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    • Reversible Deposition/Dissolution of Double Hydroxides to Modulate Electrolyte Ph Enabling High-Performance Aqueous Zinc-Ion Batteries

    Yueang Jin,Xueqian Zhang,Yongchun Zhu,Jiajia Ye,Yitai Qian,Zhiguo Hou

    ACS applied materials & interfaces（2024）SCI 2区

    Univ Sci & Technol China | Hefei Normal Univ

    Cited 1|Views17
    Abstract
    Vanadium oxide has been extensively studied as a host of zinc ion intercalation but still suffers from low conductivity, dissolution, and byproduct accumulation during cycling. Here, we hydrothermally synthesize the VO2@MXene Ti3C2 (MV) composite and find that in the MV//3 M Zn(CF3SO3)(2)//Zn system, the double hydroxide Zn-12(CF3SO3)(9)(OH)(15)nH(2)O (ZCOH) uniformly covers VO2 during the charging process and dissolves reversibly during the discharge process. In situ X-ray diffraction of the MV combined with in situ pH measurements reveals that ZCOH acts as a pH buffer during cycling, which is beneficial to the cycling stability of batteries. And the theoretical calculation indicates that the decomposition energy required by ZCOH on the MV surface is lower than that on pure VO2, which is more conducive to ZCOH dissolution. The coin battery exhibits high-rate performance of 65.1% capacity retention at a current density of 15 A g(-1) (compared to 0.6 A g(-1)) and a long cycling life of 20,000 cycles with a capacity retention of 80.7%. For a 22.4 mA h soft-packaged battery, its capacity remains at 72.1% after 2000 cycles. This work demonstrates the active role of ZCOH in the electrochemical process of VO2 and provides a new perspective for exploiting this mechanism to develop high-performance aqueous zinc-ion battery vanadium oxide cathode materials.
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    aqueous zinc-ion batteries,MXene Ti3C2,double hydroxide Zn-12(CF3SO3)(9)(OH)(15)<middle dot>nH(2)O,pH buffer,high-performance VO2 cathode
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    Chat Paper
    【要点】：本研究通过可逆沉积/溶解双氢氧化物来调节电解液pH值，实现了高性能水性锌离子电池，创新性地利用了双氢氧化物ZCOH在VO2表面的pH缓冲作用，提高了电池的循环稳定性。
    

    【方法】：采用水热合成法合成VO2@MXene Ti3C2 (MV)复合材料，并研究了其在水性锌离子电池中的电化学行为。
    

    【实验】：通过原位X射线衍射和pH测量，发现在MV//3 M Zn(CF3SO3)2//Zn电池系统中，ZCOH在充电过程中均匀覆盖在VO2表面，在放电过程中可逆溶解。实验结果表明，该电池系统在15 A g(-1)的电流密度下，容量保持率为65.1%，并且具有20,000次循环的长寿命，容量保持率为80.7%。对于22.4 mA h的软包电池，经过2000次循环后，容量保持率为72.1%。