Integrating with a tough framework and efficient self-healing behavior based on a flexible polymer skeleton for Si anode binders in lithium-ion cells

As a prospective and efficient strategy to address the volume expansion of the Si nanoparticles, the binder plays an increasingly significant role in the Si anode of lithium-ion batteries. Based on the inspiration of natural physics and cross-linked networks, a functional (named polyacrylic acid-citric acid-polyethyleneimine) binder that is similar to a flexible polymer skeleton integrated with a tough framework and efficient self-healing behavior is designed to achieve long cycling stability for Si anodes. The cross-linked network can be stabilized by the amide bonds, formed by polyethyleneimine (PEI) and polyacrylic acid (PAA). Based on this, citric acid (CA) can be added to form multiple hydrogen bonds, whose carboxyl groups can also establish a more reversible cross-linked network with Si particles. Then, PEI and CA molecules can connect with PAA to form a "rigid and flexible" structure. The expansion stress of Si nanoparticles is relieved by the protective buffer layer built by the addition of PEI and CA molecules. In addition, PAA, PEI, and CA work together to solve the problem that the action of CA and PAA alone cannot perform well under large currents. Hence, this water-based binder with a three-dimensional cross-linked network structure with self-healing ability has better performance during cycling: at a current density of 0.2C, it still has a capacity of 2017.4 mAh·g−1 after 200 cycles, with a capacity retention rate of 80.7 % (1745.3 mAh·g−1, 300 cycles, a capacity retention of 74.9 %).