Recent Advances in Constructing Oriented Ion Transport Channels with Two-dimensional Layered Materials for Electrochemical Energy Storage

doi:10.15541/jim20250429

Abstract

Abstract:

Two-dimensional (2D) layered materials have attracted extensive attention in the field of electrochemical energy storage due to their ordered layered structure, tunable interlayer spacing, and rich surface chemistry. In particular, the strategy of utilizing their 2D layered structure to construct oriented ion transport channels in electrochemical energy storage devices (e.g., metal-ion batteries, lithium-sulfur batteries, sodium-sulfur batteries, and supercapacitors) has become one of the current research hotspots. By achieving oriented alignment of 2D layered materials in various components of electrochemical energy storage devices (e.g., electrodes, separators, and solid-state electrolytes), long-range ordered ion transport channels with low tortuosity can be constructed, enabling high-speed ion transport and effectively enhancing the charge-discharge performance of these devices. This review focuses on the ion transport processes in electrochemical energy storage devices and provides a comprehensive overview of the research progress in constructing oriented ion transport channels using typical 2D layered materials (e.g., two-dimensional transition metal carbonitrides (MXenes), layered double hydroxides (LDHs), 2D layered metal-organic frameworks (2D MOFs), graphene, and layered clay minerals) in electrodes, polymer electrolytes, and separators. The advantages and disadvantages of fabrication methods(external electric/magnetic field alignment, shear force alignment, self-assembly, and template methods) for achieving oriented alignment of 2D layered materials are summarized. Furthermore, the influence of the structural characteristics of oriented ion transport channels on ion transport performance, including ionic conductivity, cation transference number, and ion diffusion coefficient, is analyzed, and the ion transport mechanisms within 2D layered oriented ion transport channels are discussed in depth. Finally, the current challenges and issues are concluded, and future research directions are proposed with the aim of providing insights for the development of high-performance electrochemical energy storage devices.

Key words: 2D layered material, electrochemical energy storage device, electrode, electrolyte, separator, oriented ion transport channel, review

CLC Number:

TB332

QIN Shanli, GUO Jiawen, CHEN Yanmeng, JU An’an, WEI Yi, HUANG Kelin, HOU Xianghua, LÜ Sishi, WEN Zhipeng, WU Lian. Recent Advances in Constructing Oriented Ion Transport Channels with Two-dimensional Layered Materials for Electrochemical Energy Storage[J]. Journal of Inorganic Materials, 2026, 41(7): 883-898.

Figures/Tables 9

Fig. 1 Schematic diagrams of constructing directional ion transport channels using 2D layered materials (a) Microscopic ion transport channel structure between 2D layered materials; (b) Microscopically disordered ion transport pathways; (c) Microscopically ordered and vertically arranged ion transport pathways

Table 1 Advantages and disadvantages of the method for constructing ion transport channels via the oriented arrangement of 2D layered materials[30,34,40 -41]

Method	Advantage	Disadvantage
Self-assembly	Simplified procedure; being free complex equipment; low cost & scalable	Dependence on specific surface groups; limited self-organization control
External field-assisted orientation arrangement	Precise tuning of orientation & order; adjustable field parameters; high-alignment performance	High operational precision; expensive equipment
Template-assisted method	Tailorable template design; accurate morphology/ size/orientation control; high alignment accuracy	Complex template fabrication; structure damage during removal; residual impurities lowering purity
Freeze-drying	Mild physical process; wide material compatibility; preserved intrinsic properties	Strict thermal control; high equipment cost; uneven ice growth inducing defects

Fig. 2 Application of 2D layered materials in constructing directional ion channels in electrode materials[42,45,50] (a) Schematic diagram of vertical alignment of VOPO4 nanosheets induced by solvent evaporation[42]; (b) Rate capability of conventional electrodes as a function of mass loading[42]; (c) Rate capability of vertically aligned nanosheets (VANS) electrode at 5 mg·cm−2[42]; (d, e) HRTEM images of Ti2CTx/C (d) before and (e) after Sn4+ intercalation[45]; (f) Rate performance of Ti2AlC/C, Ti2CTx/C, and Sn4+-Ti2CTx/C electrodes[45]; (g) Schematic fabrication of flexible V-rGO/tannic acid (TA)/laser-pretreated graphite paper (LGP) electrodes via laser assistance[50]; (h) Galvanostatic charge-discharge curves of the quasi-solid-state aqueous zinc-ion hybrid capacitors[50]

Fig. 3 Influence of the arrangement of 2D layered materials on the uniformity of lithium deposition and cycle life[52,54] (a-c) Schematics of Li deposition in (a) horizontally aligned rGO aerogel (HGA), (b) randomly arranged rGO aerogel (RGA), and (c) vertically aligned rGO aerogel (VGA)[52]; (d-f) Cross-sectional scanning electron microscope (SEM) images of (d) HGA and (e) RGA after 40 cycles, and (f) VGA after 100 cycles (cycling current density: 3 mA·cm-2, capacity: 3 mAh·cm-2, carbonate electrolyte)[52]; (g) Rate capability and long-term cycling performances of LFP||Li cells[52]; (h) Synthesis and SEM images of v-Ti3C2Tx electrodes[54]; (i) Coulombic efficiencies of V-Ti3C2Tx and H-Ti3C2Tx electrodes at 1.0 mAh·cm-2[54]

Fig. 4 Application of 2D layered materials in constructing directional ion channels in SPEs[64,68,70] (a) Schematic illustration of the synthesis of composite solid-state electrolytes (CSEs) with NFO nanosheets and a rational mechanism for ion transport in CSEs applied in lithium metal batteries[64]; (b) Arrhenius curves of CSEs with vertically aligned NFO-PEO (ANFO-PEO), random aligned NFO-PEO (RNFO-PEO), and PEO-LiTFSI (PL)[64]; (c) Average values of transference number along with their standard errors[64]; (d-f) Cross-sectional SEM images of (d) VAVS and (e) VAVS-CSPE (UV etched), (f) Li electrode surface after test for about half-month with VAVS-CSPE electrolytes[68]; (g) Galvanostatic cycling performance of Li/SPE/Li symmetric cells measured at 35 ℃ with 0.5 mA·cm-2 current density[68]; (h) Schematic illustration of the preparation of VALS-CSPE[70]; (i) Galvanostatic tests of Li|Li cells at 0.10 mA·cm−2[70]

Fig. 5 High critical current density and dendrite free lithium deposition of PEO-based solid electrolyte by Cu-MMT/gelatin vertical array[72] (a) Cross-scale synergistic rectification strategy through the ion rectifier; (b) Top view SEM images of ion rectifier of the vertical channel surface; (c) Chemical structure and electron density distribution of tripeptide (hydroxyproline-proline-glycine, Hyp-Pro-Gly) abundantly present in gelatin (top), binding energies of Hyp-Pro-Gly and PEO chain segments with Li+, respectively (bottom); (d, e) Critical current density tests of (d) CGVA-PEO/LiTFSI and (e) PEO/LiTFSI; (f) Ionic conductivity−temperature curves of different electrolytes; (g) Current variation with polarization of Li//CGVA-PEO/LiTFSI//Li symmetrical cell with an applied potential of 10 mV with inset showing electrochemical impedance spectroscopy (EIS) plots before and after polarization; (h) Top-view SEM images (top) and corresponding X-ray computed tomography (X-CT) images (bottom) of Li anodes with different electrolyte membranes after 20 cycles at 0.1 mA·cm−2 and 0.1 mAh·cm−2

Fig. 6 Application of 2D layered materials in constructing directional ion channels in GPEs[22,79] (a) Top-view SEM image of VAMMT[22]; (b) Cross-sectional SEM image of VAMMT[22]; (c) Arrhenius ionic conductivity (σ) plots of CMP/VAMMT, CMP/MMT and pure CMP[22]; (d) Li+ transference numbers of different electrolytes[22]; (e) Schematic illustration for the in situ polymerization of COF-templated method (PDCM)[79]; (f) 2D wide-angle X-ray scattering (WAXS) patterns of COF powder and COF membrane (COFM)[79]; (g) SEM images of the fracture surface for PDCM[79]; (h) Galvanostatic cycling curves of the Li||Li symmetric cells assembled with PDCM and PDOL@PP (PDPP)[79]

Fig. 7 Application of 2D layered materials in constructing directional ion channels in separator[82-83,85] (a) SEM morphologies of homogeneous membrane synthesized by low-temperature crystallization method (LTCM) (scale bar: 5 μm) with inset showing the optical image with the dimensions of 6 cm×6 cm[82]; (b) Cross-sectional SEM morphologies of TpPa-SO3H FSF (Tp: 1,3,5-triformylphloroglucinol; Pa-SO3H: 2,5-diaminobenzenesulfonic acid; FSF: free-standing form) homogeneous membrane (scale bar: 10 μm)[82]; (c) Migration number results of TpPa-SO3H HPF (HPF: high-pressure form) and TpPa-SO3H FSF in Zn-Zn symmetric batteries[82]; (d) Long cycling performance of zinc-iodine batteries using TpPa-SO3H FSF separator under the condition of 2 A·g−1 with an active mass loading of 5 mg·cm−2 with insets showing the photo of Zn anode foil after cycling (scale bar: 8 mm) and the corresponding XRD patterns[82]; (e) Coulombic efficiency (CE), voltage efficiency (VE), and energy efficiency (EE) during the charge-discharge cycling of zinc-iodine flow battery (20 mA·cm−2) using TpPa-SO3H FSF separator with inset showing the first 10 charge-discharge curves[82]; (f) Schematic of aligned ASU-LDH nanosheets under applied-electric field[83]; (g) Durability test of σ values of xDA-MMT films and Nafion NR211 film with a 25.4 μm thickness[85]; (h, i) Single-cell performances of (h) vertically aligned polydopamine-intercalated montmorillonite membrane (VAPMM)-based and (i) N117-based membrane electrode assembly from 30 to 75 ℃ with 100% relative humidity (RH)[85]

Fig. 8 Ionic transport mechanisms of 2D layered materials promoting electrochemical energy storage process[22,46,61,79] (a) 6Li solid state nuclear magnetic resonance (SSNMR) spectra of CMP/VAMMT before (left) and after (right) discharge in the 6Li‖Cu cell[22]; (b) Synchrotron radiation X-ray diffraction (λ=0.2073 Å) patterns of pristine MMT, pristine CMP/VAMMT, cycled CMP/VAMMT, and the glass window[22]; (c) Raman spectra and fitting curves of PHL1.25 and PHL1.25BN5 electrolytes in 730-760 cm−1 (CIP: contact ion pair; AGG: aggregated ion pair)[61]; (d) Quantitative analysis of CIPs and AGGs of PHL1.25 and PHL1.25BN5 electrolytes[61]; (e) COMSOL multiphysics simulation results of the Zn2+ ions distribution behaviors of LH-Ti3C2Tx and H-Ti3C2Tx[46]; (f) Zn2+ ions concentration distribution versus diffusion depth through the cathode of LH-Ti3C2Tx and H-Ti3C2Tx[46]; (g) Distribution profiles of CF3SO32− detected by time-of-flight secondary ion mass spectrometer (TOF-SIMS) from the cycled Zn anodes in Zn||LH-Ti3C2Tx and Zn||H-Ti3C2Tx[46]; (h) 2D contour plots of the in situ XRD test results within one charge/discharge cycle of Zn||LH-Ti3C2Tx ZHCs[46]; (i, j) 1H-13C cross polarization-heteronuclear correlation nuclear magnetic resonance (CP-HETCOR NMR) spectra of (i) PDOL-COF physical mixture and (j) PDCM composite[79]; (k) Theoretical elucidation of Li+ migration behaviors in PDCM and COFM (initial, intermediate, transition, and final states are abbreviated as IS, IM, TS, and FS, respectively)[79]

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