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[Display omitted] Binders play a key role in maintaining the integrity of high-capacity silicon anodes, which otherwise experience serious capacity decay during cycling caused by huge volume variation of the silicon. With an aim to developing a highly efficient polymeric binder to mitigate this capacity decay, we present a novel binder synthesized from polyacrylic acid (PAA) and polymerized β-cyclodextrin (β-CDp) for Si anodes for the lithium-ion batteries. This PAA-β-CDp binder has a 3D network structure, which provides strong adhesion between the active material and the current collector. PAA-β-CDp binder makes silicon anode achieve a specific capacity of 2326.4 mAhg−1 at the current density of 0.2 A g−1 with a capacity retention of 64.6% after 100 cycles. The experimental results show that the PAA-β-CDp binder can effectively mitigate the huge volume change and improve the capacity and cycling performance of Si anodes. [ABSTRACT FROM AUTHOR]

• The crystalline silicon nanoparticles coated with an amorphous silicon layer (a-coated-c-SiNPs) were continuously prepared by non-thermal plasma pyrolyzing of silane with the help of hydrogen and argon. • The a-Si layer with good tolerance to volume expansion prevented the electrode pulverization, while the c-Si improved the electronic conductivity. The crystallinity of the a-coated-c-SiNPs was controled by the hydrogen etching. • The combination of a-coated-c-SiNPs with a three-component polymer binder (PAA-PVA/SBR) improved the electrochemical performance of Si-based anode. The crystalline silicon nanoparticles coated with an amorphous silicon layer was prepared by continuously pyrolysing the mixture of silane and hydrogen in a non-thermal arc plasma reactor. The hydrogen in the gas mixture effectively controls the thickness of the amorphous silicon layer and further improves the electrochemical performance of the silicon anode. The mechanism of the hydrogen was investigated by experiments. At the same time, a three-component polymer binder was concocted and introduced to tolerate the volume expansion of silicon effectively. Combining the silicon nanoparticles prepared at the optimal conditions with the novel polymer binder, the resulting silicon anode exhibits excellent electrochemical performance of 2120 mAh g−1 at 400 mA g−1 after 100 cycles. [Display omitted] [ABSTRACT FROM AUTHOR]