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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

In-situ-derived carbon coated sea urchin-like Na3V2(PO4)3 from V2C MXene for high-performance capacitive deionization

Lanlan Yu,Ningning Liu,Baojun Liu,Fei Yu,Jie Ma

Cathode materials with high capacity and cyclic durability are urgently needed for capacitive deionization . Na 3 V 2 (PO 4 ) 3 is an emerging pseudocapacitive candidate for this process on account of its high capacity and Na + reversible insertion, while it suffers from the intrinsic low electrical conductivity and small electrolyte-accessible surface area. Herein, a sea urchin-like Na 3 V 2 (PO 4 ) 3 @carbon (NVP@C) compound material was synthesized from MXene-V 2 C via hydrothermal method followed by annealing treatment, and then assembled as capacitive deionization (CDI) electrode material . Benefiting from three-dimensional sea urchin-like structure, where the nanoneedles of NVP@C serve as fast transport channel for Na + , NVP@C performed high specific capacity (437 F g −1 at 5 mV s −1 ) and fast ionic diffusion kinetics. Moreover, the NVP@C showed attractive desalination performance as cathode material for CDI, achieving a remarkable adsorption capacity of 74.0 mg g −1 in a NaCl salt solution (1000 mg L −1 ) and long life cycle stability. The present work provides a novel perspective to construct practical redox-active and stable CDI electrode with 3D structure from MXene for highly capacitive and durable desalination application .

研究领域: 材料科学 · 电化学 · 环境工程 · 能源存储 · 纳米材料 · 水处理技术
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Architecting O3/P2 layered oxides by gradient Mn doping for sodium-ion batteries

Wenbin Wu,Ping Zhang,Siqi Chen,Xiaohong Liu,Guilin Feng,Meihua Zuo,Wangyan Xing,Bin Zhang,Weifeng Fan,Heng Zhang,Ping Zhang,Jie Zhang,Wei Xiang

O3 phase layered oxides are highly attractive cathode materials for sodium-ion batteries because of their high capacity and decent initial Coulombic efficiency. However, their rate capability and long cycling life are unsatisfactory due to the narrow Na + transfer channel and irreversible phase transitions of O3 phase during sodiation/desodiation process. Constructing O3/P2 multiphase structures has been proven to be an effective strategy to overcome these challenges. In this study, we synthesized bi-phasic structured O3/P2 Na(Ni 2/9 Fe 1/3 Cu 1/9 Mn 1/3 ) 1- x Mn x O 2 ( x  = 0.01, 0.02, 0.03, 0.04, 0.05) materials through Mn doping during sodiation process. Benefiting from surface P2 phase layer with the enhanced Na + transfer dynamics and high structural stability , the Na(Ni 2/9 Fe 1/3 Cu 1/9 Mn 1/3 ) 0.98 Mn 0.02 O 2 (NFCM-M2) cathode delivers a reversible capacity of 139.1 mA h g −1 at 0.1 C, and retains 71.4 % of its original capacity after 300 cycles at 1 C. Our work provides useful guidance for designing multiphase cathodes and offers new insights into the structure-performance correlation for sodium-ion cathode materials.

研究领域: 材料科学 · 电化学 · 能源存储 · 无机化学 · 固态化学
✓ 已验证 DOI 高影响因子
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Small Methods · 2024 ·Vol. 8 ·期 7 ·2301233 · IF 10.7

Tin Hybrid Flow Batteries with Ultrahigh Areal Capacities Enabled by Double Gradients

Xiaolin Ye,Ningxin Xiong,Shaopei Huang,Qixing Wu,Hongning Chen,Xuelong Zhou

Tin-based hybrid flow batteries have demonstrated dendrite-free morphology and superior performance in terms of cycle life and energy density. However, the quick accumulation of electrodeposits near the electrode/membrane interface blocks the ion transport pathway during the charging of the battery, resulting to a very limited areal capacity (especially at high current density) that significantly hinders its deployment in long-duration storage applications. Herein, a conductivity-activity dual-gradient design is disclosed by electrically passivating the carbon felt near the membrane/electrode interface and chemically activating the carbon felt near the electrode/current collector interface. In consequence, the tin metals are preferentially plated at the region near electrode/current collector, preventing the ion transport pathway from being easily blocked. The resultant gradient electrode demonstrated an unprecedentedly high areal capacity of 268 mAh cm −2 at a current density of as high as 80 mA cm −2 . Numerical modeling and experimental characterizations show that the dual-gradient electrode differs from conventional electrodes with regard to their reaction current density distribution and electrodeposit distribution during charging. This work demonstrates a new design strategy of 3D electrodes for hybrid flow batteries to induce a desirable distribution of electrodeposits and achieve a high areal capacity at commercially relevant current densities.

研究领域: 电化学储能 · 材料科学 · 能源化学 · 电池技术 · 功能材料 · 电化学工程
✓ 已验证 DOI 高影响因子
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IONICS · 2016 ·Vol. 23 ·期 10 ·2603-2611 · IF 2.119

Hybrid solid electrolytes with excellent electrochemical properties and their applications in all-solid-state cells

Chen Shaojie,Zhao Yanran,Yang Jing,Yao Lili,Xu Xiaoxiong

Three types of inorganic electrolytes [Li 10 GeP 2 S 12 (LGPS), 75Li 2 S·24P 2 S 5 ·1P 2 O 5 (LPOS), Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP)] with different particle sizes and electrochemical properties are selected as active fillers incorporated into poly(ethylene oxide) (PEO) matrix to fabricate hybrid solid electrolytes. The optimum composition of each filler is found in consideration of ionic conductivity. Their electrochemical characteristics are investigated. The optimal conductivities are 1.60 × 10 −5 , 1.18 × 10 −5 , and 2.12 × 10 −5  S cm −1 at room temperature for PEO-1%LGPS, PEO-1%LPOS, and PEO-20%LAGP, respectively. The electrochemical stability windows of these hybrid solid electrolytes are all above 5 V (vs. Li + /Li). The results show that these fillers have positive effects on the ionic conductivity, lithium ion transference number, and electrochemical stability. The relationship between the type of filler and electrochemical properties has been investigated. All-solid-state cells LiFePO 4 /Li are fabricated and present fascinating electrochemical performance with high capacity retention and good cycling stability. This work provides promising electrolytes prepared by a simple method.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态离子学 · 功能材料 · 锂电池技术
✓ 已验证 DOI 高影响因子
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Small · 2023 ·Vol. 19 ·期 39 ·2302691 · IF 13.3

Improving Room-Temperature Li-Metal Battery Performance by In Situ Creation of Fast Li+ Transport Pathways in a Polymer-Ceramic Electrolyte

Jing Yu,Guodong Zhou,Yueqing Li,Yuhao Wang,Dengjie Chen,Francesco Ciucci

Composite polymer-ceramic electrolytes have shown considerable potential for high-energy-density Li-metal batteries as they combine the benefits of both polymers and ceramics. However, low ionic conductivity and poor contact with electrodes limit their practical usage. In this study, a highly conductive and stable composite electrolyte with a high ceramic loading is developed for high-energy-density Li-metal batteries. The electrolyte, produced through in situ polymerization and composed of a polymer called poly-1,3-dioxolane in a poly(vinylidene fluoride)/ceramic matrix, exhibits excellent room-temperature ionic conductivity of 1.2 mS cm −1 and high stability with Li metal over 1500 h. When tested in a Li|electrolyte|LiFePO 4 battery, the electrolyte delivers excellent cycling performance and rate capability at room temperature, with a discharge capacity of 137 mAh g −1 over 500 cycles at 1 C. Furthermore, the electrolyte not only exhibits a high Li + transference number of 0.76 but also significantly lowers contact resistance (from 157.8 to 2.1 Ω) relative to electrodes. When used in a battery with a high-voltage LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathode, a discharge capacity of 140 mAh g −1 is achieved. These results show the potential of composite polymer-ceramic electrolytes in room-temperature solid-state Li-metal batteries and provide a strategy for designing highly conductive polymer-in-ceramic electrolytes with electrode-compatible interfaces.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态电池 · 高分子化学 · 无机非金属材料
✓ 已验证 DOI 高影响因子
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Small · 2024 ·Vol. 20 ·期 31 ·2310912 · IF 13

Vertically-Aligned Card-House Structure for Composite Solid Polymer Electrolyte with Fast and Stable Ion Transport Channels

Xunzhi Miao,Jianhe Hong,Shuo Huang,Liye Ding,Fang Wang,Min Liu,Quanquan Zhang,Hongyun Jin

All-solid-state lithium batteries (ASSLBs) are highly promising as next-generation energy storage devices owing to their potential for great safety and high energy density. This work demonstrates that composite solid polymer electrolyte with vertically-aligned card-house structure can simultaneously improve the high rate and long-term cycling performance of ASSLBs. The vertical alignment of laponite nanosheets creates fast and uniform Li + ion transport channels at the nanosheets/polymer interphase, resulting in high ionic conductivity of 8.9 × 10 −4 S cm −1 and Li + transference number of 0.32 at 60 °C, as well as uniformly distributed solid electrolyte interphase. Such electrolyte is characterized by high mechanical strength, low flammability, excellent structural stability and stable ion transport channels. In addition, the ASSLB cell with the electrolyte and LiFePO 4 cathode delivers a high discharge specific capacity of 124.8 mAh g −1 , which accounts for 85.6% of its initial capacity after 500 cycles at 1C. The reasonable design through structural control strategy by interconnecting the vertically-aligned nanosheets open a way to fabricate high performance composite solid polymer electrolytes.

研究领域: 材料科学 · 电化学 · 能源存储 · 高分子科学 · 纳米材料 · 电池技术
✓ 已验证 DOI 高影响因子
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ACS Applied Energy Materials · 2023 · IF 6.4

Oxygen Vacancy Migration in Ca2Ga2+xGe1–xO7–0.5x Melilite

Xianyi Wei,Xiaohui Li,Xiaoge Wang,Jian Liu,Zhaoji Luo,Sihao Deng,Lunhua He,Junliang Sun,Xiaojun Kuang,Xianran Xing

Compared with interstitial defects, vacancy-mediated oxide ion conduction in melilite family received little attention. Herein, melilite-type oxide ion conductors of Ga-excess compositions Ca2Ga2+xGe1–xO7–0.5x (0 ≤ x ≤ 0.15) demonstrate remarkable oxygen vacancy migration by experimental and computational verifications. Neutron powder diffraction data and defect formation energies of oxygen vacancy revealed that oxygen vacancies favor occurring at the bridging O sites shared by four-linked (Ga/Ge)O4 tetrahedra, opening the 5-fold rings coupled by the local structure relaxation around the oxygen vacancies. Molecular dynamics simulations revealed that the oxygen vacancies migration involves the cooperative rotation and deformation of adjacent tetrahedra, allowing the opening and re-forming of 5-fold rings in melilite structure. This study provides structural chemistry mechanisms on oxygen vacancy conduction in melilite structure.

研究领域: 材料科学 · 固态化学 · 离子传输 · 计算材料科学
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2023 ·Vol. 11 ·期 11 ·5615-5626 · IF 11.9

B-site mixed cationic tetrahedral layer confined the concentration and mobility of interstitial oxygen in mellite family

Xiaohui Li,Xianyi Wei,Xiaoge Wang,Chenjie Lou,Wenda Zhang,Jungu Xu,Zhaoji Luo,Mingxue Tang,Sihao Deng,Lunhua He,Xianran Xing,Junliang Sun,Xiaojun Kuang

Melilite-type oxide ion conductors usually were observed in pure gallate compounds. Here a new mellite interstitial oxide ion conductor Ca2−xLaxGa2GeO7+x/2 (0 ≤ x ≤ 0.15) was developed by the substitution of La3+ for Ca2+ in Ca2Ga2GeO7 containing mixed GaO4/GeO4 tetrahedral layers. Neutron powder diffraction data indicated that the introduced interstitial oxide ions were accommodated in the distorted pentagonal rings, close to the coordination environment of (Ga2/Ge)O4 containing terminal oxygen. Defect formation energy calculations further reveal that the interstitial oxygen not only favors to approach the GaO4 tetrahedra, in agreement with studies of other pure gallate systems, but also is confined to the GeO4 tetrahedra. Bond-valence-energy landscape calculations and molecular dynamics simulations revealed that the interstitial oxide ions were transported among the pentagonal rings within the tetrahedral layers through a cooperative mechanism involving the synergistic knock-on motion between interstitial and framework oxygens. In Ca2Ga2GeO7, the La3+ substitution for Ca2+ only extended up to x = 0.15, which is much lower than those in the La–(Ca/Sr/Ba) based gallate mellites. The x = 0.15 composition resulted in oxide ion conductivities ∼2.79 × 10−5 S cm−1 to 1.68 × 10−3 S cm−1, with oxygen transport numbers of ∼92.65%, two orders of magnitude higher than that of the parent material. However, compared with pure gallate melilite interstitial oxide ion conductors with the same interstitial oxide ion concentrations, Ca1.85La0.15Ga2GeO7.075 has about one order of magnitude lower conductivity. The lower interstitial oxide ion concentration and conductivity in Ca2−xLaxGa2GeO7+x/2 reveal that although Ge4+ has similar chemical properties to the adjacent Ga3+, the subtle differences in size and the resultant covalent bonding ability make the mixed GaO4 and GeO4 tetrahedral layers in mellite unfavorable for accommodation and transportation of interstitial oxygens.

研究领域: 材料科学 · 固体离子学 · 能源材料 · 晶体化学 · 离子传输
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Materials Today Energy · 2024 · IF 9

To achieve fast ion transport of engineered electrolyte and ultra-high rate of defected Nb16W5O55-based anode

Yaqing Guo,Xuemei Zeng,Mengting Zhou,Yuan-Cheng Cao,Yifei Yuan,Xiaobin Liao,Kun He

The maximum output power and minimum charge time of a lithium-ion battery depend on ion transport and electron transport . The electron conduction/ion diffusion within the electrochemically active materials and the ion mobility of the electrolyte usually represent the fundamental limits of the battery charge and discharge rates. Nb 16 W 5 O 55 is notable for its exceptional lithium-ion mobility and high electronic conductivity , making it a popular choice for fast-charging anode materials . However, the lithium-ion diffusion capability of the electrolyte is also crucial in determining the overall fast-charging performance of the battery. This can be a limiting factor for Nb 16 W 5 O 55 -based batteries. This work delves into the impact of electrolyte composition on fast-charging performance by examining the electrochemical properties of electrolytes with varying concentrations, in conjunction with molecular dynamics simulation . Specifically, increasing the concentration of LiTFSI salt alters the solvation structure of lithium ions due to the increasing coordination numbers of TFSI − and Li + , which hampers lithium-ion diffusion. Additionally, low-concentration electrolytes struggle with rapid mass transfer due to fewer lithium-ion carriers, limiting ultra-high-rate performance. To address these challenges, the solvation structure of the electrolyte was optimized, leading to enhanced fast-charging and discharging performance.

研究领域: 电化学 · 能源材料 · 电池技术 · 锂离子电池 · 离子传输
✓ 已验证 DOI 高影响因子
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