ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Dan Huang,Shuangshuang Tan,Maosheng Li,Dandan Wang,Chunhua Han,Qinyou An,Liqiang Mai
The application of high-energy Mg/S batteries was obstructed by the insufficiency of low-cost and non-nucleophilic electrolyte. In this work, a non-nucleophilic electrolyte was prepared by facilely dissolving Mg(CF3SO3)2, MgCl2, and AlCl3 in 1,2-dimethoxyethane (DME). The equilibrium species of the MTB electrolyte mainly comprise [Mg2(μ-Cl)2(DME)4]2+ and [(CF3SO3)AlCl3]−, which are generated by dehalodimerization reaction and Lewis acid–base reaction, respectively. The electrolyte exhibits a highly efficient reversible Mg deposition/dissolution, low overpotential of around 250 mV, and good oxidative stability up to 3.5 V after conditioning. The conditioning process that the active [Mg2(μ-Cl)2(DME)4]2+ species transforms into [Mg3(μ3-Cl)(μ2-Cl)2(DME)7]3+ was demonstrated, owing to the irreversible deposition of Al3+ on Mg foil. More importantly, this electrolyte exhibited good compatibility and kinetics for reversible Mg/MgSx redox, resulting in a high specific capacity of 866 mAh g–1 at 200 mA g–1 and high power density of 550 W kg–1. This work offers a new direction for low-cost, non-nucleophilic electrolyte and paves the way to explore high-power Mg/S batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wen Ren,Di Wu,Yanna NuLi,Xuan Zhang,Jun Yang,Jiulin Wang
The electrolyte based on magnesium bis(diisopropyl)amide (MBA), a low-cost and non-nucleophilic organic magnesium salt, is proposed to be an admirable alternative for rechargeable magnesium batteries but suffers from limited ionic conductivity and an inferior electrochemical window in the commonly used ether solvents. In this work, the 1-butyl-1-methylpiperidinium bis(trifluoromethyl sulfonyl)imide (PP14TFSI) ionic liquid as the cosolvent of tetrahydrofuran (THF) in chlorine-free MBA-based electrolytes has been first demonstrated to remarkably improve the ionic conductivity and broaden the oxidative stable potential (2.2 V vs Mg/Mg2+) on stainless steel. Reversible Mg electrochemical plating/stripping with a low overpotential below 200 mV and ca. 90% Coulombic efficiency are obtained. The current density of Mg plating/stripping is increased 238 times after the addition of PP14TFSI, where the mechanism of competitive coordination of TFSI– making an easier Mg plating/stripping is proposed theoretically. The MBA-2AlF3 electrolyte with a ratio-optimized THF/PP14TFSI cosolvent exhibits good compatibility with the Mo6S8 cathode. Furthermore, the Se@pPAN|Mg full cell exhibits an initial capacity of 447.8 mAh g–1 and as low as ∼0.66% capacity decay per cycle for more than 70 cycles at 0.2 C with the synergy of LiTFSI additives. The facile modification strategy of ionic liquid in the MBA-based electrolyte sheds inspiring light on exploring non-nucleophilic and chlorine-free electrolytes for practical rechargeable magnesium batteries.
研究领域:
材料科学
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电化学
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储能技术
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电池技术
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无机化学
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物理化学
✓ 已验证
DOI
高影响因子
Energy & Environmental Science
·
2017
·Vol. 10
·期 12
·2616-2625
·
IF 29.518
Aobing Du,Zhonghua Zhang,Hongtao Qu,Zili Cui,Lixin Qiao,Longlong Wang,Jingchao Chai,Tao Lu,Shanmu Dong,Tiantian Dong,Huimin Xu,Xinhong Zhou,Guanglei Cui
Two-electron transfer chemistry based on earth-abundant Mg and S offers great possibilities of delivering higher energy density than current Li-ion technology. The development of non-nucleophilic electrolytes that reversibly and efficiently plate and strip Mg is believed to be a major obstacle to the implementation of this divalent battery technology. In this study, we present a new type of organic magnesium borate-based electrolyte that primarily comprises tetrakis(hexafluoroisopropyl)borate anions [B(HFP)4]− and solvated cations [Mg4Cl6(DME)6]2+, which was synthesized via a facile in situ reaction of tris(hexafluoroisopropyl)borate [B(HFP)3], MgCl2 and Mg powder in 1,2-dimethoxyethane (DME). Rigorous analyses including NMR, mass spectroscopy and single-crystal XRD were conducted to identify the equilibrium species in the abovementioned solution. The as-prepared Mg-ion electrolyte exhibited unprecedented Mg plating/stripping performance, such as high anodic stability up to 3.3 V (vs. Mg/Mg2+), high ionic conductivity of 5.58 mS cm−1, a low overpotential of 0.11 V for plating processes and Coulombic efficiencies greater than 98%. By virtue of the non-nucleophilic nature of this electrolyte, a fully reversible Mg/S battery was constructed that displayed an extremely low overpotential of 0.3 V and a high discharge capacity of up to 1247 mA h g−1 and yielded a specific energy of approximately 1200 W h kg−1 (10 times higher that of the Chevrel benchmark) based on the weight of active sulfur. More significantly, commonly used sulfur-carbon nanotube (S-CNTs) cathodes with S contents of 80 wt% and S loadings of 1.5 mg cm−2 were demonstrated to withstand more than 100 cycles without obvious capacity decay and to enable fast conversion processes, which achieved a charging current rate of up to 500 mA g−1. Our findings convincingly validate the pivotal role of the newly designed non-nucleophilic Mg-ion electrolyte for practical Mg/S battery chemistry.
研究领域:
电化学
·
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Xueting Huang,Jiaxin Wen,Jinglei Lei,Guangsheng Huang,Fusheng Pan,Lingjie Li
A cost-effective and highly efficient electrolyte with a wide electrochemical window, high reversibility of Mg plating/stripping, non-/low-corrosivity, good compatibility with cathode materials, and tolerance of trace water and impurity is crucial for the commercialization of rechargeable magnesium batteries. In this work, a novel boron-centered non-nucleophilic electrolyte that meets all the above requirements is prepared via a facile and economic approach from the raw materials B(TFE)3/MgCl2/CrCl3/Mg (BMCM). The as-prepared BMCM electrolyte is mainly composed of tetracoordinated anions [B(TFE)4]− and solvated cations [Mg2(μ-Cl)2(DME)4]2+. The BMCM electrolyte demonstrates attractive electrochemical performance, with a low overpotential (∼139 mV), a high Coulombic efficiency (∼97%), a high anodic stability (∼3.5 V vs Mg/Mg2+), and a long-term (more than 500 h) cycling stability. Moreover, BMCM shows good compatibility with the CuS cathode material. The CuS|BMCM|Mg full cell delivers a discharge specific capacity of 231 mAh g–1 (at 56 mA g–1), which can retain ∼88% even after 100 cycles. Importantly, the BMCM electrolyte is cost-effective and tolerant of trace impurity and water, which has great potential to be commercialized. This work is expected to promote the development of practical rechargeable magnesium batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 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）