Multivalent Amide-Hydrogen-Bond Supramolecular Binder Enhances the Cyclic Stability of Silicon-Based Anodes for Lithium-Ion Batteries
Multivalent Amide-Hydrogen-Bond Supramolecular Binder Enhances the Cyclic Stability of Silicon-Based Anodes for Lithium-Ion Batteries
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多价酰胺氢键超分子粘合剂增强锂离子电池硅基负极的循环稳定性
DOI：
10.1021/acsami.1c04501
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发表时间：
2021
影响因子：
9.5
通讯作者：
Sun Shi-Gang
中科院分区：
文献类型：
--
作者：
Deng Li;Deng Sai-Sai;Pan Si-Yu;Wu Zhan-Yu;Hu Yi-Yang;Li Kai;Zhou Yao;Li Jun-Tao;Huang Ling;Sun Shi-Gang
合成了一种超分子聚合物聚N-丙烯酰甘氨酰胺（PNAGA），其分子链两侧均含有双酰胺基团，形成多个酰胺-氢键，可用作硅基阳极的粘合剂。该超分子聚合物粘合剂具有改善的机械性能，与形成氢键的Si颗粒呈现出良好的界面粘合性，并且提高了电极材料膜和铜集电体之间的粘合强度。得益于PNAGA粘合剂的高度稳定的分子间和分子内多酰胺-氢键，电极结构保持完整性，并且在Si颗粒表面上形成稳定的固体电解质中间相（SEI）层。通过X光电子能谱（XPS）表征，研究了不同粘合剂对SEI膜组成的影响。与具有与PNAGA类似结构的聚丙烯酰胺（PAM）和传统的海藻酸钠（SA）粘合剂相比，含有PNAGA粘合剂的Si电极显示出改善的电化学性能。在420 mA g-1下循环100次后容量保持率为84%，在1260 mA g-1下循环400次后容量保持率为1942.6 mAh g-1。即使在1.2 mg cm-2 Si的质量负载下，具有PNAGA粘合剂的电极也表现出高的初始面积容量（2.64 mAh cm-2）和良好的循环性能（50次循环后81%的容量保持率）。此外，PNAGA粘合剂的应用还为商业Si-石墨（SiC）负极材料带来了稳定的循环性能。
A supramolecular polymer, poly(N-acryloyl glycinamide) (PNAGA), with a bisamide group on each side of the chain forming multiple amide-hydrogen bonds was synthesized in this work as a binder for silicon (Si)-based anodes. This supramolecular polymer binder with improved mechanical properties presents good interfacial adhesion with Si particles forming hydrogen bonds and enhances the adhesive strength between the electrode material film and the copper current collector. Benefiting from the highly stable inter- and intramolecular multiple amide-hydrogen bonds of the PNAGA binder, the electrode structure maintains integrity and a stable solid electrolyte interphase (SEI) layer is formed on the surface of Si particles. The effect of different binders on the composition of the SEI film was also investigated by X-photoelectron spectroscopy (XPS) characterization. In comparison with polyacrylamide (PAM), which has a similar structure to PNAGA, and the traditional sodium alginate (SA) binder, the Si electrode containing the PNAGA binder shows improved electrochemical performance. The capacity retention is 84% after 100 cycles at 420 mA g–1, and the capacity remains at 1942.6 mAh g–1after 400 cycles at 1260 mA g–1. Even with a mass loading of 1.2 mg cm–2Si, the electrode with the PNAGA binder exhibits high initial areal capacity (2.64 mAh cm–2) and good cycling performance (81% capacity retention after 50 cycles). Moreover, the application of the PNAGA binder also brings a stable cycle performance to the commercial Si-graphite (SiC) anode material.