Nano Energy
·
2023
·
IF 17.6
Wei Zhong,Siwu Li,Mengchuang Liu,Qiang Wu,Ziqi Zeng,Shijie Cheng,Jia Xie
The self-sacrificing Li 2 C 2 O 4 is a promising lithium replenisher benefiting from its high specific capacity, residue-free and low-cost properties. However, the intrinsic low electrochemical activity leads to a decomposition potential up to 4.7 V, posing a challenge for the compatibility of electrolyte and cathode materials . Herein, a three-dimensional (3D) hierarchical spherical Mo 2 C/N-doped graphene co-catalysts is synthesized by self-polymerization and high-temperature annealing. It is shown that the synergistic catalytic effect of Mo 2 C and N-doped activated graphene enhances the reactivity of Li 2 C 2 O 4 and the hierarchical three-dimensional conducting network accelerates the electron-ion transport. When the nano-Li 2 C 2 O 4 is homogeneously encapsulated in the spherical catalytic center using a freeze-drying technique, the electrochemical reaction of Li 2 C 2 O 4 is greatly promoted, resulting a significant drop of decomposition potential from 4.7 V to 4.16 V. As a result, the specific capacity of Gr||LFP and SiC||LFP full cells with composite lithium replenisher can be increased by 15% and 22%, respectively. Moreover, the solid electrolyte interface (SEI) is appropriately strengthened with pre-lithiation and thus guarantees superior cycling performance.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Liyuan Li,Tao Li,Yifan Sha,Chi Zhang,Baozeng Ren,Lan Zhang,Suojiang Zhang
Silicon-based anode materials attract ever-increasing attention owing to their high theoretical capacity. However, their practical application is significantly hindered by the dramatic volume change during the charge/discharge process, during which not only the solid electrolyte interface (SEI) but also the electrode might be ruined. Here, we propose a H-bond network-regulated binder by introducing low-molecular-weight cross-linkers, lithium oxalate and α-cyclodextrin (α-CD), into alginate (Alg). The balance between the binding strength and Li ion diffusion is realized through the control of the ratio between them. Lithium oxalate and α-CD can effectively regulate the H-bond network of the binder by forming intermolecular dynamic H bonds with Alg and reducing the intramolecular ones. Although the hybrid binder shows lower adhesion force than Alg, better electrode integrity is obtained during the charge/discharge process. Meanwhile, Li+ transportation is facilitated due to extra Li+ supplied by lithium oxalate, thereby achieving better rate capability.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 30
·2404815
·
IF 27.4
Yi-Hong Tan,Zhu Liu,Jian-Hui Zheng,Zhi-Jin Ju,Xiao-Ya He,Wei Hao,Ye-Chao Wu,Wen-Shan Xu,Hao-Jie Zhang,Guo-Qing Li,Li-Sha Zhou,Fei Zhou,Xinyong Tao,Hong-Bin Yao,Zheng Liang
The solid electrolyte interphase (SEI) with lithium fluoride (LiF) is critical to the performance of lithium metal batteries (LMBs) due to its high stability and mechanical properties. However, the low Li ion conductivity of LiF impedes the rapid diffusion of Li ions in the SEI, which leads to localized Li ion oversaturation dendritic deposition and hinders the practical applications of LMBs at high-current regions (>3 C). To address this issue, a fluorophosphated SEI rich with fast ion-diffusing inorganic grain boundaries (LiF/Li 3 P) is introduced. By utilizing a sol electrolyte that contains highly dispersed porous LiF nanoparticles modified with phosphorus-containing functional groups, a fluorophosphated SEI is constructed and the presence of electrochemically active Li within these fast ion-diffusing grain boundaries (GBs-Li) that are non-nucleated is demonstrated, ensuring the stability of the Li || NCM811 cell for over 1000 cycles at fast-charging rates of 5 C (11 mA cm −2 ). Additionally, a practical, long cycling, and intrinsically safe LMB pouch cell with high energy density (400 Wh kg −1 ) is fabricated. The work reveals how SEI components and structure design can enable fast-charging LMBs.
研究领域:
材料科学
·
电化学
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储能
·
电池技术
✓ 已验证
DOI
高影响因子
Science Advances
·
2025
·Vol. 11
·期 27
·
IF 12.5
Chutao Wang,Kun Wang,Hongbin Ni,Congcong Du,Xiaoting Yin,Jingmin Fan,Ruming Yuan,Yuxin Tang,Jiawei Yan,Mingsen Zheng,Quanfeng Dong
Direct metal anodes are plating/stripping processes without a supporting framework and bulk ion conductivity; they are the electrodes susceptible to collapse and limiting the electrochemical reaction to the two-dimensional surface. The focus of this era is mostly on building a solid electrolyte interface (SEI). However, simply building protective layers cannot address essential issues; a thorough transformation of the metal electrode bulk is critical. We propose a reconstructed sodium metal anode (RSMA) by implanting an activatable ion-conductive network to the bulk. NaPF 6 will be activated with an electrolyte to conduct ions and form an anion-derived SEI. Conductive polymers become the supporting skeleton; thus, the RSMA has a metal-bulk storage matrix and an expanded three-dimensional plating/stripping mechanism and permits the homogeneous deposition/dissolution of Na + in high dimensions. Last, RSMA symmetric cells were stably cycled for 2700 hours and achieved a 100% depth of discharge. RSMA||PB cells can achieve 10-coulomb cycling and a proof-of-concept pouch cell energy density of 367 watt-hours per kilogram.
研究领域:
电化学
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储能技术
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材料科学
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电池技术
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Chencheng Xu,Jiangmin Jiang,Shuang Li,Zhan Wang,Gaoyu Zhou,Yaxin Chen,Xiangkai Kong,Quanchao Zhuang,Zhicheng Ju
Graphite (Gr) is a low-cost, highly stable anode material for lithium-ion batteries (LIBs). However, the Gr anode has the disadvantage of low initial coulombic efficiency (ICE) due to the loss of active lithium caused by the formation of solid electrolyte interface (SEI). Chemical pre-lithiation is an effective method to compensate for the loss of active lithium, but the redox potential of traditional chemical pre-lithiation reagents is higher than the Li + insertion potential of Gr (≈0.2 V vs Li/Li + ), which leads to the inability of lithiation reaction. In this work, a methoxybiphenyl lithium chemical pre-lithiation system is designed by molecular tailoring engineering, density functional theory (DFT) and experimental investigations demonstrate the system's reduced redox potential (0.075–0.142 V vs Li/Li + ) and a suitable Li + binding energy. The results demonstrate that the ICE of Gr anode chemically pre-lithiated for 4 min is 103.32 % and the process is stable and efficient by using the molecularly tailored chemical pre-lithiation reagent. In practical applications, the lithium-ion full-battery assembled with LiFePO 4 (pGr||LFP) exhibits high ICE (93.05 %) and energy density (321.7 Wh kg −1 ). The novel methoxybiphenyl lithium chemical pre-lithiation system prepared by molecular tailoring engineering provides a promising approach for chemical pre-lithiation engineering.
研究领域:
材料科学
·
电化学
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储能技术
·
化学工程
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Guoqiang Qin,Zhitong Jia,Songyuan Sun,Huigui Wu,Kaihan Hu,Dongmei Liu,Yiqun Gao,Jingbo Chen
Silicon (Si) and Si-based compounds have been considered by many researchers as one of the anode materials for the next-generation lithium-ion batteries (LIBs) due to their extraordinarily large theoretical capacity, moderate operating voltage, and abundant resources. However, silicon’s poor conductivity and significant volume changes during charge and discharge, compared to conventional carbon materials, severely restrict its widespread use in LIBs. In this study, a two-dimensional (2D) mesoporous Si nanosheet/carbon (pSi@C) composite is designed using cetrimonium bromide–disodium edetate dihydrate (CTAB–EDTA) as a template via a sol–gel method, magnesium thermal reduction method, and thermal decomposition method. The vertical diffusion distance of Li+ is significantly reduced by the 2D Si nanosheets. Additionally, the carbon coating on the Si surface provides a protective layer to limit the volume expansion of Si and form a stable solid electrolyte interface (SEI). This enhances the structural integrity and cycle stability of the pSi@C anode material during Li+ insertion and extraction. At a current density of 1 A g–1, the reversible capacity of the pSi@C composite after 150 cycles is 2236 mAh g–1, with a capacity retention rate of 71.5%. The electrode’s capacity is 467.8 mAh g–1 after 500 cycles at a current density of 5 A g–1. Therefore, this unique template and technology can be used to design 2D anode composites with excellent properties, thereby providing an effective strategy for commercial application of LIBs.
研究领域:
材料科学
·
电化学
·
纳米技术
·
能量存储
✓ 已验证
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-14
·
IF 16.6
Zhang Junbo,Zhang Haikuo,Weng Suting,Li Ruhong,Lu Di,Deng Tao,Zhang Shuoqing,Lv Ling,Qi Jiacheng,Xiao Xuezhang,Fan Liwu,Geng Shujiang,Wang Fuhui,Chen Lixin,Noked Malachi,Wang Xuefeng,Fan Xiulin
Elevating the charging cut-off voltage is one of the efficient approaches to boost the energy density of Li-ion batteries (LIBs). However, this method is limited by the occurrence of severe parasitic reactions at the electrolyte/electrode interfaces. Herein, to address this issue, we design a non-flammable fluorinated sulfonate electrolyte by multifunctional solvent molecule design, which enables the formation of an inorganic-rich cathode electrolyte interphase (CEI) on high-voltage cathodes and a hybrid organic/inorganic solid electrolyte interphase (SEI) on the graphite anode. The electrolyte, consisting of 1.9 M LiFSI in a 1:2 v / v mixture of 2,2,2-trifluoroethyl trifluoromethanesulfonate and 2,2,2-trifluoroethyl methanesulfonate, endows 4.55 V-charged graphite||LiCoO 2 and 4.6 V-charged graphite||NCM811 batteries with capacity retentions of 89% over 5329 cycles and 85% over 2002 cycles, respectively, thus resulting in energy density increases of 33% and 16% compared to those charged to 4.3 V. This work demonstrates a practical strategy for upgrading the commercial LIBs.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Fengwei Bai,Yan Li,Ziyu Chen,Yongchao Zhou,Chengzong Li,Tao Li
High-voltage lithium (Li)-metal batteries with cell-level energy density over 350 Wh kg −1 are promising energy storage systems . However, the aggressive interphase chemistries associated with highly reactive Li-metal anode and high-voltage cathodes impede their practical applications. Herein, we demonstrate the targeted stabilization of solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI) in high-voltage Li-metal batteries by asymmetrically sustained-releasing different additives. An asymmetric sustained-release film loaded with lithium bis-(oxalate)borate (LiBOB) and LiNO 3 on each side is investigated as a proof-of-concept. The sustained-releasing of LiBOB and LiNO 3 can maintain a localized concentration at the high-voltage cathode and Li-metal anode fronts respectively, thus forming a stable B-containing CEI and N-containing SEI. As such, issues like dendrites growth, parasitic side reactions and transition metals dissolution under high-voltage are addressed simultaneously. Based on this strategy, the 30 μm Li|LiNi 0.5 Co 0.2 Mn 0.3 O 2 (4.1 mAh cm −2 ) batteries deliver a capacity retention of 80% after 173 cycles under a cut-off voltage of 4.5 V.
研究领域:
储能系统
·
电池技术
·
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2023
·
IF 6.4
Xin Li,Cancan Bian,Jun Zhang,Jian Hong,Rusheng Fu,Xufeng Zhou,Zhaoping Liu,Guangjie Shao
Silicon monoxide (SiOx, x ∼ 1) has emerged as a highly promising candidate for high-energy-density lithium-ion batteries due to its high specific capacity and suitable working potential. Nevertheless, the formation of a large quantity of irreversible products, such as Li2O and lithium silicates, during the initial lithiation process results in a low initial coulombic efficiency (ICE) of SiOx, which is a significant impediment to its commercial application. To overcome this limitation, two lithium aromatic complexes, namely, lithium-naphthalene-2-methyl-tetrahydrofuran (N-LAC) and lithium-biphenyl-2-methyl-tetrahydrofuran (B-LAC), with a low redox potential are used to pre-lithiate SiOx anodes. The differences in lithiation kinetics and efficacy of the two LAC solutions are identified and assessed by scrutinizing the pre-lithiation process of SiOx materials. It is revealed that both pre-lithiation agents produce solid electrolyte interphase (SEI) films on the material surface enriched with substances such as LiF, Li2CO3, and ROCO2Li, but the LiF content in the SEI of the N-LAC pre-lithiated electrode is significantly higher. Furthermore, the surface roughness of the N-LAC pre-lithiated electrode is lower, and the horizontal distribution of mechanical properties and surface potential tend to be more homogeneous, even during cycling, at approximately the same degree of lithiation. The results indicate that the N-LAC solutions not only improve the ICE of the SiOx material but also optimize the interfacial and structural stability of the SiOx electrode. When the pre-lithiated SiOx anode is paired with lithium-rich layered oxide cathode materials, the energy density and ICE are significantly improved compared to the cell using pristine SiOx anode.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Jin Chengbin,Huang Yiyu,Li Lanhang,Wei Guoying,Li Hongyan,Shang Qiyao,Ju Zhijin,Lu Gongxun,Zheng Jiale,Sheng Ouwei,Tao Xinyong
Reactive negative electrodes like lithium (Li) suffer serious chemical and electrochemical corrosion by electrolytes during battery storage and operation, resulting in rapidly deteriorated cyclability and short lifespans of batteries. Li corrosion supposedly relates to the features of solid-electrolyte-interphase (SEI). Herein, we quantitatively monitor the Li corrosion and SEI progression (e.g., dissolution, reformation) in typical electrolytes through devised electrochemical tools and cryo-electron microscopy. The continuous Li corrosion is validated to be positively correlated with SEI dissolution. More importantly, an anti-corrosion and interface-stabilizing artificial passivation layer comprising low-solubility polymer and metal fluoride is designed. Prolonged operations of Li symmetric cells and Li | |LiFePO 4 cells with reduced Li corrosion by ~74% are achieved (0.66 versus 2.5 μAh h −1 ). The success can further be extended to ampere-hour-scale pouch cells. This work uncovers the SEI dissolution and its correlation with Li corrosion, enabling the durable operation of Li metal batteries by reducing the Li loss.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yue Lei,Xin Xu,Junying Yin,Jianping Xu,Kang Xi,Lai Wei,Haihua Wu,Sen Jiang,Yunfang Gao
Commercial Li-ion batteries use LiPF6-based carbonate electrolytes extensively, but there are many challenges associated with them, like dendritic Li growth and electrolyte decomposition, while supporting the aggressive chemical and electrochemical reactivity of lithium metal batteries (LMBs). This work proposes 1,1,1,3,3,3-hexafluoroisopropyl methacrylate (HFM) as a multifunctional electrolyte additive, constructing protective solid-/cathode-electrolyte interphases (SEI/CEI) on the surfaces for both lithium metal anode (LMA) and Ni-rich cathode to solve these challenges simultaneously. The highly fluorinated group (−CF3) of the HFM molecule contributes to the construction of SEI/CEI films rich in LiF that offer excellent electronic insulation, high mechanical strength, and surface energy. Accordingly, the HFM-derived LiF-rich interphases can minimize the electrolyte–electrode parasitic reactions and promote uniform Li deposition. Also, the problems of LiNi0.8Co0.1Mn0.1O2 particles’ inner microcrack evolution and the growth of dendritic Li are adequately addressed. Consequently, the HFM additive enables a Li/LiNi0.8Co0.1Mn0.1O2 cell with higher capacity retention after 200 cycles at 1 C than the cell with no additive (74.7 vs 52.8%), as well as a better rate performance, especially at 9 C. Furthermore, at 0.5/0.5 mAh cm–2, the Li/Li symmetrical battery displays supersteadfast cyclic performance beyond 500 h when HFM is present. For high-performance LMBs, the HFM additive offers a straightforward, cost-effective route.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yongrui Luo,Yinnan Qian,Minghui Cai,Pengtao Zhang,Jixiao Li,Zhaoyan Luo,Jiangtao Hu,Yongliang Li,Qianling Zhang,Xiangzhong Ren
Plastic-crystal-embedded elastomer electrolytes (PCEEs), produced through polymerization-induced phase separation (PIPS), are gaining popularity as solid polymer electrolytes (SPEs). However, it remains to be investigated whether all monomer molecules can achieve polymerization-induced phase separation and the corresponding differences in lithium metal battery performance. Herein, we prepared PCEEs with different functional groups ( OH, CN, F) through in situ polymerization. Research findings show that PCEE containing – CN or – F achieves the separation of the plastic crystalline phase and succinonitrile (SN) phase, whereas PCEE containing OH cannot due to hydrogen bonding with the SN phase. Notably, the PCEE synthesized with the F monomer (FBA-PCEE) exhibited exceptional interfacial stability with lithium metal anodes and lithium iron phosphate (LFP) cathodes, due to its unique coordination mechanism with lithium ions. The FBA-PCEE demonstrated a high ionic conductivity (2.02 × 10 −3 S cm −1 ) and lithium-ion migration number ( t Li + = 0.75). Moreover, lithium symmetric cells incorporating FBA-PCEE demonstrated stable cycling performance for more than 1000 h at a current density of 0.1 mA cm −2 , resulting in the development of a solid electrolyte interphase (SEI) rich in LiF, Li 3 N, and Li 2 CO 3 over time. Additionally, incorporating FBA-PCEE facilitated the stable cycling of LPF over 1000 cycles at 0.5C, maintaining a capacity retention of 77.38 % after 500 cycles. When coupled with high-voltage Nickel Cobalt Manganese Oxide (NCM-622) cathodes and lithium metal anodes, a discharge capacity of 119.70 mAh g −1 at 0.1C was sustained after 100 cycles, exhibiting a capacity retention of 78.95 %. This study elucidates the critical role of monomer design in achieving PIPS, offering valuable insights into developing high-performance polymer composite electrolytes for advanced lithium metal batteries.
研究领域:
材料科学
·
电化学
·
电池技术
·
高分子化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）