Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 25
·12012-12017
·
IF 9.931
Lina Gao,Juner Chen,Yaqin Liu,Yusuke Yamauchi,Zhenguo Huang,Xueqian Kong
Stabilizing the reactive metal anode is a critical challenge for the development of next-generation alkali metal batteries. This work demonstrates that sodium-difluoro(oxalato)borate (NaDFOB)-based carbonate-ester electrolytes have excellent compatibility with the anode in sodium metal batteries, enabling high rate performance and long cycle life. The NaDFOB-based electrolytes possess favourable electrochemical stability and effectively passivate the Na metal anode by forming a compact, robust and conductive solid-electrolyte interphase (SEI) layer. Quantitative nuclear magnetic resonance (NMR) measurements of electrolyte solvents indicated that the SEI layer forms mainly in the initial cycles, and it prevents further solvent degradation. Solid-state NMR and X-ray photoelectron spectroscopy studies revealed the chemical composition of the NaDFOB-derived SEI film, which includes a mixed phase consisting primarily of sodium diborate, tetrafluoroborate and carbonate. The formation of such a composite SEI rich in borate and tetrafluoroborate provides robust structural and chemical stability, and facilitates fast ion transport for uniform Na stripping/plating.
研究领域:
化学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Enmin Li,Xin Tang,Juncheng Zhou,Haomiao Zhao,Jinhan Teng,Junjie Huang,Binghan Dai,Tianming Lu,Qingdong Tao,Kaibo Zhang,Weifeng Deng,Jing Li
Sodium-ion batteries are a promising energy storage system due to their rich sodium resources and many other advantages. However, its development is severely hampered by the electrolyte's low compatibility with the electrode contact. Herein, we propose a solvation control strategy with ethoxy (pentafluoro) cyclotriphosphazene (PFPN) and NaClO 4 double additives to reconstruct the solvation structure of sodium ions in electrolytes. This enables the electrolyte to form a dense and stable solid electrolyte interlayer (SEI) and double-layer cathode electrolyte interphase (CEI) on the surface of the electrode material to achieve long-cycle and high-capacity sodium-ion batteries. PFPN can form a stable SEI rich in inorganic components at the anode interface. ClO 4 - can first reach the cathode surface to create a NaCl and polymer-like chain CEI with sodium ions and solvents, and then the PFPN derivatives are migrated to the cathode surface to open the ring and decompose, thus forming a double-layer stable CEI. Therefore, the PEDN electrolyte can simultaneously improve the interface stability of the battery's cathode and anode solid electrolyte. Hence, the capacity retention rate of the 4.5 Ah Na 3 Fe 2 (PO 4 )P 2 O 7 (NFP)||hard carbon (HC) pouch cell after 2500 cycles at 1C is 88.26%.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Haoyu Ma,Baogang Zhao,Zhuobin Han,Mengjia Yu,Kexin Liu,Zhongting Wang,Bingqing Yan,Yinghao Zhou,Xin Feng,Rongrong Jia,Yin Zhao,Zhuyi Wang,Yumei Wang,Li Lu,Shuai Yuan,Liyi Shi,Yingying Lv
Silicon (Si) based anode materials for lithium ion (Li + ) batteries have garnered significant attention due to their high specific capacity, low lithium insertion potential, but higher cost than usual graphite anode. The generation of Si scrap from the slicing of photovoltaic Si leads to substantial material scrap. Here, we present a novel technique that an organic molecular encapsulation with elastic polymer silane coupling agent (KH570) crosslinking with trifluoromethyl ethyl methacrylate (TFEMA) on the surface of micrometer-scale photovoltaic Si scrap particles via hydrolysis followed by polymerization. The fluorination termination functional groups would induce a more stable LiF-rich solid electrolyte interface (SEI) during the cycling, which lead to the reduction in Li + and charge transfer resistance. More importantly, the crosslinking network of the elastic polymer, enables micrometer-sized Si scrap maintain the capacity retention of at 5 A/g for 500 cycles (985mAh/g, 5 times than pure Si scrap) and achieves a 90 % retention rate after 100 cycles (131mAh/g) in a full cell system. Furthermore, the Si scraps with such a functional organic coating could be matching with a polymer-based electrolyte as an all-solid battery, which present a specific capacity of 1000mAh/g. This technique of organic molecular encapsulation is straightforward, replicable and holds considerable practical value for the recycling of resources.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Boyuan Liu,Heng Zhou,Shiqiang Wei,Shuangming Chen,Hong Wang,Hengjie Liu,Yixiu Wang,Jialin Shi,Zijun Zhang,Qian Zhou,Zhandong Wang,Li Song
Electrolyte additives represent a promising strategy for regulating the solid-electrolyte interphase (SEI) in aqueous zinc-ion batteries. However, the underlying molecular mechanisms by which these additives mediate SEI formation remain insufficiently understood. Here, we employ 1-acetyl-2-pyrrolidone (APD) as a model organic additive to mechanistically map molecular cracking pathways involved in constructing a robust SEI on zinc anodes. Using in situ synchrotron radiation vacuum ultraviolet photolysis mass spectrometry (SR-VUPM), for the first time, we reveal the dynamic cleavage process of the additive to form a hybrid SEI. The in situ synchrotron radiation X-ray diffraction and Fourier transform infrared spectroscopy further indicate that the resulting hybrid SEI serves as a hydrophobic barrier and regulates the uniform deposition of zinc. The functional SEI plays a crucial role in optimizing interfacial reaction kinetics and deposition/stripping reversibility. As a result, the Zn/Zn symmetric cells deliver over 1500 h at 5.0 mA cm −2 and 5.0 mA h cm −2 . The cycle life of the Zn/I 2 @AC full battery is extended to 6000 cycles, while the optimized pouch cell also displays excellent cyclic stability. These findings provide mechanistic insight into additive-derived SEI formation for developing durable metal anodes.
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DOI
高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Yiping Liu,Yuxin Huang,Qiang Zhang,Rouyan Guo,Guangqi Zhang,Jie Dong,Liancheng Zhao,Liming Gao
Ideal solid electrolyte interphase (SEI) is required for non-dendrite lithium (Li) deposition of lithium metal batteries (LMBs). However, the spontaneously-formed SEI is non-homogenous in the composition and structure and thus cause oriented distribution of Li + flux, which leads to the detrimental formation of lithium dendrites and poor cyclability of batteries. Here we propose a vertical & lateral ion-flux modulated ion-conductive SEI for high-voltage Li-metal batteries. A fluorinated MCM-41 (FMCM-41) modified LiPF 6 electrolyte is designed to construct the SEI film, which consists of homogenously distributed LiF and Li x SiO y , to regulate Li + transport paths in the lateral and the vertical direction, respectively, achieving uniform lithium plating. With the FMCM-41 modified electrolyte, the prepared Li||Li cell presents a long-term stability over 1000 h, and the Li||NCM622 full cell exhibits outstanding cycling performance with a high specific capacity of 169.9 mAh g -1 and a high-capacity retention of 93.3 % over 100 cycles at 0.5 C. This lateral-vertical concept provides a promising strategy for designing a desired SEI with uniform Li + transport paths to achieve ultra-long and high-rates lithium metal batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Cheng Ding,Yan Lu,Lihua Pu,Chengshuai Bao,Kaiying Shi,Jun Jin,Zhaoyin Wen
Lithium‑sulfur batteries, known for their high theoretical energy density, cost-effectiveness, and environmental friendliness, stand out as one of the most promising technologies in advanced secondary batteries. Nevertheless, they are facing challenges like polysulfide shuttling and the growth of lithium dendrites. In this study, we present the utilization of a bifunctional initiator, InF 3 , incorporated into DOL-based electrolytes for in-situ polymerization to mitigate polysulfide shuttling. Simultaneously, it promotes the development of a solid electrolyte interface (SEI) enriched with LiF and LiIn alloy on the lithium metal surface. The assembled Li|Li symmetric cells exhibit a high critical current density of 3.0 mA cm −2 , together with durable cycling performance over 4000 h at a current density of 0.5 mA cm −2 . Most importantly, benefiting from the effective blocking effect of PDOL-based polymer electrolytes and the robustness of the formed e − /Li + dual conductive SEI layer, the solid-state lithium‑sulfur batteries demonstrate excellent electrochemical performance, with a high retention capacity of 774.3 mA h g −1 after 200 cycles at a 0.2 C rate, showcasing significant potential for practical applications in high-energy-density solid-state batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 35
·15519-15529
·
IF 7.6
He Xuemei,Liu Hongyu,Zheng Chaohe,Tan Xin,Zhang Heng,Zheng Qiaoji,Lam Kwok-Ho,Lin Dunmin
The instability of the zinc/electrolyte interphase remains a critical bottleneck for advancing aqueous zinc-ion batteries (AZIBs). Here, we demonstrate a shift from passive surface protection to active “smart” interphase regulation by introducing BIS-TRIS hydrochloride (BT) as a dynamic multifunctional electrolyte additive. Unlike conventional additives, BT enables a proton-coupled mechanism within the electric double layer that dynamically buffers interfacial pH fluctuations and directs the in situ formation of an adaptive solid–electrolyte interphase (SEI). The resulting SEI features a conductive inorganic inner layer and is continuously self-stabilized under operating conditions, ensuring robust interphase integrity. In situ Raman spectroscopy intuitively captures the establishment of a dynamic steady-state interphase microenvironment, which effectively suppresses H 2 O– and SO 4 2– -induced parasitic reactions. Benefiting from this intelligently regulated interphase, Zn||Zn cells exhibit an extended lifespan exceeding 2500 h at 5 mA cm –2 and 5 mAh cm –2 , while Zn//Cu cells deliver more than 3100 cycles with an average coulombic efficiency (CE) of 99.90% at 2 mA cm –2 and 0.5 mAh cm –2 . This work introduces proton-coupled intelligent interphase regulation as a promising strategy for enabling next-generation durable metal batteries.
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DOI
高影响因子
DALTON TRANSACTIONS
·
2025
·Vol. 54
·期 11
·4743-4754
·
IF 3.3
Zhenbo Peng,Bifen Chen,Shan Yu,Kaiyu Wu,Farao Zhang,Peng Gao
Na3V2(PO4)3 (NVP) suffers from poor ionic and electronic conductivity. Herein, a dual-optimized design with Cu2+ doping and wrapping in tubular carbon nanotubes (CNTs) is proposed for the first time. This strategy not only modifies the internal electronic structure but also regulates the morphological features of NVP material. Notably, Cu2+ occupying V3+ sites introduces favorable p-type doping effects. Consequently, newly generated holes can act as charge carriers to improve electronic conductivity. Meanwhile, to conserve the charge balance of the whole system, a series of distinctive Na3+xV2−xCux(PO4)3 cathode materials are designed. The Na-rich scheme maintains charge integrity, as well as supplying more active Na+ to take part in the reversible de-intercalation process. Due to the larger ionic radius of Cu2+, Cu2+ doping plays a great role as a pillar to support the crystal skeleton and then expand the Na+ migration channels, thus significantly elevating the ionic transport rate. Furthermore, moderate CNTs are wrapped around the active grains, functioning together with coated carbon layers to construct a highly conductive framework, enhancing electronic transfer. Meanwhile, the tubular CNTs and porous morphology effectively increase the contact areas between active particles and electrolyte, providing more active sites. Furthermore, in situ EIS measurement demonstrates that a stable SEI membrane covers the cycled Na3.07V1.93Cu0.07(PO4)3@CNTs grains to maintain electrode stability and prevent the occurrence of side-effects. Comprehensively, the Na3.07V1.93Cu0.07(PO4)3@CNTs sample releases 124.2 mA h g−1 at 0.1 C. It releases 101.9 and 98.6 mA h g−1 at 10 and 50 C, suggesting superior rate capability.
研究领域:
材料科学
·
电化学
·
储能
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Energy
·
2020
·
IF 16.602
Feihong Ren,Zhendong Li,Yun Zhu,Patrice Huguet,Stefano Deabate,Deyu Wang,Zhe Peng
Uneven nucleation and fragile solid electrolyte interphase (SEI) restrict the practical application of lithium (Li) metal anode. A versatile strategy to simultaneously overcome these two drawbacks is critical for Li metal batteries (LMBs). Herein we propose an “aggressive aluminum (Al) pulverization” strategy to form abundant artificial nucleation sites and robust SEI films adjacently, leading to homogeneous Li deposition/stripping and high Li Coulombic efficiency. A core-shell structure with Al core and alumina-silica (Al 2 O 3 –SiO 2 ) shell, Al@Al 2 O 3 –SiO 2 (AAS), could be easily synthesized, by modulating the chemical diffusion of silicon (Si) element towards Si–Al alloy surface. The active SiO 2 sites not only contribute to form the robust SEI layer, but also facility the lithiation of the AAS, accelerating the conversion of reversible Li–Al alloy into inert Li 3 Al 2 phase. The as-generated AAS with Li 3 Al 2 and Li 12 Si 7 phases possess negligible Li nucleation over-potential (~0.7 mV), serving as an optimal structure for dendrite-free Li plating/stripping with a prolonged life-span of 6 times longer than that of the unprotected counterpart in carbonate electrolytes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
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
·
储能
·
电池技术
✓ 已验证
DOI
高影响因子
Green Energy & Environment
·
2024
·
IF 10.7
Wei Lu,Anshun Zhao,Qiuxu Chen,Sihan Liu,Mingxi Yu,Zihao Wang,Ze Gao,Xue Zhao,Guiru Sun,Ming Feng
An artificial solid electrolyte interphase (SEI) with lithiophilic sites and chemical bonds anchoring lithium polysulfides (LiPSs) has been developed as a potential solution to protect the lithium (Li) metal anode of Lithium−sulfur (Li–S) batteries. This strategy aims to guide consistent Li deposition and relieve lithium corrosion. Herein, the evolution process of lithiophilic sites based on aluminum fluoride (AlF 3 ) in an artificial SEI is disclosed in Li–S batteries with metal−based lithiophilic sites. The polyester polymer (PMMA and PPC)/AlF 3 artificial SEI (MPAF−SEI) was homogeneously anchored on Li anode by in−situ polymerization. The conversion of AlF 3 into Li–Al and LiF lithiophilic sites effectively reduce the Li nucleation overpotential and prevents the formation of Li dendrites. At the same time, the polymer can anchor LiPSs by chemical bonds and prevents Li corrosion. The optimized MPAF−SEI protected Li demonstrates excellent stability for over 3000 h at a capacity of 1 mAh cm −2 in Li || Li symmetric cells. The Li–S battery with low N/P (4) exhibits a capacity of 532.6 mAh g −1 over 300 cycles lifespan at 0.5 C.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
MOLECULES
·
2022
·Vol. 27
·期 22
·7827
·
IF 4.927
Yunhao Zhao,Yueyue Wang,Rui Liang,Guobin Zhu,Weixing Xiong,Honghe Zheng
The overall electrochemical performance of natural graphite is intimately associated with the solid electrolyte interphase (SEI) layer developed on its surface. To suppress the interfacial electrolyte decomposition reactions and the high irreversible capacity loss relating to the SEI formation on a natural graphite (NG) surface, we propose a new design of the artificial SEI by the functional molecular cross-linking framework layer, which was synthesized by grafting acrylic acid (AA) and N,N′−methylenebisacrylamide (MBAA) via an in situ polymerization reaction. The functional polymeric framework constructs a robust covalent bonding onto the NG surface with —COOH and facilitates Li+conduction owing to the effect of the —CONH group, contributing to forming an SEI layer of excellent stability, flexibility, and compactness. From all the benefits, the initial coulombic efficiency, rate performance, and cycling performance of the graphite anode are remarkably improved. In addition, the full cell using the LiNi0.5Co0.2Mn0.3O2cathode against the modified NG anode exhibits much-prolonged cycle life with a capacity retention of 82.75% after 500 cycles, significantly higher than the cell using the pristine NG anode. The mechanisms relating to the artificial SEI growth on the graphite surface were analyzed. This strategy provides an efficient and feasible approach to the surface optimization for the NG anode in LIBs.Keywords:natural graphite;artificial SEI;in situ polymerization;lithium-ion batteries
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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