NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 31
·15016-15023
·
IF 3.925
Yayue He,Youjia Zhang,Zhenxi Li,Peng-Fei Cao,Huabin Yang,Shilun Gao
As a promising anode material for next-generation high-energy density lithium-ion batteries (LIBs), one of the main technical issues for silicon (Si) electrodes is the low initial Coulombic efficiency (ICE). By a pre-lithiation process, preparation of lithium–silicon (Li–Si) alloy electrodes can efficiently improve the ICE, thus leading to excellent electrochemical performance. Herein, with solid wastes as precursors, we report a cost-efficient approach for the fabrication of Li3.25Si anode materials via simple magnesiothermic reduction and then mechanical alloy reaction methods, combining the advantages of low-cost and high ICE. The prepared Li3.25Si@acetylene black (Li3.25Si@A) electrode exhibits excellent electrochemical performance with a high reversible capacity of 1138.9 mA h g−1 over 90 cycles at a current density of 100 mA g−1 and its ICE is as high as 107.7%, which is superior to that of the commercial Li3.25Si@A electrode. With a simple and low-cost manufacturing process and high ICE, the fabrication process will be definitely meaningful in achieving low-cost and high-capacity anode materials with a prolonged cycle life.
研究领域:
材料科学
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电化学
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能源存储
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可持续材料
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电池技术
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 17
·10780-10788
·
IF 12.732
Minghao Zhang,Yu Li,Feng Wu,Zhaohua Wang,Ying Bai,Chuan Wu
Porous carbon materials are regarded as one of the most promising candidates for sodium-ion batteries (SIBs) due to their fast sodium storage performance. However, the inadequate initial coulombic efficiency (ICE) resulting from the large specific surface area still hinders the commercialization of porous carbon anodes. Thus, it is important to synthesize porous carbon anodes with high electrochemical performance and improved ICE. Here we prepare a nitrogen and oxygen rich porous carbon material (NOPC) and construct a uniform passivation layer using a sodium carboxymethyl cellulose (CMC) binder on the surface of the NOPC material. The uniform passivation layer effectively deactivates the functional groups and suppresses the decomposition of electrolytes, resulting in an excellent ICE of 90%, which is ultrahigh and competitive among the reported carbon-based anodes in SIBs. Specifically, the as-prepared porous carbon anode delivers a reversible capacity of 191.7 mA h g−1 after 1000 cycles at 10 A g−1 with a capacity retention of 90%. This work suggests a general method to improve the ICE of a carbon material and hopefully facilitates the commercialization process of SIBs.
研究领域:
电化学
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材料科学
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能源存储
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纳米材料
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电池技术
✓ 已验证
DOI
高影响因子
Batteries & Supercaps
·
2022
·Vol. 6
·期 1
·e202200427
·
IF 6.043
Sheng Wu,Xiaoyi Lu,Kaili Zhang,Junling Xu,Zhipeng Sun
Among anode materials for sodium-ion batteries (SIBs), hard carbon (HC) gains more attention due to its low cost, high electronic conductivity, and renewable resources. However, sluggish kinetics result in its low-rate capability and unfavorable cycle stability. Moreover, HC often presents low initial Coulombic efficiency (ICE), which also limits the utilization of the battery capacity and energy density. Herein, nitrogen and phosphorus dual-doped HC (denoted as NPHC) with network structure is synthesized by a facile interfacial polymerization method, which endows the NPHC with synergistic effects of the enlarged interlayer spacing and improved conductivity. Consequently, the obtained NPHC exhibits a high reversible capacity (286 mAh g −1 at 0.1 A g −1 ), excellent rate capability (144 mAh g −1 at 10 A g −1 ), high ICE (71 %), and remarkable cyclability over 2000 cycles at 1 A g −1 . Moreover, the storage mechanism of sodium ions is examined by a series of ex-situ characterizations. Additionally, when coupled with Na 3 V 2 (PO 4 ) 2 F 3 as a cathode, the full cell delivers superior cyclability (capacity retains 90 % over 300 cycles at 1 A g −1 ). This work may shed new insight into designing other carbon-based electrode materials for high-performance energy storage. Graphical With hard carbon : we use a facile interfacial polymerization method to prepare hard carbon with N/P dual-doped (NPHC), which shows superb rate capability (286 and 144 mAh g −1 at 0.1 and 10 A g −1 , respectively). Through a series of analyses, NPHCS demonstrates a higher ion diffusion coefficient, capacitive contribution, and conductivity. This confirms that N/P dual-doping is more beneficial to improve electrochemical performance.
研究领域:
材料科学
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电化学
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能源存储
·
纳米材料
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电池技术
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Yan Ji,Zhiqing Ge,Huali Zhu,Junfei Duan,Yanxia Wang,Yanling Gu,Zhaoyong Chen
Constructing an artificial SEI on a hard carbon surface effectively enhances initial coulombic efficiency (ICE) and cycling stability. A polymer electrolyte binder containing sodium ions (SPEB), consisting of PAAS and PEO , is designed using a straightforward method. A high ion conductivity artificial SEI is constructed on a pomelo peel-derived hard carbon (PHC) surface through esterification and hydrogen bonding . In hard carbon anodes for sodium ion batteries (SIBs), SPEB plays a crucial role by facilitating pre-sodiation in PHC, enhancing ion conductivity, and guiding the construction of a NaF-rich, ultra-thin, and stable SEI. The synthesized PHC possesses an outstanding reversible specific capacity of 375.13 mAh·g −1 , a superior ICE of 90.94 %, good rate capability, and excellent cycle stability. After 400 cycles at 0.9 A·g −1 , it retains 152.52 mAh·g −1 with almost no decay. Meanwhile, SPEB demonstrates an exciting performance in other hard carbons and helps its commercialization application in SIBs.
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2021
·
IF 17.881
Yuantao Yan,Yu-Shi He,Xiaoli Zhao,Wanyu Zhao,Zi-Feng Ma,Xiaowei Yang
Nanostructured silicon-based materials are the promising anodes for next-generation lithium-ion batteries. However, as the result of the weak adhesion of solid-electrolyte interphase (SEI) to Si, the fracture, exfoliation and subsequent regrowth of SEI layer on the expanded Si remains unsolved, leading to low initial Coulombic efficiency (ICE) (50–80%). Herein, the Ti‒Si covalent bond between nano-Si and MXene-derived artificial SEI layer is elaborately introduced, to effectively strengthen the interfacial stability and suppress the excessive interfacial side reaction. Upon the three-times expansion during first cycling, the as-obtained anodes with the ultrathin SEI still deliver a high ICE of 91.4%. Due to the stable interfacial ionic conduction, remarkable capacity retention of 90.7% after 1000 cycles at 5 A g −1 with an average Coulombic efficiency of 99.8% could be maintained. This strategy provides new insight into designing durable alloy anodes from the point of the interfacial adhesion strength .
研究领域:
材料科学
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电化学
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纳米科技
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能源存储
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界面化学
·
锂离子电池
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Helin Wang,Weiwei Wu,Qiurong Jia,Ting Liu,Fu Liu,Min Zhang,Miao Bai,Shaowen Li,Xiaoyu Tang,Bin Gan,Yue Ma
The Si anodes suffer from the repetitive buildup of the solid electrolyte interphase, electrode pulverization upon the lithiation/delithiation process, as well as the Li trapping in the alloy intermediates. Herein, a facile electrostatic self-assembly process of the Si nanosheets (SiNS) and graphite microsheets (GMs) is proposed as a viable high-capacity composite anode. Upon the appropriate interfacial tailoring, the SiNS/GMs composite not only guarantees the intimate contact mode between the sand-milled Si nanosheets and the positively charged graphite sheets but also renders the enhanced electrode conductivity and high-rate performance (886.2 mAh g–1 at current density of 5 A g–1). In addition, the prelithiated SiNS/GMs (Pre-SiNS/GMs) are fabricated by spraying stabilized lithium metal powder (SLMP) at the predetermined amounts onto the electrodes, contributing to the improved initial Coulombic efficiency (ICE) of the half cell (99%). As the Pre-SiNS/GMs anodes are assembled with the diverse commercial cathodes, the full cell models reveal the balanced cycling endurance and the high gravimetric energy/power densities.
研究领域:
材料科学
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电化学
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能源存储
·
纳米材料
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电池技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Longfei Wang,Jiayang Sun,Yirui Liang,Linze Lv,Lei Huang,Yan Wang,Qunting Qu,Ming Shen,Honghe Zheng
Graphite is still the dominant anode material for the state-of-the-art lithium-ion batteries. Natural graphite (NG) has the advantages of high specific capacity, abundant resources and less energy consumption. However, the high surface area, high interfacial reactivity, and the sluggish interfacial kinetics result in low initial Coulombic efficiency (ICE), poor rate performance and unsatisfactory cycle-life. Herein, we propose a uniform and fast Li + -conductive LiAlO 2 interface on NG surface with polydopamine-mediated Al 3+ anchoring route. After proper heat-treatment, the in-situ developed inorganic LiAlO 2 layer greatly reduces interfacial resistance by accelerating the interfacial Li + migration kinetics. More importantly, the inorganic LiAlO 2 layer reduces the surface reactivity of the NG anode and promotes the formation of fluorinated SEI with enhanced electron work function, high stability and fast Li + diffusion properties. As the result, the ICE of the prepared NG@PLAO anode exhibits a high ICE of 92.5 % due to the suppressed interfacial side reactions of the electrolyte components. At a high charge-discharge rate of 4C, the fabricated NCM523||NG@PLAO full cell retains 80.3 % of its nominal capacity over 800 cycles. The novel interfacial chemistry engineering well solves the uniform growth of inorganic interface on NG surface via polydopamine-mediation. It provides new thoughts to improve the fast charge and cycleability of NG anode in lithium-ion batteries.
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Jing Li,Jianguang Guo,Qing Sun,Xiangkun Nie,Linna Dai,Yu Wang,Lijie Ci
Silicon monoxide (SiO) has captured great attention as one of the most promising anode materials due to its great cycling stability as well as high theoretical capacity. However, hindered by its low initial Coulombic efficiency, the possible large-scale application remains an urgent issue. Herein, through a facile method, potassium ions are introduced into the disproportionation process of SiO to promote the transition from amorphous SiOx into the cristobalite phase with higher crystallinity. The cristobalite phase exhibits lower reaction activity with lithium ions, which reduces the formation of lithium silicate. As a consequence, the cycling stability and the initial Coulombic efficiency (ICE) are improved. In addition, it is proved in our study that increasing the heating temperature is helpful to improve the ICE and cycling stability of SiO. This work provides a facile disproportionation method for the microstructure regulation of SiO, offering a possible avenue for the development of large-scale applications of the SiO anode.
研究领域:
材料科学
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电化学
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纳米材料
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能源存储
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固体化学
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电池技术
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Zhang Yibo,Zhang Si-Wei,Chu Yue,Zhang Jun,Xue Haoyu,Jia Yiran,Cao Tengfei,Qiu Dong,Zou Xiaolong,Wang Da-Wei,Tao Ying,Zhong Guiming,Peng Zhangquan,Kang Feiyu,Lv Wei,Yang Quan-Hong
Closed pores are widely accepted as the critical structure for hard carbon negative electrodes in sodium-ion batteries. However, the lack of a clear definition and design principle of closed pores leads to the undesirable electrochemical performance of hard carbon negative electrodes. Herein, we reveal how the evolution of pore mouth sizes determines the solvation structure and thereby redefine the closed pores. The precise and uniform control of the pore mouth sizes is achieved by using carbon molecular sieves as a model material. We show when the pore mouth is inaccessible to N 2 but accessible to CO 2 molecular probes, only a portion of solvent shells is removed before entering the pores and contact ion pairs dominate inside pores. When the pore mouth is inaccessible to CO 2 molecular probes, namely smaller than 0.35 nm, solvent shells are mostly sieved and dominated anion aggregates produce a thin and inorganic NaF-rich solid electrolyte interphase inside pores. Closed pores are accordingly redefined, and initial coulombic efficiency, cycling and low-temperature performance are largely improved. Furthermore, we show that intrinsic defects inside the redefined closed pores are effectively shielded from the interfacial passivation and contribute to the increased low-potential plateau capacity.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yong Wu,Honglei Liu,Deli Li,Ranlin Dong,Mengfan Bu,Bei Liu,Xiaoming Fan,Weixin Zhang
Silicon (Si) is emerging as a highly promising anode material candidate for high energy-density lithium-ion batteries (LIBs). However, its significant volume expansion during cell cycling poses a substantial challenge. Herein, fluorinated carbon derived from a fluorine-rich polymer is employed as a functional layer to engineer the solid electrolyte interface (SEI) of Si based anode material, featuring LiF-rich components in the SEI film. The strong initial Coulombic efficiency (ICE)-semi-ionic F/C linear correlation in Si@C/F nanoparticles demonstrates the essential function of semi-ionic fluorine in high-efficiency Si anodes. Semi-ionic fluorine promotes preferential LiF nucleation during SEI formation, which simultaneously suppresses lithium-consuming side reactions to enhance ICE and stabilizes the electrode interface. The homogeneous LiF distribution creates low-barrier Li + diffusion channels, markedly boosting electrode kinetics for enhanced high-rate capability. As a result, the Si@C/F composite exhibits outstanding electrochemical performance, with an ICE value as high as 88.8 %. The Si@C/F composite also demonstrates excellent long-cycling stability and high-rate capability, maintaining a reversible capacity of 971.8 mAh g −1 even under 1 A g −1 for 500 cycles. This work reveals the regulation of C F bonds in the carbon layer to construct robust SEI layer in the Si/C composites, offering a strategy for advanced Si-based anode materials with both high ICE and stable cycling performance.
研究领域:
储能
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材料科学
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电化学
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纳米技术
·
电池技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhan Wang,Zhongyuan Feng,Shuang Li,Gaoyu Zhou,Quanchao Zhuang,Zhicheng Ju,Jiangmin Jiang,Huaiyu Shao
Silicon is a promising anode material for next-generation lithium-ion batteries (LIBs) due to its high specific capacity and low cost. However, its practical application is severely hindered by significant volume expansion during lithiation and delithiation, which causes mechanical stress and instability of the solid electrolyte interphase (SEI). These issues lead to poor cycling performance and low initial Coulombic efficiency (ICE), posing substantial challenges for commercial implementation. Herein, we propose an innovative strategy of co-derived fluorinated SEI pre-construction through chemical prelithiation, employing a 2-fluorobiphenyl-lithium-dimethyltetrahydrofuran (2-F-BP-Li-2MT) system designed for silicon-carbon (Si@C) anodes. Unlike conventional prelithiation methods that solely compensate for lithium loss, simultaneously forming a robust SEI layer enriched with lithium fluoride (LiF) components directly on the surface of Si@C. The co-derived fluorinated SEI exhibits a unique “fluorine-homogeneous” structure during cycling, significantly enhancing mechanical durability and facilitating rapid Li + transport. The chemically prelithiated Si@C anodes with co-derived fluorinated SEI (Pr-F-Si@C) achieve a high ICE of 99.5 % and remarkable capacity retention of 86.3 % after 300 cycles. Furthermore, the assembled full cells (LiFePO 4 //Pr-F-Si@C) deliver high energy density (246.3 Wh kg −1 , based on total mass) and stable cycling performance. This work provides critical insights into interface design and prelithiation, providing new pathways toward practical high-energy and long-life Si-based batteries.
研究领域:
材料科学
·
电化学
·
纳米能源
·
储能技术
·
界面化学
·
锂离子电池
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Zihao Su,Zhihao Guo,Haoyu Xie,Meizhen Qu,Gongchang Peng,Hao Wang
Li-rich Mn-based cathode materials (LLOs) are often faced with problems such as low initial Coulombic efficiency (ICE), limited rate performance, voltage decay, and structural instability. Addressing these problems with a single approach is challenging. To overcome these limitations, we developed an LLO with surface functionalization using a simple fabrication method. This two-step process involved a liquid-stage NaBF4 treatment followed by an in situ chemical reaction during sintering. This reaction led to the creation of oxygen vacancies (OV), spinel structures, and doping with Na at the Li site, B at the tetrahedral interstitial spaces of O in both the transition-metal (TM) layer and Li layers as well as the octahedral interstices in the TM layer, and F at the O site. We have carried out a thorough study and employed density functional theory calculations to reveal the hidden mechanisms. The treatment not only increases the electrical conductivity but also changes the oxygen charge environment and inhibits lattice oxygen activity. Surprisingly, the B–O bond is so strong that it prevents the migration of TM within the tetrahedral interstitial spaces of O in both the TM and Li layers, hence stabilizing its structure. This bonding interaction strengthens the transition of the TM 3d and O 2p states to lower energy levels, thus causing an increase in the redox potentials. Hence, a rise in the operating voltage occurs. Of special importance, this therapy dramatically increases the ICE to 90.29% and keeps a specified capacity of 203.3 mAh/g after 100 cycles at 1C, which is an excellent capacity retention of 89.94%. This study introduces ideas and methods to tackle the challenges associated with LLOs in batteries. It also provides compelling evidence for the development of high-energy-density Li-ion batteries.
研究领域:
材料科学
·
电化学
·
锂离子电池
·
固态化学
·
能源材料
·
表面工程
·
计算材料学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）