Rechargeable aqueous zinc-ion batteries are considered as ideal candidates for large-scale energy storage due to their high safety, eco-friendliness, and low cost. However, Zn anode invites dendrite growth and parasitic reactions at anode-electrolyte interface, impeding the practical realization of the battery. In this study, the electrochemical performance of the Zn-metal anode is proposed to improve by using a 3D ZnTe semiconductor substrate. The substrate features high zincophilicity, high electronic conductivity and electron affinity, and a low Zn nucleation energy barrier to promote dendrite-proof Zn deposition along the (002) crystal plane, while it also maintains high chemical stability against parasitic metal corrosion and hydrogen evolution reactions at surface, and a stable skeleton structure against the volume variation of anode. A Zn-metal anode based on the telluride substrate shows a long cycle life of over 3300 h with a small voltage hysteresis of 48 and 320 mV at 1 and 30 mA cm −2 , respectively. A zinc telluride@Zn//MnO 2 full cell can operate for over 500 cycles under practical conditions in terms of lean electrolyte (18 µL mAh −1 ) and limited Zn metal ( negative/positive capacity ratio of 3:1, and a high mass loading of the cathode.

Sustainable organic electrode materials, as promising alternatives to conventional inorganic electrode materials for sodium‐ion batteries (SIBs), are still challenging to realize long‐lifetime and high‐rate batteries because of their poor conductivity, limited electroactivity, and severe dissolution. It is also urgent to deeply reveal their electrochemical mechanism and evolution processes. A porous organic polymer (POP) with a conjugated and hierarchical structure is designed and synthesized here. The unique molecule and structure endow the POP with electron delocalization, high ionic diffusivity, plentiful active sites, exceptional structure stability, and limited solubility in electrolytes. When evaluated as an anode for SIBs, the POP exhibits appealing electrochemical properties regarding reversible capacity, rate behaviors, and long‐duration life. Importantly, using judiciously combined experiments and theoretical computation, including in situ transmission electron microscopy (TEM), and ex situ spectroscopy, we reveal the Na‐storage mechanism and dynamic evolution processes of the POP, including 12‐electron reaction process with Na, low volume expansion (125–106% vs the initial 100%), and stable composition and structure evolution during repeating sodiation/de‐sodiation processes. This quantitative design for ultrafast and highly durable sodium storage in the POP could be of immediate benefit for the rational design of organic electrode materials with ideal electrochemical properties.

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