ADVANCED MATERIALS
·
2025
·
IF 26.8
Xin He,Yujie Zhang,Haomiao Li,Maoshu Xu,Qixing Li,Zidong Zhang,Jianping Luo,Yumeng Liu,Qingyuan Wang,Sihang Li,Min Zhou,Wei Wang,Kai Jiang,Kangli Wang
Electrolyte engineering to enhance the cathode-electrolyte interface stability is widely recognized as a promising strategy for achieving high-voltage lithium-ion batteries, which are currently hindered by the meta-stable surface of lithium-rich layered oxides. Despite significant progress in electrolyte development, clear design guidelines for high-voltage electrolytes remain lacking, making solvent selection unpredictable. Here, a dual-descriptor tailoring concept based on Mulliken charge (adsorption) and Laplacian bond order (antioxidation) to identify ideal solvent molecules for high-voltage electrolytes is proposed. This concept stabilizes meta-stable transition metal atoms in surface tetrahedral interstices through interactions between bottom solvent molecules and cathode dangling bonds. Acetonitrile (AN) is eventually selected as a promising bottom solvent that interacts strongly with unstable surface bonds, improving interfacial stability. Consequently, the prepared 0.6 Ah graphite||LCO pouch cell using AN-based electrolyte maintained a remarkable 80% capacity retention after 900 cycles with an average Coulombic efficiency of 99.92% at high cut-off voltage. This work revisits the interfacial stability mechanism across different electrolyte classes, where strong solvent adsorption mitigates the instability of the meta-stable Co spin state, reduces surface band overlap, and alleviates the instability of lattice oxygen at the interface. This dual-descriptor-guided design opens a new avenue for high-voltage Li-ion batteries is believed.
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高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Fangfang Shang,Hengdao Quan,Xiaoxun Ma
In this study, 3-trifluoromethylpyrazole (TMPZ) was developed as a multifunctional electrolyte additive to enhance wettability between separator and electrolyte, CEI formation and remove HF to improve the performance of Li/NCM622 batteries by experiment and theoretical calculation. After 200 cycles at 30 °C, the discharge capacity retention of batteries at 1 C with 0.5 wt% TMPZ additive is remarkably enhanced from 68.3 % to 83.2 %. The enhanced electrochemical performance of the batteries by adding TMPZ additive is evaluated by the spectroscopic characterization and theoretical calculation. It is demonstrated that TMPZ can generate uniform and dense CEI film via ring-opening electrochemical polymerization of TMPZ on the NCM622 electrode surface. The CEI film helps to suppress the breakdown of LiPF 6 electrolyte and the leaching of transition metals, effectively avoiding harmful side reactions between the NCM622 electrode and the electrolyte. Furthermore, introducing TMPZ can enhance the wettability between separator and electrolyte, therefore providing more channels of Li + to accelerate reaction kinetics of batteries.
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Journal of Energy Storage
·
2024
·
IF 8.9
Hongying Hou,Yixuan Wang,Xianxi Liu,Xiaohua Yu,Ju Rong,Yutao Niu,Meng Ye,Yanpeng Jia
Solid state lithium batteries have been encountering a bottle neck of high solid-solid interface resistance of the membrane/electrode assembly, which is one industrial pain point. Herein, the composite solid electrolyte materials were designed and prepared to act as the double functions of solid state electrolyte membrane and the electrode binder for constructing a continuous homogeneous Li + transmission channels with high compatibility and ionic conductivity . Firstly, dopamine was oxidized and self-polymerized on the surface of polyvinylidene fluoride hexafluoropropylene (PVDF-HFP) to form a polydopamine (PDA) active layer , and the zwitterionic betaine sulfonate (SB) was chemically grafted onto the PDA active layer by Michael addition reaction. Secondly, the composite solid electrolyte materials were prepared by mixing the resultant SB-modified PVDF-HFP was mixed with different contents (0 %, 10 %, 20 %, 30 %) of Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 (LLZTO) and 20 % bis(trifluoromethane) sulphonyl lithium (LiTFSI). Finally, a series of composite solid electrolyte membranes were prepared by scraping method and labeled as 0%LLZTO/SB-PVDF-HFP/LiTFSI, 10%LLZTO/SB-PVDF-HFP/LiTFSI, 20 %LLZTO/SB-PVDF-HFP/LiTFSI, 30%LLZTO/SB-PVDF-HFP/LiTFSI, respectively. As expected, the cell with optimal 20 %LLZTO/SB-PVDF-HFP/LiTFSI as the solid electrolyte membrane and the electrode binder delivered the reversible capacity of 135.2 mAh/g at 1.0C and maintained high capacity retention of 94.8 % for 200 cycles. The construction of the continuous and homogeneous ion transmission channels should be responsible for high Li-storage performances by improving the interface compatibility of the membrane/electrode assembly and promoting the Li + transmission.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Tian Yang,Fengming Ma,Xinqun Zhang,Ya'nan Yang,Jinsheng Lv,Zifeng Jin,Liru Wang,Huimin Gao,Xiaolin Wang,Nan Chen
Rechargeable aqueous magnesium ion batteries (AMIBs) are considered a promising energy storage system due to the relatively high energy density, excellent rate performance and reversibility, and absence of dendrite formation during cycling. However, the high surface charge density of Mg 2+ ions results in slow diffusion kinetics, and high voltage leads to excessive electrolyte decomposition at the electrode/aqueous electrolyte interface, thereby limiting the development of high-energy–density MIBs. In this work, we extend the electrochemical stability window of the aqueous electrolyte to 2.1 V by using a hybrid ion superconcentrated electrolyte at concentrations not achievable with Mg 2+ electrolytes alone. The AMIB with a water-in-salt (WIS) electrolyte delivers discharge capacities of up to 200.6 and 84.4 mAh g −1 , and energy densities of 170.1 and 68.1 Wh Kg −1 at 0.5 and 20 A g −1 , respectively, representing excellent rate performance, while retaining 85 % of the specific capacity after 2000 cycles. Additionally, we explore the corresponding electrochemical reaction mechanism, revealing the synergistic effect of Mg 2+ and Li + ions in the charge/discharge process, which supports the excellent electrochemical performance of AMIB.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Cai Liu,Peng Zhao,Keren Lu,Shuai Han,Chao Zhang,Xifeng Xia,Wu Lei,Qiubo Guo,Qingli Hao
Heterostructured composites, inheriting the integrated properties of the individual components due to the synergistic effect, have engendered great attention in materials science and energy storage. However, conventional biphasic heterostructures not only optimize the performance of the composites but also aggregate the inevitable drawbacks, which can be addressed with the construction of the triphasic heterostructures by introducing an appropriate intermediate phase, significantly. Herein, a two-dimensional (2D) double-heterostructures MoSe 2 -TiO 2 -MXene anode is architected for Li-ion storage, which combines the advantages of the high theoretical capacity of MoSe 2 and metallic conductivity of MXene. Besides, the in-situ derived TiO 2 can alleviate the irreversible phase transition of MoSe 2 , arising from the low electronic/ionic conductivities, through electronic coupling effects. Meanwhile, the intermediate phase of TiO 2 can further prevent the restacking issue of MXene, thus sustaining its high conductivity. Finally, the three-dimensional (3D) printing technology is employed to further improve the kinetics of the electrodes for Li-ion capacitors (LICs), which deliver the power density of 5563 W kg −1 at an energy density of 51 Wh kg −1 , and a remarkable cycling stability for 20 000 cycles at 1 A g −1 . This work deepens the understanding of the influence of heterostructured engineering on the design of high-energy/power storage devices.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Boyang Zhang,Gesong Huang,Wenjie Huang,Xiaola Li,Wenzhao Huang,Ziyang Liang,Yuqing Liu,Chenyu Liu,Zhan Lin,Dong Luo
Undesirable interfacial reactions and the resulting capacity degradation hinder the widespread application of lithium-rich layered oxide (LLO) as a cathode in high-energy lithium-ion batteries. Herein, a method to suppress the interfacial reactions of LLO is devised by treating the carbonate precursor with weak-base salts to induce elemental segregation and promote particle growth, by which a rock-salt structure is in-situ constructed on the particle surface. This rock-salt structure is in excellent lattice alignment with the internal structure, which is conducive to enhancing surface structural stability and suppressing interfacial reactions. As a result, the two treated samples deliver a capacity retention ratio larger than 93.9 % after 200 cycles, with much superior voltage and capacity stability than the untreated sample. This in-situ construction method is beneficial for developing advanced LLO cathodes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Chenxi Tian,Da Lei,Yongchao Qian,Xiang-Yu Kong,Zhong Liu
The development of advanced membranes with precise ion selectivity is essential for efficient Li + /Mg 2+ separation. In this study, we synthesized a novel Lys-TMC membrane via a nucleophilic addition reaction between Lysine and trimesoyl chloride (TMC), yielding in a negatively charged surface interconnected by amide bonds. We systematically investigated the effects of varying Lys:TMC ratios on the membrane’s chemical structure, surface morphology, and ion separation performance. Our results revealed that the degree of cross-linking increases initially with the Lysine content, reaching an optimum at a Lys:TMC ratio of 10:1, where the membrane exhibited prominent Turing patterns on its surface. These patterns were critical for achieving effective ion separation. In contrast, excessive Lysine led to spontaneous polymerization, resulting in irregular ‘stone-like’ structures and the loss of Turing patterns. The optimally cross-linked Lys-TMC membrane displayed superior Li + /Mg 2+ separation performance, highlighting the crucial role of controlled cross-linking and Turing structure formation in enhancing ion selectivity. This work provides a mechanistic understanding of the relationship between Turing structure formation and ion sieving performance, offering a promising strategy for designing advanced separation membranes.
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Journal of Energy Storage
·
2024
·
IF 8.9
Meichen Guo,Wu Tang,Chenbin Tang,Xuesong He,Cong Fan
Organic cathodes face the challenge of dissolution problem, which severely hinders their electrochemical performances in lithium-ion batteries (LIBs). Herein, a bipolar organic cathode namely [ N , N ′-bis(4-(9H-carbazol-9-yl)phenyl)]-perylene-3,4,9,10-tetracarboxydiimide (PTCDI-DPC, 4-electron C T = 123 mAh g −1 ) is optimized by in-situ electropolymerization to eliminate its dissolution problem, and thus the good cathode performance of the electropolymerized PTCDI-DPC can be fully released in LIBs. In half cells, PTCDI-DPC delivers a peak specific capacity of 164 mAh g −1 and the good retention of 96 % over 450 cycles. Meanwhile, PTCDI-DPC still remains 121 mAh g −1 after 2000 cycles at 1 A g −1 , and a superior rate performance of 98 mAh g −1 at 8 A g −1 . Furthermore, the fabricated 2PF 6 -PTCDI-DPC||LiC 6 Li-ion full cells can possess the peak discharge capacity of 157 mAh g −1 cathode and a high energy density of 385 Wh kg −1 cathode in 1.4–4.3 V, with 90 % capacity retention during 2000 cycles at 1 A g −1 . As far as we know, the cathode performance of the improved PTCDI-DPC is one of the best among bipolar organic cathodes reported for LIBs.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Futing Sun,Zesen Gao,Yan Yang,Haijie Chen
The halides have attracted much attention as novel solid electrolytes because of their easy synthesis, high electrochemical stability, and high ionic conductivities. However, the reported halides for solid electrolytes are still understudied compared with the oxides and sulfides. Here, we studied the Li–Fe–Cl phases that include Li2FeCl4 and Li6FeCl8. Using the self-doping approach, a maximum ionic conductivity of 2.0 × 10–4 S cm–1 at 50 °C was achieved for Li1.8Fe1.1Cl4. It was improved by 3 orders of magnitude compared with that of Li2FeCl4 (8.27 × 10–7 S cm–1 at 50 °C). For the Li|Li1.8Fe1.1Cl4|Li half-cell, it cycled for 2000 h at 50 °C under a current density of 0.01 mA cm–2, indicating an acceptable compatibility between Li2FeCl4 and Li. Finally, an all-solid-state battery was successfully assembled with Li1.8Fe1.1Cl4@LFP as the cathode, Li1.8Fe1.1Cl4 as the electrolyte, and a Li sheet as the anode. The initial specific charge capacity of the battery was 76.36 mAh g–1 at 0.1C and 50 °C. The initial Coulombic efficiency was 73.06%. This study suggests Li2FeCl4 as a new solid electrolyte, and the introduction of Li vacancies into the Li site is an efficient way to improve the electrochemical properties of halides.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Hongxu Zhou,Weichen Han,Hongquan Chai,Hao Huang,Jingang Zheng,Han Zhang,Lixiang Li,Weimin Zhou,Baigang An,Chengguo Sun
Sluggish reaction kinetics in lithium–sulfur (Li–S) batteries has seriously hindered their practical application. Herein, a three-dimensional (3D) granular carbon skeleton decorated with nickel-rich NCM materials (NCM@3D-SP) is prepared as a cathode host for Li–S batteries, where the carbon matrix is rich in pore channels, can provide good conductivity and electrolyte diffusion, and NCM811 particles contribute abundant metal sulfides active sites through metal-ion exsolution. The different metal sulfides (NiS, Ni3S2, Ni7S6, and CoS) in heterogeneous structures exhibit outstanding catalytic and adsorption effects on polysulfides during cycling, where the ion diffusion coefficient is increased by approximately 2.5 times compared to the cathode without catalytic active sites (3D-SP). A Li metal battery using NCM@3D-SP/S as the cathode exhibits a capacity decay of only 0.051% per cycle at 2C after 500 cycles. Even at an ultra-high current density of 10C and a sulfur-loading of 6 mg cm−2, the cells maintain a stable reversible discharge capacity of 453.1 mA h g−1 after 500 cycles and 4 mA h cm−2. The incorporation of nickel-rich cathode materials and 3D sulfur host structure presents a novel strategy for high-catalytic activity cathodes of Li–S batteries.
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Nature Energy
·
2024
·
IF 49.7
Zhang Shuoqing,Li Ruhong,Deng Tao,Ma Qiang,Hong Xiang,Zhang Hao,Zhang Ruixin,Ding Shouhong,Wu Yongjian,Zhu Haotian,Li Menglu,Zhang Haikuo,Lu Di,Ma Baochen,Lv Ling,Li Yong,Chen Lixin,Shen Yanbin,Guo Rui,Fan Xiulin
Cation solvation is well understood in the bulk solution phase, but knowledge is limited regarding the electrode–electrolyte interface. The process by which cation solvation conforms to the interfacial field to form interphases remains unclear. Here we examine the synergistic effects of external and intramolecular fields on accommodating Li + solvates to the Li-metal anode, leading to dielectric-mediated transfer dynamics on the interface. At charged interfaces, cation–anion pairs arrange in a periodic oscillatory distribution. A low-oscillation amplitude exacerbates the electrolyte decomposition and increases surface impedance. We propose a dielectric protocol that maintains cation–anion coordination with a high oscillation amplitude at the interfaces, addressing these issues. Accordingly, we demonstrate a Li-metal pouch cell with an energy density of 500 Wh kg −1 at the Ah level using an ultra-lean electrolyte (1 g Ah −1 ). Our study offers insights into solid/liquid interfaces that are crucial in advancing battery technologies.
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Energy Technology
·
2017
·Vol. 6
·期 7
·1342-1351
·
IF 2.789
Ying Zhang,Ronglan Zhang,Fei Yang,Jianshe Zhao
Four kinds of binuclear metal phthalocyanines (MPcs) complexes M 2 (PcTN) 2 Nap and M 2 (PcTA) 2 Nap (M=Ni II , Zn II ) are synthesized and used in Li/SOCl 2 battery as electrocatalysts to enhance capacity and discharge voltage. Density functional theory (DFT) calculations are carried out to investigate the improvement in electrochemical performance by carefully observing the shape of the frontier molecular orbitals (MOs). It is confirmed that a close relationship exists between MOs and catalytic performance of MPcs. The variation in reduction potentials of electrolyte SOCl 2 are also related to the MOs. Based on cyclic voltammetry measurements and the energy gap of MOs, a reaction mechanism that involves an irreversible two-step electron transfer process can be deduced, and a better strategy for the selection of catalysts is obtained.
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