The practical application of Zn‐metal anodes (ZMAs) is mainly impeded by the limited lifespan and low Coulombic efficiency (CE) resulting from the Zn dendrite growth and side reactions. Herein, a 3D multifunctional host consisting of N‐doped carbon fibers embedded with Cu nanoboxes (denoted as Cu NBs@NCFs) is rationally designed and developed for stable ZMAs. The 3D macroporous configuration and hollow structure can lower the local current density and alleviate the large volume change during the repeated cycling processes. Furthermore, zincophilic Cu and in‐situ‐formed Cu–Zn alloy can act as homogeneous nucleation sites to minimize the Zn nucleation overpotential, further guiding uniform and dense Zn deposition. As a result, this Cu NBs@NCFs host exhibits high CE of Zn plating/stripping for 1000 cycles. The Cu NBs@NCFs–Zn electrode shows low voltage hysteresis and prolonged cycling life (450 h) with dendrite‐free behaviors. As a proof‐of‐concept demonstration, a Zn‐ion full cell is fabricated based on this Cu NBs@NCFs–Zn anode, which demonstrates decent rate capability and improved cycling performance.

Nitrogen‐Doped Carbon Fibers Embedded with Zincophilic Cu Nanoboxes for Stable Zn‐Metal Anodes

Zinc ion batteries (ZIBs) have been gradually developed in recent years due to their abundant resources, low cost, and environmental friendliness. Therefore, ZIBs have received a great deal of attention from researchers, which are considered as the next generation of portable energy storage systems. However, poor overall performance of ZIBs restricts their development, which is attributed to zinc dendrites and a series of side reactions. Constructing 3D zinc anodes has proven to be an effective way to significantly improve their electrochemical performance. In this review, the challenges of zinc anodes in ZIBs, including zinc dendrites, hydrogen evolution and corrosion, as well as passivation, are comprehensively summarized and the energy storage mechanisms of the zinc anodes and 3D zinc anodes are discussed. 3D zinc anodes with different structures including fiberous, porous, ridge‐like structures, plated zinc anodes on different substrates and other 3D zinc anodes, are subsequently discussed in detail. Finally, emerging opportunities and perspectives on the material design of 3D zinc anodes are highlighted and challenges that need to be solved in future practical applications are discussed, hopefully illuminating the way forward for the development of ZIBs.

A Review on 3D Zinc Anodes for Zinc Ion Batteries

Although zinc metal anodes have some intrinsic advantages for aqueous zinc ion batteries, the notorious dendrites hamper its practical applications. Herein, a charge‐enriched strategy through MXene‐based polypyrrole (MXene‐mPPy) layers is explored toward dendrite‐free Zn metal anode. The MXene‐mPPy layers composed of mesoporous PPy on both sides of Ti3C2Tx‐MXene exhibit an exceptional charge enrichment ability (149 F g−1, 5 mV s−1), which is beneficial not onlying terms of accumulating the charge levels, but also to homogenize the dispersions of electric field and ion flux as used as an artificial interface on a Zn anode. Thus, a dendrite‐free Zn anode with an ultralong cycling lifespan up to 2500 h and superior rate capability is achieved, which is further applied as an anode for aqueous zinc ion batteries with a long‐term span over 3000 cycles at 10 A g−1.

Charge‐Enriched Strategy Based on MXene‐Based Polypyrrole Layers Toward Dendrite‐Free Zinc Metal Anodes

Zn-based aqueous batteries (ZABs) have been regarded as promising candidates for safe and large-scale energy storage in the "post-Li" era. However, kinetics and stability problems of Zn capture cannot be concomitantly regulated, especially at high rates and loadings. Herein, a hierarchical confinement strategy is proposed to design zincophilic and spatial traps through a host of porous Co-embedded carbon cages (denoted as CoCC). The zincophilic Co sites act as preferred nucleation sites with low nucleation barriers (within 0.5 mA h cm-2), and the carbon cage can further spatially confine Zn deposition (within 5.0 mA h cm-2). Theoretical simulations and in situ/ex situ structural observations reveal the hierarchical spatial confinement by the elaborated all-in-one network (within 12 mA h cm-2). Consequently, the elaborate strategy enables a dendrite-free behavior with excellent kinetics (low overpotential of ca. 65 mV at a high rate of 20 mA cm-2) and stable cycle life (over 800 cycles), pushing forward the next-generation high-performance ZABs.

Hierarchical Confinement Effect with Zincophilic and Spatial Traps Stabilized Zn-Based Aqueous Battery.

The growing demand for safe and renewable energy storage systems has driven the recent renaissance of Zn‐ion batteries (ZIBs). Nevertheless, the intrinsic drawbacks of inhomogeneous electric distribution and sluggish ion replenishment worsen the Zn dendrite issues that seriously impede their practical application. Herein, for the first time, a functional 3D printed reservoir‐integrated N‐doped carbon host (3DP‐NC) is designed to remodel the electric/ionic fields. The customized 3D printed structure equipped with regular micron‐sized holes induces reduced local current density and homogeneous electric distribution. The micron‐sized holes function as reservoirs to ensure unobstructed ion diffusion and quasi‐steady‐state ionic supplements. A N‐doping interfacial modification strategy is further employed to encourage a highly zincophilic surface, hence reducing the nucleation energy barrier and motivating uniform Zn nucleation. As a result, the Zn‐deposited 3DP‐NC electrode (3DP‐NC@Zn) affords dendrite‐free morphology and highly reversible Zn plating/stripping with an ultra‐small overpotential of 15.3 mV even at 10 mA cm−2. Additionally, these appealing features also endow the 3DP‐NC@Zn electrode with an outstanding lifespan over 380 h at 1 mA cm−2 and 1 mAh cm−2. The thrilling performance establishes a new roadmap that advances the development of dendrite‐free and durable metal batteries by exploiting this unique 3D printing technique.

3D Printing Architecting Reservoir‐Integrated Anode for Dendrite‐Free, Safe, and Durable Zn Batteries

Synergistic Manipulation of Zn2+ Ion Flux and Nucleation Induction Effect Enabled by 3D Hollow SiO2/TiO2/Carbon Fiber for Long-Lifespan and Dendrite-Free Zn–Metal Composite Anodes

The construction of a heterointerface by structure-induced partial phase transformation is an effective strategy to synchronously boost conductivity and regulate the ion diffusion kinetics of TiO2 considered as an anode material for sodium ion batteries. However, construction of a highly conductive heterostructure in well-crystallized TiO2 is still a great challenge. Herein, a structure-induced partial phase transformation method is reported to synthesize hierarchical hollow TiO2/TiN heterostructure fibers (HTTFs) with a high specific surface area for use as an anode. The interfacial effect of the heterostructures for the anode materials could improve charge transfer capability. The improvement of the conductivity is due to the electric field generated inside the nanocrystals, which greatly reduces the ion diffusion resistance of nanocrystals and promotes the interfacial electron transport. Density functional theory calculations and experimental results demonstrate that HTTFs greatly facilitated the mobility of holes and ion diffusion, which result in excellent rate capability (270.9 and 113.1 mA h g−1 at 50 and 10 000 mA g−1, respectively) and excellent cycling stability (132.5 mA h g−1 with an average capacity fading of only 0.002% per cycle at 5000 mA g−1 over 10 000 cycles). Such improvements signify that suitable heterogeneous interface design provides an innovative and versatile approach for achieving advanced battery materials.

Structure-induced partial phase transformation endows hollow TiO2/TiN heterostructure fibers stacked with nanosheet arrays with extraordinary sodium storage performance

Thermo-managing and flame-retardant scaffolds suppressing dendritic growth and polysulfide shuttling toward high-safety lithium–sulfur batteries

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Synergistic Manipulation of Zn2+ Ion Flux and Nucleation Induction Effect Enabled by 3D Hollow SiO2/TiO2/Carbon Fiber for Long-Lifespan and Dendrite-Free Zn–Metal Composite Anodes

Structure-induced partial phase transformation endows hollow TiO2/TiN heterostructure fibers stacked with nanosheet arrays with extraordinary sodium storage performance

Thermo-managing and flame-retardant scaffolds suppressing dendritic growth and polysulfide shuttling toward high-safety lithium–sulfur batteries