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    • Synergistic Polarization Engineering on BaTiO3 Bulk and Surface for Boosting Redox Kinetics of Polysulfides in Lithium–sulfur Batteries

    Li Ma,Chunxiao Zhang,Youquan Zhang,Shuai Zhang,Baolei Xu,Mingyang Yan,Yuejiao Chen,Libao Chen,Li Wang,Liangjun Zhou,Weifeng Wei

    Acta Materialia（2023）

    Cent South Univ

    Cited 3|Views25
    Abstract
    The notorious shuttle effect of intermediate lithium polysulfides and the sluggish kinetics of sulfur redox reactions restrict the further development of high-energy-density lithium-sulfur (Li-S) batteries. Herein, a strategy of synergistic polarization engineering on ferroelectric barium titanate (BaTiO3) bulk and surface is reported, aiming to collectively improve the adsorption-catalytic ability of ferroelectric BaTiO3 to polysulfides. Differential phase contrast-scanning transmission electron microscopy (DPC-STEM) demonstrates that the introduction of ultrathin heteroepitaxial TiOx surface can give rise to the surface local electric field differing from bulk internal polarization field. Experimental and theoretical results further reveal that synergistic polarization engineering by integrating the enhanced bulk internal polarization field with the surface local electric field can collaboratively realize excellent adsorption-catalytic activity resulting from rapid electrons transfer and optimized active sites. As a result, employing BaTiO3@TiOx modified separator can endow the batteries with favorable rate performance (the discharge specific capacity achieves 710 mAh g- 1 at 4 C) and substantial enhancement on cyclic performance (64.5 % capacity retention at 2 C over 500 cycles). Impressively, even at high sulfur loading of 2.5 mg cm-2, the BaTiO3@TiOx-based cell still stabilizes 78 % capacity retention with at 1 C over 150 cycles, showing the practical potential of BaTiO3@TiOx in optimizing catalytic efficiency.
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    Li-S batteries,HeteroepitaxialTiOx surface,Synergistic polarization Enhanced internal,polarization field Improved redox kinetics
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    【要点】：本研究通过在钛酸钡（BaTiO3）体相和表面进行协同极化工程，提高了铁电BaTiO3对多硫化锂的吸附-催化能力，显著提升了锂-硫电池的氧化还原动力学。
    

    【方法】：该策略通过在BaTiO3表面引入超薄异质外延TiOx层，与体相内部极化场形成表面局部电场差异。
    

    【实验】：使用差分相位对比扫描透射电子显微镜（DPC-STEM）验证了这一策略，通过增强的体相内部极化场与表面局部电场的协同作用，实现了优异的吸附-催化活性，表现为快速的电子转移和优化的活性位点。基于BaTiO3@TiOx修饰的隔膜，锂-硫电池展现出良好的倍率性能（在4C时放电比容量达到710 mAh g^-1）和显著的循环性能（在2C时500次循环后容量保持率为64.5%）。即使在高硫负载2.5 mg cm^-2下，BaTiO3@TiOx基电池在1C下150个循环后仍保持78%的容量，显示出BaTiO3@TiOx优化催化效率的实际潜力。