Molecular deciphering of hydrophobic, Zinc-philic and robust Amino-functionalized Polysilane for Dendrite-free Zn Anode

•A hydrophobic and amorphous layer of polysilane on Zn is prepared in a new way.•NH2 in the layer regulates the Zn2+ flux and facilitates uniform deposition.•Propyl in the layer increases surface hydrophobicity and inhibits side reactions.•Si-O-M endow the layer and the interface robust mechanical properties.•NH2-functionalized polysilane coated Zn exhibits outstanding performances.