Surface Patterning of Metal Zinc Electrode with an In-Region Zincophilic Interface for High-Rate and Long-Cycle-Life Zinc Metal Anode

doi:10.1007/s40820-024-01327-2

Abstract

Abstract:

The undesirable dendrite growth induced by non-planar zinc (Zn) deposition and low Coulombic efficiency resulting from severe side reactions have been long-standing challenges for metallic Zn anodes and substantially impede the practical application of rechargeable aqueous Zn metal batteries (ZMBs). Herein, we present a strategy for achieving a high-rate and long-cycle-life Zn metal anode by patterning Zn foil surfaces and endowing a Zn-Indium (Zn-In) interface in the microchannels. The accumulation of electrons in the microchannel and the zincophilicity of the Zn-In interface promote preferential heteroepitaxial Zn deposition in the microchannel region and enhance the tolerance of the electrode at high current densities. Meanwhile, electron aggregation accelerates the dissolution of non-(002) plane Zn atoms on the array surface, thereby directing the subsequent homoepitaxial Zn deposition on the array surface. Consequently, the planar dendrite-free Zn deposition and long-term cycling stability are achieved (5,050 h at 10.0 mA cm⁻² and 27,000 cycles at 20.0 mA cm⁻²). Furthermore, a Zn/I₂ full cell assembled by pairing with such an anode can maintain good stability for 3,500 cycles at 5.0 C, demonstrating the application potential of the as-prepared ZnIn anode for high-performance aqueous ZMBs.

Key words: Zn metal anode, Surface patterning, Directional Zn deposition, Aqueous Zn-I₂ batteries

Tian Wang, Qiao Xi, Kai Yao, Yuhang Liu, Hao Fu, Venkata Siva Kavarthapu, Jun Kyu Lee, Shaocong Tang, Dina Fattakhova-Rohlfing, Wei Ai, Jae Su Yu. Surface Patterning of Metal Zinc Electrode with an In-Region Zincophilic Interface for High-Rate and Long-Cycle-Life Zinc Metal Anode[J]. Nano-Micro Letters, 2024, 16(1): 112-.

Tian Wang, Qiao Xi, Kai Yao, Yuhang Liu, Hao Fu, Venkata Siva Kavarthapu, Jun Kyu Lee, Shaocong Tang, Dina Fattakhova-Rohlfing, Wei Ai, Jae Su Yu. [J]. Nano-Micro Letters, 2024, 16(1): 112-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-024-01327-2

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/112

Figures/Tables 6

Fig. 1 Fabrication and characterization of the ZnIn electrode. a Schematic illustration of Zn deposition morphology evolution on the pristine Zn anode and b preparation of the patterned ZnIn anode and the Zn plating behavior. SEM images of the c patterned Zn electrode and d ZnIn electrode (the inset figures show the corresponding optical microscopic images). e, f EDS elemental mapping images of the ZnIn electrode. g Thickness measurement of the prepared ZnIn electrode. h XRD patterns of the pristine Zn and ZnIn electrodes

Fig. 2 Dynamic evolution of the ZnIn electrode morphology during Zn plating and analysis of the underlying mechanism. a SEM images of the ZnIn electrode after Zn deposition of (i) 0 mAh cm⁻², (ii) 3.0 mAh cm⁻², (iii) 5.0 mAh cm⁻², and (iv) 10.0 mAh cm⁻². b In situ optical observations of Zn plating behavior of pristine Zn and ZnIn electrodes. Scale bars are 100 μm. Cross-sectional SEM images for the Zn deposition with different areal capacities of c 5.0 mAh cm⁻², d 10.0 mAh cm⁻², and e 15.0 mAh cm⁻² (Scale bars are 200 μm) and f magnified image of e. g SEM image of the planar deposited Zn flakes. Simulation of the evolution process of h current density distribution and i Zn-ion concentration distribution on the ZnIn electrode surface at different times. j Schematic illustration of the morphology evolution of the ZnIn electrode during Zn deposition

Fig. 3 Side reaction resistance of the ZnIn electrode. a Binding energy barrier for Zn atom on In (002), In (110), Zn (002), and Zn (100) planes (the insets show the corresponding charge density difference, respectively) and b corresponding sliced 2D contour map of the Zn atom bonded with In (110) and Zn (100) planes. c Chronoamperometry curves, d linear polarization curves, and e hydrogen evolution polarization curves of the pristine Zn and ZnIn electrodes. f XRD patterns of the ZnIn electrodes with different area capacities. g Band contrast image and h corresponding EBSD mapping image of the ZnIn electrode after cycling 100 h. i Absorption energy of H₂O molecule on various Zn crystal planes (the insets show the corresponding charge density difference, respectively)

Fig. 4 Zn deposition mechanism of the ZnIn electrode. a Free energy diagram for the HER. DEMS plots of H₂ evolution rate of the b pristine Zn and c ZnIn symmetrical cells during the continuous plating, respectively. d XRD patterns and e surface roughness of the different electrodes before and after cycling test. The current density is 2.0 mA cm⁻². f Stripping energy of Zn atom from different crystal planes and g surface energy of the different Zn planes. h Schematic depiction of Zn deposition behavior on the ZnIn electrode

Fig. 5 Electrochemical performance characterizations of Zn metal deposition on the difference electrodes. Galvanostatic cycling of symmetrical ZnIn and pristine Zn cells with the plating-stripping conditions of a10.0 mA cm⁻² and 1.0 mAh cm⁻², b 20.0 mA cm⁻² and 1.0 mAh cm⁻² (the insets show the magnified curves at specific cycles), and c 20.0 mA cm⁻² and 5.0 mAh cm⁻². d Rate performance of the ZnIn and pristine Zn symmetric cells. e Galvanostatic cycling of the ZnIn and pristine Zn symmetric pouch cells at 10.0 mA cm⁻² and 1.0 mAh cm⁻². f Comparative cycling performance of the ZnIn anode with others

Fig. 6 Electrochemical properties of aqueous Zn/I₂ cells. a Charge/discharge profiles of the ZnIn/I₂-CFs full cell and b their corresponding dQ/dV curves. c Cycle performance at 0.5 C. Self-discharge curves of the d ZnIn/I₂-CFs and e Zn/I₂-CFs full cells. f Nyquist plots, g cycle performance at 5.0 C of the full cells, and h, i optical photographic images of the quasi-solid-state ZnIn/I₂-CFs pouch cells powering a LED device

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