Investigation into lithium plating/stripping behavior employed symmetric cells with ether electrolyte composed of a 1:1 volume ratio of 1,3-dioxolane (DOL) and 1,2-dimethoxyethane (DME) solvents with 1 M lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and 1% LiNO3. A total of 40 μL of electrolyte was added to each cell. The cathode material was prepared by blending LiNi0.5Mn1.5O4 (LNMO, Xiamen TOB new energy), Super P conductive carbon, and Poly(vinylidene fluoride) (PVDF) mixed in a mass ratio of 8:1:1 in Nmethyl-2-pyrrolidone (NMP). A cathode sheet was fabricated by tape casting the slurry onto a corroded aluminum foil, resulting in an LNMO loading weight of approximately 7.8 mg per centimeter square, an areal capacity of 1.0 mAh per centimeter square, and an N/P ratio of 73. Full cells utilizing an LNMO cathode (Φ15 mm) with an ester electrolyte consisting of 1:1 volume ratio of ethylene carbonate (EC)/dimethylcarbonate (DMC) solvent with 1 M lithium hexafluorophosphate (LiPF6), The electrolyte amount and separator are same with symmetric cell. Galvanostatic charge-discharge experiments for thesee cells involved charging from 3.5 V to 4.95 V. Figure illustrates the role of plasma in the synthesis of uniform and tight adhered ZIF-8 layer on the carbon fiber. In Figure , without plasma activation, the Zn(NO3)2 and 2-MeIm fails to fully infiltrate the carbon fiber, resulting in incomplete coverage and agglomeration of ZIF-8 particles (Figure ). However, upon activation by oxygen plasma, surface contaminants are removed, and oxygen functional groups are uniformly distributed on the carbon fiber surface, enhancing zincophilicity. As a result, Zn(NO3)2 and 2-MeIm can fully infiltrate the carbon fiber (Figure ), enabling tight and homogeneous growth of ZIF-8 particles on the carbon fiber surface (Figure ). Figure and 3b depict SEM images of p-ZNCC. Following sintering in N2 atmosphere, the ZIF-8 particles on the carbon fiber transform into a composite of carbon nanoweb and particles. TEM (Figure ) and selected surface area diffraction (SAED) (Figure ) confirm the presence of nanocrystals with a lattice spacing of 2.81 Å, corresponding to the (100) plane of lithiophilic ZnO. Additionally, Figure shows the energy-dispersive X-ray spectroscopy (EDS) mapping of p-ZNCC, revealing the presence of nitrogen (N), oxygen (O), zine (Zn), and carbon (C) species. The high-angle annular dark-field (HAADF) image and element distribution suggest a hollow structure of p-ZNCC. The hollow structure is advantageous fo increasing surface area and reducing current density during charging/discharging, promoting uniform lithium plating/stripping. In Figure , the XRD spectra exhibit sharp peaks that align closely with the simulated pattern of ZIF-8, confirming the successful synthesis of ZIF-8 on carbon fiber. The board peak observed between 20 and 30 degrees can be attributed to the presence of amorphous carbon from the carbon cloth. Following sintering, the peaks associated with ZIF-8 vanish in the spectrum of p-ZNCC, replaced by a broad peak between 20 and 30 degrees, indicating complete carbonization ZIF-8. In Figure , the N 1s XPS spectra reveal significantly stronger peak for p-ZNCC and ZNCC compared to p-CC and CC, indicating the introduction of additional nitrogen by ZIF-8 to the carbon fiber. Furthermore, the spectra can be deconvoluted into three nitrogen species: Graphitic N (401.1 eV), pyrrolic N (399.6 eV), and pyridinic N (399.0 eV). The pyrrolic N content in p-ZNCC is higher than ZNCC, likely due to the tighter and more uniform growth of ZIF-8 carbon fiber facilitated by plasma treatment, resulting in increased pyrrolic N generation after sintering. Figure displays the O 1s XPS spectra, showing a significant increase in oxygen content of p-CC compared to CC after oxygen plasma treatment. The peak can be resolved into two components: O-C=O (533.3 eV) and C=O (531.6 eV). After sintering, the oxygen bonds transform into C-O (532.6 eV) and Zn-O (531.0 eV). Notably, the oxygen content of p-ZNCC is much higher than ZNCC due to the introduction of oxygen by the plasma and the presence of oxygen in ZIF-8. Since ZIF-8 is more prevalent on p-CC, more oxygen remains on p-CC after sintering. Figure illustrates the Zn 2p3/2 spectra, where p-ZNCC exhibits a peak at 1022.4 eV, corresponding to ZnO. In contrast, the peak for ZNCC is situated at 1021.7 eV, indicating the existence of Zn. This difference may be attributed to the active oxygen introduced by plasma, which readily reacts with Zn, aided by the hollow carbon web of p-ZNCC. The lithiophilic property of ZnO is advantageous for the lithium-ion desolvation and stable plating /stripping process. In Figure , the synchrotron O K-edge X-ray absorption near-edge structure (XANES) displays two peaks for p-ZIF-CC and ZIF-CC at 541.2 eV and 534 eV, potentially corresponding to O-C=O and C=O bonds. Moreover, the peak intensity of p-ZIF-CC exceeds that of ZIF-CC, indicating higher oxygen content in p-ZIF-CC. After sintering, the two peaks merge into a single peak at 539.4 eV. The peak for p-ZNCC is notably larger than that for ZNCC, likely due to the higher oxygen content in p-ZNCC, consistent with the O 1s XPS spectra in Figure . Figure illustrates the synchrotron N K-edge XANES, revealing two distinct peaks at 407.2 eV and 401.8 eV for p-ZNCC, ZNCC, p-ZIF-CC, and ZIF-CC. These peaks likely correspond to the same type of nitrogen present. The nitrogen content of p-ZIF-CC surpasses that of ZIF-CC, indicating increased ZIF-8 growth on p-CC after plasma treatment. Although the peak intensity of p-ZNCC and ZNCC appears similar, convolution of N 1s XPS spectra suggests that p-ZNCC contains significantly more pyrrolic nitrogen than ZNCC, which is the most lithiophilic nitrogen species. Figure depicts the schematic diagram illustrating the interaction between nitrogen species and solvated lithium ions ). The binding energies of pyrrolic N, pyridinic N, and graphitic N are determined to be -4.46 eV, -4.26 eV, and -3.29 eV, respectively. Due to the higher electronegativity of oxygen (3.44) and nitrogen (3.07) atoms compared to lithium (0.98), the interactions between these atoms and lithium ions closely resemble donor-acceptor relationships and can be elucidated by the theory of Lewis acid-base. The electronic configurations of nitrogen play a crucial role in these interactions: pyrrolic nitrogen possesses a lone pair in the p orbital, while pyridinic nitrogen has a lone pair occupying the sp 2 orbital. Both pyrrolic and pyridinic N, with their extra pair of electrons, exhibit high chemical reactivity as electron-rich donors, facilitating the de-solvation process of lithium ions. Conversely, graphitic nitrogen is unreactive with lithium ions due to its provision of two single electrons in two orbitals. Lithium symmetric cell analysis. In Figure , the p-ZNCC-Li demonstrates a voltage hysteresis of merely 40 mV after 2000 h charge-discharge cycling at a current density of 1 mA cm -2 and an energy density of 1 mAh cm -2 . Figure provides an enlarged view of the charge-discharge profiles of the Li symmetric cells. The pronounced sharp peaks observed are associated with the surface oxidized impurities, the formation of the solid electrolyte interface (SEI), and dead lithium caused high surface resistance. The peaks of CC-Li nearly vanish after the first 5 cycles, likely due to the exposure of fresh Li beneath surface oxidation impurities and the stabilization of the SEI during cycling. The abrupt increase in the peaks of ZNCC-Li after 500 cycles could be attributed to the formation of dead lithium leading to additional surface resistance. In contrast, p-ZNCC-Li exhibits smaller initial peaks, which curves eventually becoming peak-free during prolonged cycling, indicating high reversibility, low resistance, and a clean surface state. In Figure , at an elevated current density of 5 mA cm -2 -5 mAh cm -2 , the voltage hysteresis of p-ZNCC-Li remains remarkably low at only 17 mV after 2500 h. In Figure , further increasing the current density to 10 mA cm -2 -10 mAh cm -2 , the voltage hysteresis of p-ZNCC-Li after 3000 h remains low at 36 mV. The initial fluctuation in voltage hysteresis may be attributed to the formation of SEI. Figure and show the morphologies of the lithium anode were examined after 500 cycles at 5 mA cm -2 -1 mAh cm -2 . In Figure , corresponding schematic figures are created to elucidate the distinct Li dendrite morphologies on different substrates. Notably, on the bare Li anode, evident dead Li is observed after cycling, with a thickness of 105 μm (Figure ). The Li dendrite appear as thick particles with a diameter of approximately 5 μm, and the spacing between them is considerable and deep (Figure and). When employing a carbon cloth (CC) skeleton, the surface becomes somewhat smoother, and the Li dendrites consist of smaller particles, resulting in a dead Li thickness of 162 μm (Figure ). Conversely, the surface of ZNCC-Li appears relatively smoother, with smaller Li dendrites, although clear spaces between them persist. Here, the dead Li thickness decreases to 57 μm (Figure ).