Data_Sheet_1_Impact of Polypyrrole Functionalization on the Anodic Performance of Boron Nitride Nanosheets: Insights From First-Principles Calculations.pdf

Lithium-ion batteries (LIBs) have displayed superior performance compared to other types of rechargeable batteries. However, the depleting lithium mineral reserve might be the most discouraging setback for the LIBs technological advancements. Alternative materials are thus desirable to salvage these limitations. Herein, we have investigated using first-principles DFT simulations the role of polypyrrole, PP functionalization in improving the anodic performance of boron nitride nanosheet, BNNS-based lithium-ion batteries and extended the same to sodium, beryllium, and magnesium ion batteries. The HOMO-LUMO energy states were stabilized by the PP functional unit, resulting in a significantly reduced energy gap of the BNNS by 45%, improved electronic properties, and cell reaction kinetics. The cell voltage, ΔEcell was predicted to improve upon functionalization with PP, especially for Li-ion (from 1.55 to 2.06 V) and Na-ion (from 1.03 to 1.37 V), the trend of which revealed the influence of the size and the charge on the metal ions in promoting the energy efficiency of the batteries. The present study provides an insight into the role of conducting polymers in improving the energy efficiency of metal-ion batteries and could pave the way for the effective design of highly efficient energy storage materials.

锂离子电池（LIBs）相较于其他类型的可充电电池展现出更优异的性能。然而，锂矿储量日渐枯竭或许是阻碍LIBs技术发展的最令人沮丧的瓶颈。因此，亟需开发替代材料以弥补上述局限。本文中，我们借助第一性原理DFT模拟，探究了聚吡咯（polypyrrole, PP）功能化对氮化硼纳米片（BNNS）基锂离子电池阳极性能的提升作用，并将该研究拓展至钠离子、铍离子与镁离子电池体系。聚吡咯功能单元可稳定HOMO-LUMO能级，使氮化硼纳米片的能隙显著降低45%，同时优化了电子特性与电池反应动力学。经聚吡咯功能化后，预测的电池电压ΔE_cell得到提升：锂离子电池从1.55 V升至2.06 V，钠离子电池从1.03 V升至1.37 V；该变化趋势揭示了金属离子的尺寸与电荷对提升电池能源效率的调控作用。本研究阐明了导电聚合物在提升金属离子电池能源效率中的作用，可为高效储能材料的精准设计提供理论指导与研发新思路。