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.

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Figure 5. a) CV curves conducted at 0.1 mV s −1 and b) EIS spectra of VO 2 //Zn full cells with 3DP-BU@Zn, 3DP-HG@Zn, and 3DP-UB@Zn as anodes. c) Rate performances collected at 0.1-4.0 A g −1 of the VO 2 //Zn full cells with 3DP-BU@Zn, 3DP-HG@Zn, and 3DP-UB@Zn as anodes, respectively. d) The capacity retention of the VO 2 //3DP-BU@Zn full cell under a current density of 1 A g −1 . e,f) Photos of serial VO 2 //3DP-BU@Zn full cells powering a water pump (e) and a table lamp (f).

for use in SIBs due to its small interlayer spacings and inability to generate stable Na-C intercalation compounds. [3] Fortunately, disordered carbonaceous materials with randomly oriented graphitic layers and tunable microstructures have shown great commercialization prospects for SIBs. [4a,b] The electrochemical properties of disordered carbonaceous materials are highly dependent on their microstructures. Based on the degree of graphitization difficulty at high temperature (usually over 2500 °C), disordered carbonaceous materials can be sorted into soft carbon and hard carbon, of which the former displays long-range and highly ordered graphitic layers, while the latter shows a disordered structure with turbostratic domains. [5] In contrast to the low reversible capacity and negligible plateau of soft carbon, hard carbon materials generally exhibit high reversible capacities as well as long and flat plateaus below 0.1 V owing to their large interlayer spacings and disordered pore-rich textures, making them promising for high energy-density SIBs. Hard carbon materials are generally derived from pyrolysis of thermosetting resins, [6a-c] organic macromolecules, [7a-c] biomass, [8a-c] etc., at high temperatures (usually above 1300 °C). The high costs and low yields of these carbon precursors, as well as the complicated and costly production processes, significantly impede practical application. In addition, hard carbon derived from direct pyrolysis of these precursors generally delivers unsatisfactory rate capability, low initial Coulombic efficiency, and poor cycling stability because of the unsuitable sodium ion storage microstructure. [9a,b] Therefore, low-cost and high-yield carbon precursors for hard carbon exhibiting excellent electrochemical performance are highly anticipated.Pitch is a low-cost and abundant byproduct of the petroleum industry, and it is mainly composed of polycyclic aromatic hydrocarbons, which ensures high carbon yield after pyrolysis. [10a,b] Normally, the direct pyrolysis of pitch undergoes an uncontrollable fusion-state carbonization process because of the presence of excess hydrogen and strong π-π interactions between aromatic molecules, resulting in highly graphitized soft carbon with small interlayer spacing. [11] This microstructure ultimately leads to unsatisfactory sodium-ion storage performance, i.e., low reversible capacity and negligible plateau. It has been found that increasing crosslinking of Direct pyrolysis of low-cost and resource-abundant pitch generally produces highly graphitized soft carbon, showing low reversible capacity and a negligible charge-discharge plateau owing to its unsuitable microstructure for sodium storage. Herein, for the first time, an innovative dual-interfering chemistry strategy is proposed to solve the soft-hard carbon translation challenge. Multifunctional zinc gluconate generates dual-mechanism interference upon decomposition and successfully regulates pitch pyrolysis: 1) the gas decomposition products (carbon oxides) may consume excess ...

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