advanced SnO 2 -based anodes in lithium-ion batteries.

CAS / MDL: 7440-48-4 18282-10-5
研究领域: 材料科学 · 电化学
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Scientific Reports · 2024 ·Vol. 14 ·期 1 ·1-12 · IF 3.8

Nonporous TiO2@C microsphere with a highly integrated structure for high volumetric lithium storage and enhance initial coulombic efficiency

Yin Jinpeng,Wang Guanqin,Kong Dongqing,Li Chuang,Zhang Qiang,Xie Dongbai,Yan Yangyang,Li Ning,Li Qiang

To enhance the volumetric energy density and initial coulombic efficiency (ICE) of titanium oxide (TiO 2 ) as anode electrode material for lithium-ion batteries (LIB), this study employed a surface-confined in-situ inter-growth mechanism to prepare a TiO 2 embedded carbon microsphere composite. The results revealed that the composite exhibited a highly integrated structure of TiO 2 with oxygen vacancies and carbon, along with an exceptionally small specific surface area of 11.52 m 2 /g. Due to its unique microstructure, the composite demonstrated remarkable lithium storage properties, including a high ICE of 75%, a notable capacity of 426.8 mAh/g after 200 cycles at 0.2 A/g, superior rate performance of 210.1 mAh/g at 5 A/g, and an outstanding cycle life, with a capacity decay rate of only 0.003% per cycle over 2000 cycles. Furthermore, electrochemical kinetic studies further validated the advantages of this microstructure.

研究领域: 材料科学 · 电化学
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ADVANCED FUNCTIONAL MATERIALS · 2021 ·Vol. 31 ·期 40 ·2104137 · IF 18.808

Rational Design of a Trifunctional Binder for Hard Carbon Anodes Showing High Initial Coulombic Efficiency and Superior Rate Capability for Sodium-Ion Batteries

Ji-Li Xia,An-Hui Lu,Xiao-Fei Yu,Wen-Cui Li

Hard carbon (HC) has emerged as a promising anode material for sodium-ion batteries (SIBs), whereas it suffers from low initial Coulombic efficiency (ICE) and poor rate capability. Binders endowed with high electron/ion transport and strong mechanical integrity are expected to boost the practical application of HC anodes, which cannot be realized via the functional design of commercially available binders. Herein, a trifunctional sodium alginate (SA)/polyethylene oxide (PEO) binder with massive hydrophilic functional groups and abundant Na + is synthesized via a feasible esterification reaction. The binder forms a passivation film on glucose-derived carbon (GC) to suppress the electrolyte decomposition and offer stronger adhesion strength. Furthermore, the sluggish Na + conduction is improved via sufficient ionic transfer channels provided by PEO. Notably, effects of Na + compensation and interfacial ionic transport of Na + -containing binder for HC anodes are revealed. Therefore, the SA/PEO binder for the GC anode delivers a high ICE up to 87% and a high capacity of 270 mA h g −1 at 0.1 A g −1 , both 10% and 80 mA h g −1 higher than that of poly(vinylidene fluoride) binder, respectively. Significantly, this SA/PEO binder can also be applied to coal-based and polymer-based carbon anodes, exhibiting universal applicability.

研究领域: 材料科学 · 电化学
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ChemElectroChem · 2019 ·Vol. 6 ·期 19 ·5060-5069 · IF 3.975

Phosphorization-Induced Void-Containing Fe3O4 Nanoparticles Enabling Low Lithiation/Delithiation Potential for High-Performance Lithium-Ion Batteries

Yan Nie,Hang Zhang,Jinfeng Zhang,Lei Wang,Siyu Zhong,Yinglong Wu,Junfei Duan,Huimin Shi,Kipkoech Kirui Victor,Guanhua Zhang,Huigao Duan

Graphical Don′t fill the void : A void-containing P−Fe 3 O 4 electrode derived from a phosphorization method exhibits a low lithiation/delithiation potential and high initial coulombic efficiency (80.8 % at 100 mA g −1 ) in the half-cell. The P−Fe 3 O 4 //NCM full-cell delivers a higher capacity (341 mAh g −1 ) than that of the Fe 3 O 4 //NCM full-cell (98 mAh g −1 ) in the high voltage range from 4 to 2.6 V as well as a remarkable capacity of 452 mAh g −1 at 200 mA g −1 after 50 cycles. In terms of Fe 3 O 4 -based anodes, enormous academic progress has been achieved over the past two decades; however, even with excellent half-cell performance, the relatively high lithiation potential and unsatisfactory initial coulombic efficiency (ICE) represent two major barriers to their commercial application, at present. We propose partially phosphorized Fe 3 O 4 (P−Fe 3 O 4 ) with interior void spaces induced by phosphorization to enhance the Li + storage property of Fe 3 O 4 -based anodes. P−Fe 3 O 4 anodes offer a much higher capacity at low potential compared with bare Fe 3 O 4 electrodes. Additionally, the well-designed nanostructure with preferable specific surface area prevents the initial irreversible lithium loss, which contributes to a brilliant ICE (80.8 % at 100 mA g −1 ). Moreover, in-situ X-ray diffraction proves that the formation of the Li x Fe 3 O 4 phase results from an initial intercalation process. In particular, the output voltage and energy density of P−Fe 3 O 4 full-cells are much greater than those of Fe 3 O 4 full-cells. In this work, the P−Fe 3 O 4 full-cell exhibits a capacity of 680 mAh g −1 at 200 mA g −1 as well as an excellent rate capability of 267 mAh g −1 with a current density up to 1000 mA g −1 . This study presents a new strategy to enhance Li + storage of Fe 3 O 4 enabling low lithiation/delithiation potential and high ICE, which may offer exciting opportunities toward designing high-performance full-cells with commercial cathodes.

CAS / MDL: 5949-29-1 7782-61-8
研究领域: 材料科学 · 电化学 · 能源存储
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

In Situ Synthesis and Dual Functionalization of Nano Silicon Enabled by a Semisolid Lithium Rechargeable Flow Battery

Laihao Liu,Xiuxia Zuo,Yajun Cheng,Yonggao Xia

Nanosized silicon has attracted considerable attentions as a new-generation anode material for lithium-ion batteries (LIBs) due to its exceptional theoretical capacity and reasonable cyclic stability. However, serious side reactions often take place at the nanosized silicon/electrolyte interface in LIBs, where critical electrochemical properties such as initial Coulombic efficiency (ICE) are compromised. On the basis of this feature, a new method is developed to synthesize nanosilicon-based particles in a facile, scalable way, which are endowed with the function of prelithiation and storage stability in air. A semisolid lithium rechargeable flow battery (SSFB) technology is used for the first time to convert the micrometer-sized silicon raw material into an amorphous-nanosilicon-based material (ANSBM), as a result of the pulverization process induced by the repeated lithiation/delithiation cycles. The particle size is successfully reduced from 1–4 μm to around 30 nm after cycles in the flow battery. Bulk functionalization of the nano silicon is introduced by the unbalanced lithiation/delithiation cyclic process, which endows ANSBM with a unique prelithiation capability universally applicable to different anode systems such as nanosized Si, SiOx, and graphite, as evidenced by the significantly improved ICEs. Superior air stability (10% relative humidity) is exhibited by ANSBM due to surface functionalization by the stable interfacial layer encapsulated by electron-conductive carbon. The outcome of this work provides a promising way to synthesize dual-functionalized nano silicon with good electrochemical performance in terms of improved capacity and increased initial Coulombic efficiency when it is composited with other typical anode materials.

CAS / MDL: 9003-01-4 7440-21-3
研究领域: 材料科学 · 电化学
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Small Methods · 2022 ·Vol. 6 ·期 8 ·2200404 · IF 15.367

Na1.51Fe[Fe(CN)6]0.87·1.83H2O Hollow Nanospheres via Non-Aqueous Ball-Milling Route to Achieve High Initial Coulombic Efficiency and High Rate Capability in Sodium-Ion Batteries

Chun-Mei Xu,Jian Peng,Xiao-Hao Liu,Wei-Hong Lai,Xiang-Xi He,Zhuo Yang,Jia-Zhao Wang,Yun Qiao,Li Li,Shu-Lei Chou

Prussian blue analogues (PBAs) have attracted extensive attention as cathode materials in sodium-ion batteries (SIBs) due to their low cost, high theoretical capacity, and facile synthesis process. However, it is of great challenge to control the crystal vacancies and interstitial water formed during the aqueous co-precipitation method, which are also the key factors in determining the electrochemical performance. Herein, an antioxidant and chelating agent co-assisted non-aqueous ball-milling method to generate highly-crystallized Na 2- x Fe[Fe(CN) 6 ] y with hollow structure is proposed by suppressing the speed and space of crystal growth. The as-prepared Na 2- x Fe[Fe(CN) 6 ] y hollow nanospheres show low vacancies and interstitial water content, leading to a high sodium content. As a result, the Na-rich Na 1.51 Fe[Fe(CN) 6 ] 0.87 ·1.83H 2 O hollow nanospheres exhibit a high initial Coulombic efficiency, excellent cycling stability, and rate performance via a highly reversible two-phase transition reaction confirmed by in situ X-ray diffraction. It delivers a specific capacity of 124.2 mAh g −1 at 17 mA g −1 , presenting ultra-high rate capability (84.1 mAh g −1 at 3400 mA g −1 ) and cycling stability (65.3% capacity retention after 1000 cycles at 170 mA g −1 ). Furthermore, the as-reported non-aqueous ball-milling method could be regarded as a promising method for the scalable production of PBAs as cathode materials for high-performance SIBs.

研究领域: 材料科学 · 电化学 · 能源存储
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