Sequence‐Defined Peptoids with —OH and —COOH Groups As Binders to Reduce Cracks of Si Nanoparticles of Lithium‐Ion Batteries

Silicone (Si) is one type of anode materials with intriguingly high theoretical capacity. However, the severe volume change associated with the repeated lithiation and delithiation processes hampers the mechanical/electrical integrity of Si anodes and hence reduces the battery's cycle‐life. To address this issue, sequence‐defined peptoids are designed and fabricated with two tailored functional groups, “—OH” and “—COOH”, as cross‐linkable polymeric binders for Si anodes of LIBs. Experimental results show that both the capacity and stability of such peptoids‐bound Si anodes can be significantly improved due to the decreased cracks of Si nanoparticles. Particularly, the 15‐mer peptoid binder in Si anode can result in a much higher reversible capacity (ca. 3110 mAh g(−1)) after 500 cycles at 1.0 A g(−1) compared to other reported binders in literature. According to the density functional theory (DFT) calculations, it is the functional groups presented on the side chains of peptoids that facilitate the formation of Si−O binding efficiency and robustness, and then maintain the integrity of the Si anode. The sequence‐designed polymers can act as a new platform for understanding the interactions between binders and Si anode materials, and promote the realization of high‐performance batteries.