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基于阴离子-溶剂配位的镁金属负极固体电解质界面新型调控策略

A Novel Regulation Strategy of Solid Electrolyte Interphase Based on Anion-Solvent Coordination for Magnesium Metal Anode.

作者信息

Tang Kun, Du Aobing, Du Xiaofan, Dong Shanmu, Lu Chenglong, Cui Zili, Li Longshan, Ding Guoliang, Chen Fengxian, Zhou Xinhong, Cui Guanglei

机构信息

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, No. 189 Songling Road, Qingdao, 266101, China.

College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, No. 53 Zhengzhou Road, Qingdao, 266042, China.

出版信息

Small. 2020 Dec;16(49):e2005424. doi: 10.1002/smll.202005424. Epub 2020 Nov 17.

Abstract

Magnesium (Mg) metal anode is a highly desirable candidate among various high energy density metal anodes, possessing higher volumetric capacity and better safety characteristic compared to lithium metal. However, most Mg salts in conventional Mg electrolytes easily react with Mg metal to form blocking layers, leading to inferior reversibility of Mg plating/stripping. Here, a stable Mg -conducting solid electrolyte interphase (SEI) is successfully constructed on Mg metal anode by regulating the molecular-orbital-energy-level toward an aluminum(III)-centered anion Mg salt through anion-solvent coordination. Of which, the LUMO energy level of perfluorinated pinacolatoaluminate (Al(O C (CF ) ) , abbreviated as FPA) anion has been adjusted by coordinating with solvent molecule (tetrahydrofuran) for facilitating the formation of advantageous SEI. The existence of SEI formed by FPA anion greatly improves the reversibility and long-term stability of Mg plating/stripping process. More importantly, based on this aluminum(III)-centered Mg electrolyte, the Mo S /Mg batteries can achieve a fantastic cycle performance of 9000 cycles, proving the beneficial effect of SEI on the cycling stability of Mg battery system. These findings open up a promising avenue to construct stable and compatible SEI on Mg metal anode, and lay significant foundations for the successful development of rechargeable Mg metal batteries.

摘要

镁(Mg)金属阳极是各种高能量密度金属阳极中非常理想的候选者,与锂金属相比,它具有更高的体积容量和更好的安全特性。然而,传统镁电解质中的大多数镁盐很容易与镁金属反应形成阻挡层,导致镁电镀/剥离的可逆性较差。在此,通过阴离子-溶剂配位将分子轨道能级调节至以铝(III)为中心的阴离子镁盐,成功地在镁金属阳极上构建了稳定的镁导电固体电解质界面(SEI)。其中,全氟频哪醇铝酸酯(Al(OC(CF3)2)3,缩写为FPA)阴离子的最低未占分子轨道(LUMO)能级通过与溶剂分子(四氢呋喃)配位进行了调整,以促进有利SEI的形成。由FPA阴离子形成的SEI的存在极大地提高了镁电镀/剥离过程的可逆性和长期稳定性。更重要的是,基于这种以铝(III)为中心的镁电解质,MoS2/Mg电池可以实现9000次循环的出色循环性能,证明了SEI对镁电池系统循环稳定性的有益作用。这些发现为在镁金属阳极上构建稳定且兼容的SEI开辟了一条有前途的途径,并为可充电镁金属电池的成功开发奠定了重要基础。

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