Conjugated Imine Polymer Synthesized via Step-Growth Metathesis for Highly Stable Silicon Nanoparticle Anodes in Lithium-Ion Batteries,Advanced Energy Materials

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Conjugated Imine Polymer Synthesized via Step-Growth Metathesis for Highly Stable Silicon Nanoparticle Anodes in Lithium-Ion Batteries
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-02-17 , DOI: 10.1002/aenm.202203921
Trevor R. Martin ₁ , Leah Rynearson ₂ , Mackenzie Kuller ₁ , Joseph Quinn ₃ , Chongmin Wang ₃ , Brett Lucht ₂ , Nathan R. Neale ₁

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This work reports a new method to synthesize polyphenylmethanimine (polyPMI) as a linear or a hyperbranched, conjugated polymer using an aldehyde-imine metathesis reaction. This work details the reaction mechanisms of this polymerization by characterizing a red-shift in its absorption spectrum as polymer conjugation length increases and verifies that this optical shift results from extended π-condensation using density functional theory. This new synthetic approach provides a polymer that can potentially be depolymerized for facile recyclability and is compatible with air- and water-sensitive chemistries. As an example of the utility of this new approach, this work demonstrates that this polymer can be directly grown on silicon nanoparticles to create silicon anodes for lithium-ion batteries with a high degree of electrochemical interfacial passivation. These silicon anodes exhibit Coulombic efficiencies above 99.9% and can accommodate silicon nanoparticle expansion and contraction during lithiation and delithiation as demonstrated by stable reversible capacities for 500 cycles. Finally, this work demonstrates that polyPMI facilitates the formation of a lithium fluoride rich solid electrolyte interphase that remains chemically and mechanically stable after long term cycling.

中文翻译：

通过逐步生长复分解合成的共轭亚胺聚合物用于锂离子电池中的高稳定性硅纳米颗粒阳极

这项工作报告了一种使用醛-亚胺复分解反应将聚苯甲胺 (polyPMI) 合成为线性或超支化共轭聚合物的新方法。这项工作详细描述了这种聚合反应的反应机制，其特征是随着聚合物共轭长度的增加，其吸收光谱发生红移，并使用密度泛函理论验证了这种光学偏移是由扩展的 π 缩合引起的。这种新的合成方法提供了一种聚合物，这种聚合物可以被解聚以便于回收利用，并且与对空气和水敏感的化学物质兼容。作为这种新方法实用性的一个例子，这项工作表明，这种聚合物可以直接在硅纳米粒子上生长，从而为具有高度电化学界面钝化的锂离子电池制造硅阳极。这些硅阳极表现出超过 99.9% 的库仑效率，并且可以在锂化和脱锂过程中适应硅纳米颗粒的膨胀和收缩，如 500 次循环的稳定可逆容量所证明的那样。最后，这项工作表明，polyPMI 有助于形成富含氟化锂的固体电解质界面，该界面在长期循环后仍保持化学和机械稳定性。9%，并且可以适应硅纳米颗粒在锂化和脱锂过程中的膨胀和收缩，正如 500 次循环的稳定可逆容量所证明的那样。最后，这项工作表明，polyPMI 有助于形成富含氟化锂的固体电解质界面，该界面在长期循环后仍保持化学和机械稳定性。9%，并且可以适应硅纳米颗粒在锂化和脱锂过程中的膨胀和收缩，如 500 次循环的稳定可逆容量所证明的那样。最后，这项工作表明，polyPMI 有助于形成富含氟化锂的固体电解质界面，该界面在长期循环后仍保持化学和机械稳定性。

更新日期：2023-02-17

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