Regulating Grafting Density to Realize High‐Areal‐Capacity Silicon Submicroparticle Anodes Under Ultralow Binder Content

Abstract Grafted biopolymer binders are demonstrated to improve the processability and cycling stability of the silicon (Si) nanoparticle anodes. However, there is little systematical exploration regarding the relationship between grafting density and performance of grafted binder for Si anodes, especially when Si particles exceed the critical breaking size. Herein, a series of guar gum grafted polyacrylamide (GP) binders with different grafting densities are designed and prepared to determine the optimal grafting density for maximizing the electrochemical performance of Si submicroparticle (SiSMP) anodes. Among various GP binders, GP5 with recommended grafting density demonstrates the strongest adhesion strength, best mechanical properties, and highest intrinsic ionic conductivity. These characteristics enable the SiSMP electrodes to sustain the electrode integrity and accelerate lithium‐ion transport kinetics during cycling, resulting in high capacity and stable cyclability. The superior role of GP5 binder in enabling robust structure and stable interface of SiSMP electrodes is revealed through the PeakForce atomic force microscopy and in situ differential electrochemical mass spectrometry. Furthermore, the stable cyclabilities of high‐loading SiSMP@GP5 electrode with ultralow GP5 content (1 wt%) at high areal capacity as well as the good cyclability of Ah‐level LiNi 0.8 Co 0.1 Mn 0.1 O 2 /SiSMP@GP5 pouch cell strongly confirms the practical viability of the GP5 binder.