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. 2026 Jan 28;12(5):eaeb1378. doi: 10.1126/sciadv.aeb1378

In situ anchoring 2D hexagonal Zn-MOF on MXene toward robust anode-less 5 V–class Li metal batteries

Yuan Tian 1, Zhihao Pei 1, Deyan Luan 1, Xiong Wen (David) Lou 1,*
PMCID: PMC12851024  PMID: 41604491

Abstract

Anode-less 5 V–class lithium metal batteries (LMBs) promise high energy density and safety yet, in practice, face critical challenges including dendrite growth, interfacial instability, pulverization associated with “dead” lithium accumulation, and energy density compromise from the use of heavy copper collector. Here, we demonstrate an elaborate design of two-dimensional hexagonal zinc-containing metal-organic framework anchored on conductive titanium carbide (Ti3C2Tx) MXene sheets (MX/2D-Zn-MOF) as a three-dimensional lightweight host for anode-less 5 V–class LMBs. The abundant nitrogen/fluorine/zinc-rich lithiophilic sites effectively decrease lithium nucleation energy barriers, ensure uniform lithium deposition, and stabilize solid electrolyte interphase. The interconnected three-dimensional framework further guides uniform lithium deposition by spatially homogenizing lithium ion flux and reducing local current density as well as offers sufficient space to alleviate structural change, thus affording structural integrity against pulverization. As a result, the MX/2D-Zn-MOF host demonstrates uniform lithium deposition, reversible lithium plating and stripping behavior, and stable cycling performance (~1800 hours at 1.0 milliamperes per square centimeter and 5.0 milliampere hours per square centimeter). Impressively, the assembled anode-less 5 V–class lithium metal pouch cell delivers stable cycling performance and high energy density.

2D hexagonal Zn-MOF is in situ anchored on MXene as a host for robust anode-less 5 V–class Li metal batteries.

INTRODUCTION

Advanced energy storage systems with superior energy density, cycling stability, and safety are imperative to meet the surging energy demands in electric mobility, portable electronics, and artificial intelligence infrastructure (1, 2). Li metal stands out as an exceptional anode, featuring an unparalleled theoretical specific capacity (3860 mAh g−1) and the most negative electrochemical potential (−3.04 V versus standard hydrogen electrode) (3–5). In particular, anode-less 5 V–class Li metal batteries (LMBs) integrating lean-Li anodes with 5 V–class LiNi0.5Mn1.5O4 (LNMO) cathodes show great promise for achieving high energy density and safety through minimized Li usage and maximized operating voltage (6–9).

Nevertheless, their implementation faces multiple challenges. Under limited Li conditions, a stable substrate is essential to support the small amount of Li. However, the commonly used heavy and inactive Cu collector substantially compromises high-capacity advantages of lean-Li anodes (10–12). Moreover, uneven Li nucleation and growth on the lithiophobic Cu substrate and massive volume fluctuations of Li during cycling trigger continuous dendritic growth, repeated destruction and regeneration of solid electrolyte interphase (SEI), and electrochemically inactive “dead” Li accumulation (13–17). These issues, combined with finite Li reserves, exacerbate electrode pulverization and accelerate capacity decay (16–19).

Interfacial engineering, such as introducing lithiophilic seeds [e.g., Sn (4), Zn (20), and Ag (21, 22)] and constructing artificial SEI layers [e.g., N-rich (3, 23) and F-rich (1, 24–26) species], has proven effective in improving kinetics and interfacial thermodynamic stability, homogenizing Li nucleation, and suppressing dendrites. Among various materials, metal-organic frameworks (MOFs), featuring tunable networks and diverse compositions through multifarious coordination of metal nodes and ligands, show great promise as effective interface modifiers (27–32). However, solely applying interfacial engineering to the Cu current collector is hard to prevent electrode electro-chemo-mechanical pulverization, especially under Li-limited conditions (10, 33). To further prevent electrode pulverization, integrated three-dimensional (3D) freestanding electrode is desirable to buffer volume fluctuation, maintain structural integrity, and provide additional spatial regulation for Li deposition (10, 34). Given these considerations, developing multifunctional all-in-one hosts with integrated features of lightweight, robust lithiophilicity, and pulverization resistance is fundamental to achieve high reversibility and extended cycle life in anode-less 5 V–class LMBs.

Here, we design a facile strategy to construct a 3D network architecture comprising Ti3C2Tx MXene (MX) sheets anchored by 2D hexagonal Zn-containing MOF (MX/2D-Zn-MOF) as a lightweight host for stable anode-less 5 V–class LMBs. Tailoring Zn2+/ligand concentrations enables precise control over Zn-MOF morphology. The MX/2D-Zn-MOF leverages the conductivity of MX and ion-regulation capability of 2D-Zn-MOF, effectively prevents MX restacking, and exposes abundant N/F/Zn-rich active sites, thereby ensuring homogeneous Li deposition and stabilizing SEI. Moreover, the interconnected 3D bicontinuous networks not only spatially homogenize Li deposition by uniformizing electric field and decreasing local current density but also offer sufficient space to buffer volume fluctuations, thus affording structural integrity and suppressing pulverization. Benefiting from these structural and interfacial advantages, the MX/2D-Zn-MOF realizes low overpotential enabling dendrite-free Li deposition, high plating/stripping reversibility with small voltage hysteresis, and stable cycling performance for more than 1800 hours at 1.0 mA cm−2 and 5.0 mAh cm−2. The assembled anode-less 5 V–class Li metal pouch cell (MX/2D-Zn-MOF-Li||LNMO) achieves stable cycling performance with 90% capacity retention after 120 cycles. Furthermore, a 0.37 Ah–level anode-less Li metal pouch cell is assembled and exhibits decent cycling stability and high energy density of 538.6 Wh kg−1 based on the active materials of both cathode and anode.

RESULTS

Formation process and characterization of MX/2D-Zn-MOF

The synthesis procedure of lightweight flexible MX@2D-Zn-MOF is schematically illustrated in Fig. 1A. Initially, the MX colloidal solution comprising 2D Ti3C2Tx sheets is synthesized through the chemical etching from bulk Ti3AlC2 (fig. S1) using HCl/LiF etchants, followed by mild exfoliation. Multiple characterizations, including transmission electron microscopy (TEM), field-emission scanning electron microscopy (FESEM), energy-dispersive x-ray (EDX) spectroscopy, x-ray diffraction (XRD), and x-ray photoelectron spectroscopy (XPS) (Fig. 2, A and D, and figs. S2 and S3), indicate the successful synthesis of single/few-layered Ti3C2Tx sheets with abundant electronegative functional groups (-F, -O, and -OH) (22, 35, 36). Subsequently, Zn2+ ions are added into MX colloidal solution, forming a robust Ti3C2Tx-Zn2+ precursor through electrostatic interaction between positively charged Zn2+ and electronegative terminals of MX. Afterward, Zn-MOF crystals are in situ grown on MX sheets through coordination reaction between Ti3C2Tx-Zn2+ precursor and 2-methylimidazole ligands.

Fig. 1. Formation process of MX/2D-Zn-MOF.

Fig. 1.

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(A) Schematic illustration of the synthetic route for Zn-MOF and MX/2D-Zn-MOF. (B to E) FESEM, (F to I) TEM, (J to M) high-angle annular dark-field (HAADF)–scanning TEM (STEM) and corresponding elemental mapping images of (B, F, and J) dodecahedral Zn-MOF (dodeca-Zn-MOF), (C, G, and K) accordion-like Zn-MOF (accordion-Zn-MOF), (D, H, and L) 2D-Zn-MOF, and (E, I, and M) MX/2D-Zn-MOF. Scale bars, 500 nm [(J) to (M)].

Fig. 2. Structural and morphological characterizations.

Fig. 2.

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(A to C) FESEM and (D and E) TEM images of (A and D) MX and (B, C, and E) MX/2D-Zn-MOF. (F) HAADF-STEM images of MX/2D-Zn-MOF. (G) XRD pattern of 2D-Zn-MOF with Pawley-refined crystal structure. a.u., arbitrary units. (H) C 1s XPS spectra of MX/2D-Zn-MOF and 2D-Zn-MOF. (I) N 1s, F 1s, and Zn 2p XPS spectra of MX/2D-Zn-MOF.

Notably, the crystal structure and morphology of Zn-MOF can be precisely modulated by adjusting the concentrations of Zn2+ and 2-methylimidazole in the reaction medium (i.e., deionized water or MX colloidal solution). Under a constant molar ratio of Zn2+/2-methylimidazole, decreasing reactant concentrations in deionized water yields three distinct Zn-MOFs, i.e., rhombic dodecahedral Zn-MOF with sodalite topology (dodeca-Zn-MOF; Fig. 1, B and F, and fig. S4), accordion-like Zn-MOF (accordion-Zn-MOF; Fig. 1, C and J, and fig. S5), and hexagonal 2D Zn-MOF with diamondoid topology (2D-Zn-MOF; Fig. 1, D and H, and fig. S6). EDX spectra (fig. S7) and elemental mapping images (Fig. 1, J to L) reveal the existence and homogeneous distribution of Zn, C, and N elements throughout three Zn-MOFs but distinct morphology. XRD patterns (fig. S8) further confirm the structural differences. The dodeca-Zn-MOF exhibits characteristic peaks consistent with zeolitic imidazolate framework-8 (37). However, the accordion-Zn-MOF and hexagonal 2D-Zn-MOF show uncommon crystallographic features that fit well with diamondoid topology (38). To validate the diamondoid structure of hexagonal 2D-Zn-MOF, we collected the synchrotron XRD pattern and subjected to Pawley refinement. The excellent agreement between experimental data (red) and calculated patterns (black), with minimal difference (blue line) and well-defined Bragg positions (Fig. 2G), proves the diamondoid topology structure of hexagonal 2D-Zn-MOF.

When directly using MX colloidal solution as the reaction medium, the concentration regulation of Zn2+ and 2-methylimidazole presents versatile morphological and structural evolutions, forming MX/dodeca-Zn-MOF film (fig. S9), MX/accordion-Zn-MOF film (fig. S10), and MX/2D-Zn-MOF film (Fig. 1, E, I, and M, and fig. S11). Cross-sectional FESEM analysis demonstrates that all three MX/Zn-MOF films feature freestanding integrated 3D architectures, indicating successful fabrication of flexible electrodes. The enlarged FESEM images reveal the distribution of rhombic dodeca-Zn-MOF, accordion-Zn-MOF, and 2D-Zn-MOFs within the three composites. Top-view FESEM images (Fig. 2B) demonstrate that the MX/2D-Zn-MOF surface is abundantly decorated with 2D sheets forming a capillary-like texture, distinct from the compact wrinkled surface of MX film. The structural difference between MX and MX/2D-Zn-MOF reveals that the direct growth of 2D-Zn-MOF on MX matrix effectively prevents Ti3C2Tx sheets stacking and exposes abundant active sites, potentially promoting reaction kinetics (37). The enhanced accessibility of these active sites is verified by comparing the N2 adsorption-desorption isotherms of MX and MX/2D-Zn-MOF films (fig. S12). The enlarged FESEM image (Fig. 2C) further indicates that the MX/2D-Zn-MOF has a loose open-channeled architecture conducive to capillary transport. This hierarchical structure ensures rapid electrolyte penetration as evidenced by the negligible contact angle between the MX/2D-Zn-MOF film and electrolyte (fig. S13).

Microscopic characterizations via TEM (Fig. 1I) and elemental mapping images (Fig. 1M) reveal the hexagonal distribution of C, N, and Zn elements superimposed on the underlying MX matrix (C, Ti, and F). High-resolution TEM image (Fig. 2E) exhibits the overlapped lattice fringes of Ti3C2Tx and 2D-Zn-MOF, validating the successful growth of 2D-Zn-MOF on MX matrix. Atomic-resolution high-angle annular dark-field (HAADF)–scanning TEM (STEM) analysis of MX/2D-Zn-MOF (Fig. 2F) demonstrates that the Ti atomic arrangements align with the projected Ti3C2Tx structural models while exhibiting an expanded interlayer spacing of ~1.6 nm along the (002) crystallographic plane compared to pristine Ti3C2Tx (~1.2 nm; Fig. 2D). This structural expansion indicates the strong interaction and binding between 2D-Zn-MOF and MX. The chemical interaction, coupled with the intrinsic high electrical conductivity and 2D feature of MX, could contribute to forming intimate electrical contact and stable heterostructure interfaces, potentially promoting ionic transport kinetics and cycling stability.

The chemical composition and structure of the MX/dodeca-Zn-MOF and MX/2D-Zn-MOF hosts are further confirmed by EDX spectroscopy, XRD, and XPS analyses (figs. S14 to S16). These results prove that the MX/2D-Zn-MOF film combines characteristic peaks of MX and 2D-Zn-MOF (38), indicating their successful integration. High-resolution XPS analysis reveals the chemical environment of the MX/2D-Zn-MOF film, 2D-Zn-MOF powder, and MX film. The deconvolution of high-resolution C 1s spectra reveals multiple chemical states in MX/2D-Zn-MOF, including C-Ti-Tx, C─C, C─N, C═N, and π-π* bonds (Fig. 2H) (28, 39–42), further confirming the successful integration of 2D-Zn-MOF and MX. Moreover, the presence of N, F, and Zn signals (Fig. 2I) in the MX/2D-Zn-MOF host is anticipated to endow it enhanced lithiophilicity (43).

Electrochemical and theoretical evaluation of MX/2D-Zn-MOF for LMBs

To elucidate the functional roles of different components in MX/2D-Zn-MOF during Li nucleation and growth processes, we conducted density functional theory (DFT) calculations (figs. S17 and S18) (24). The calculated Li-binding energies (Eb) with 2D-Zn-MOF, Ti3C2Fx, and Cu (111) are presented in Fig. 3A. Notably, the 2D-Zn-MOF exhibits the highest Eb value, followed by Ti3C2Fx, both exceeding that of conventional Cu. This trend is corroborated by Bader charge analysis (table S2). Interfacial charge density distribution analysis further reveals pronounced charge polarization at the 2D-Zn-MOF/Li interface, confirming strong electronic interactions that facilitate Li nucleation (Fig. 3B) (44). These results indicate superior lithiophilicity of 2D-Zn-MOF, which facilitates uniform Li nucleation and growth.

Fig. 3. Mechanistic investigation of Li plating behavior on different hosts.

Fig. 3.

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(A) Binding energies and (B) interfacial charge density distributions of Li atom on 2D-Zn-MOF, Ti3C2Fx, and Cu (111). (C) Voltage-capacity profiles of Li plating on different hosts tested at 2.0 mA cm−2. Summary of (D) nucleation and (E) plateau overpotentials on different hosts tested at current densities of 1.0, 2.0, and 3.0 mA cm−2. FESEM images of (F) MX/2D-Zn-MOF, (G) MX/accordion-Zn-MOF, and (H) MX hosts after being plated with 20.0 mAh cm−2 of Li.

The synergistic structural and compositional design of the MX/2D-Zn-MOF is expected to enhance lithiophilicity, mitigate dendritic growth, promote reaction kinetics, and improve electrochemical reversibility. To validate these hypotheses, we systematically investigate the energy barriers of Li plating on various substrates at current densities of 1.0, 2.0, and 3.0 mA cm−2 (Fig. 3C and fig. S19). At a current density of 1.0 mA cm−2, different from the sharp potential drop observed in the MX host, both MX/2D-Zn-MOF and MX/accordion-Zn-MOF display gradual potential decline during the Li plating. Quantitatively, the nucleation and plateau overpotentials of MX/2D-Zn-MOF (57.7 and 54.5 mV) are lower than those of MX/accordion-Zn-MOF (65.6 and 62 mV) and MX (194.5 and 57.7 mV). At higher current densities, the MX/2D-Zn-MOF host exhibits comparable but slightly lower nucleation and plateau overpotentials compared to the MX/accordion-Zn-MOF and MX (Fig. 3, D and E). The sharp comparison indicates the decreased Li nucleation barriers on the MX/2D-Zn-MOF owing to abundant lithiophilic species (21, 37). To validate the superiority of MX/2D-Zn-MOF, we further investigate the Li plating behavior on different electrodes. At a current density of 1.0 mA cm−2 with a capacity of 4.0 mAh cm−2, the surface of MX/2D-Zn-MOF is covered by smooth and sparse Li deposits with partially visible 2D-Zn-MOF (fig. S20), whereas the MX shows scattered deposition and dendrites (fig. S21). When Li plating capacity is extended to 20 mAh cm−2, the MX is covered by severe dendrites, reflecting its limited regulation over Li nucleation and deposition. However, the MX/2D-Zn-MOF presents smooth and dendrite-free surface morphology even at higher plating capacities (Fig. 3F) compared to the MX and MX/accordion-Zn-MOF (Fig. 3, G and H). Cross-sectional FESEM images (fig. S22) further verify that the MX/2D-Zn-MOF enables homogeneous Li deposition, as the deposition capacity increases from 15 to 30 mAh cm−2. These results collectively reflect that the MX/2D-Zn-MOF can effectively accommodate volume expansion and promote uniform Li deposition.

The Li plating/stripping reversibility of the MX/2D-Zn-MOF host is evaluated through Coulombic efficiency (CE) measurement. As shown in Fig. 4A, the MX/2D-Zn-MOF demonstrates improved reversibility and cycling stability under diverse current densities and areal capacities (i.e., 1.0 mA cm−2 and 1.0 mAh cm−2, 2.0 mA cm−2 and 1.0 mAh cm−2, 2.0 mA cm−2 and 4.0 mAh cm−2). The voltage-capacity profiles at 2.0 mA cm−2 and 4.0 mAh cm−2 (Fig. 4B) exhibit that the MX/2D-Zn-MOF host maintains minimal voltage hysteresis and highest CE value compared to other hosts, demonstrating enhanced reaction kinetics and reversibility. However, the MX and MX/accordion-MOF exhibit obvious CE fluctuations and faster failure than MX/2D-Zn-MOF, which might be caused by dendrite growth and accumulated dead Li. FESEM images (fig. S23) reveal severe dendrite formation and residual Li deposits on the MX electrode after 100 cycles. Impressively, the cycled MX/2D-Zn-MOF electrode (figs. S24 and S25) maintains structural integrity without visible Li accumulation, suggesting enhanced interfacial stability. This difference likely stems from distinct interfacial chemistry. Thus, to elucidate the underlying interfacial mechanisms, XPS surface analysis and in-depth measurements are conducted. XPS spectra (fig. S26) of MX/2D-Zn-MOF show a slight shift of Zn 2p1/2 and Zn 2p3/2 toward lower binding energies, accompanied by the emergence of Li-N species after Li plating, indicating strong interactions between 2D-Zn-MOF and deposited Li (30, 45, 46). The almost unchanged SEI components after 20 cycles reflect stable interfacial properties. XPS in-depth analysis (fig. S27) of the 100th cycled MX/2D-Zn-MOF with increasing sputtering times demonstrates that the SEI is dominated by LiF constituents, responsible for stable and reversible plating/stripping performance (9, 30, 47). The favorable interfacial properties are proven by electrochemical impedance spectroscopy (EIS) results. The MX/2D-Zn-MOF exhibits consistently lower and more stable charge transfer resistance (Rct) and Li+ ion transport resistance through the SEI (RSEI) than MX at different cycles (fig. S28 and table S3), confirming the formation of stable interphases and enhanced reaction kinetics (48–50). Additional CE measurements at other current densities and areal capacities (0.5 mA cm−2 and 1.0 mAh cm−2, 0.5 mA cm−2 and 2.0 mAh cm−2, 1.0 mA cm−2 and 2.0 mAh cm−2, and 2.0 mA cm−2 and 2.0 mAh cm−2; Fig. 4C and figs. S29 to S32) further validate the superiority of MX/2D-Zn-MOF. At a high areal capacity (5.0 mAh cm−2), the MX/2D-Zn-MOF also realizes reversible and stable Li plating/stripping behavior for ~1800 hours at 1.0 mA cm−2 (Fig. 4D and fig. S33), extending to 2400 hours at 0.5 mA cm−2 (fig. S34). Moreover, even in conventional carbonate-based electrolyte [1 M lithium hexafluorophosphate (LiPF6) in ethylene carbonate (EC)/diethyl carbonate (DEC) (v/v = 1:1) with 5 wt % fluoroethylene carbonate (FEC)], the MX/2D-Zn-MOF host also maintains stable cycling performance over 400 cycles at 2.0 mA cm−2 and 2.0 mAh cm−2 with an average CE of 96.46% (fig. S35).

Fig. 4. Electrochemical performance of different electrodes.

Fig. 4.

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(A) CEs of MX/2D-Zn-MOF, MX/accordion-Zn-MOF, and MX hosts tested at varied current densities and areal capacities. (B) Voltage-capacity profiles of different hosts tested at 2.0 mA cm−2 and 4.0 mAh cm−2. (C) Voltage-time profiles of MX/2D-Zn-MOF tested at 0.5, 1.0, and 5.0 mA cm−2. (D) Long-term cycling stability of MX/2D-Zn-MOF tested at 1.0 mA cm−2 and 5.0 mAh cm−2. (E) Rate performance of different anodes tested at 1.0, 2.0, 3.0, 4.0, 5.0, and 1.0 mA cm−2 with a fixed areal capacity of 1.0 mAh cm−2. (F) Cycling performance of MX/2D-Zn-MOF-Li anode tested at 2.0 mA cm−2 and 3.0 mA cm−2.

Symmetric cells are also assembled using the MX/2D-Zn-MOF-Li, MX/accordion-Zn-MOF-Li, and MX-Li electrodes. The MX/2D-Zn-MOF-Li electrode demonstrates superior rate performance with steadily increased voltage hysteresis of 29.4, 49.9, 70.9, 92.2, and 112.3 mV at current densities from 1.0, 2.0, 3.0, 4.0, to 5.0 mA cm−2 (Fig. 4E). In contrast, the MX/accordion-Zn-MOF-Li electrode displays gradual increased voltage hysteresis after 500 hours, and the MX-Li experiences rapid voltage increase and cell failure after only 200 hours. Even tested at 2.0 and 3.0 mA cm−2, the MX/2D-Zn-MOF-Li electrode can still maintain stable cycling performance for more than 600 hours (Fig. 4F), further highlighting the superior structural stability and Li plating/stripping reversibility of MX/2D-Zn-MOF-Li. The galvanostatic intermittent titration technique (GITT) profiles further reveal distinct kinetic behaviors between the MX-Li and MX/2D-Zn-MOF-Li electrodes. As shown in fig. S36, the MX-Li shows higher polarization, particularly prominent at the start and end of each GITT curve. However, the MX/2D-Zn-MOF-Li shows much lower and more stable voltage profiles during repeated Li plating/stripping process, indicating improved Li+ diffusion capability and faster charge-transfer kinetics (51).

Electrochemical performance of anode-less 5 V–class full cells

To further evaluate the practical potential of lightweight flexible MX/2D-Zn-MOF-Li anode, we assembled anode-less 5 V–class LMBs by coupling a LNMO cathode (fig. S37) with the MX/2D-Zn-MOF-Li anode. For comparison, the full cells with MX/accordion-Zn-MOF-Li and MX-Li anodes are also investigated under same conditions. Cyclic voltammetry profiles of three full cells show similar redox peaks (Fig. 5A). The MX/2D-Zn-MOF-Li||LNMO full cell exhibits a smaller voltage polarization (inset of Fig. 5A), indicating enhanced reaction kinetics endowed by the MX/2D-Zn-MOF-Li anode. Moreover, the MX/2D-Zn-MOF-Li||LNMO full cell with a negative/positive electrode capacity (N/P) ratio of 3 delivers a capacity of 125.8 mAh g−1 with a capacity retention of up to 98.3% upon 120 cycles at 0.5 C (Fig. 5B). In contrast, the full cells using the MX/accordion-Zn-MOF-Li and MX-Li anodes retain merely 78.7 and 39.7% of their initial capacity after 120 cycles, highlighting the superiority of the MX/2D-Zn-MOF-Li anode. The galvanostatic charge/discharge voltage profiles from the first to 120th cycles further validate the results (fig. S38). Complementary EIS analysis (Fig. 5C) demonstrates the lower charge transfer resistance of the MX/2D-Zn-MOF-Li||LNMO full cell, suggesting enhanced reaction kinetics when using the MX/2D-Zn-MOF host (12, 52). The superiority of the MX/2D-Zn-MOF-Li anode is further validated through rate tests (Fig. 5D and fig. S39). The MX/2D-Zn-MOF-Li||LNMO full cell delivers a capacity of 129.8 mAh g−1 at 0.5 C and maintains discharge capacities of 126, 123, 122, and 119 mAh g−1 at 1.0, 1.5, 2.0, and 2.5 C, respectively, outperforming those of full cells based on the MX/accordion-Zn-MOF-Li and MX-Li anodes. At N/P ratios of 2.5 and 3.5, the MX/2D-Zn-MOF-Li||LNMO full cells achieve stable cycling performance upon 120 cycles with capacity retentions of 89.3 and 96.4% at 0.5 C (Fig. 5E), respectively. Besides, at a lower N/P ratio of 1.5, a stable cycling performance with a capacity of 108.4 mAh g−1 after 90 cycles is realized. Even at an N/P ratio of 1.1, the MX/2D-Zn-MOF-Li||LNMO·full cell still exhibits stable cycling performance (fig. S40).

Fig. 5. Electrochemical performance of anode-less 5 V–class Li metal full cells.

Fig. 5.

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(A) Cyclic voltammetry profiles at 0.2 mV s−1; (B) cycling performance; (C) Nyquist plots after 100 cycles; and (D) rate capabilities of MX/2D-Zn-MOF-Li||LNMO, MX/accordion-MOF-Zn-Li||LNMO, and MX-Li||LNMO at an N/P ratio of 3. (E) Cycling stability of MX/2D-Zn-MOF-Li||LNMO at different N/P ratios. (F) Practical demonstration of MX/2D-Zn-MOF-Li||LNMO pouch cell powering a mobile phone. (G) Galvanostatic charge/discharge voltage profiles from first to 100th cycles and (H) cycling performance of anode-less MX/2D-Zn-MOF-Li||LNMO pouch cell. (I) Cycling stability of 0.37 Ah–level anode-less MX/2D-Zn-MOF-Li||LNMO pouch cell.

To further evaluate its practical applications, we assembled a single-layer MX/2D-Zn-MOF-Li||LNMO pouch cell with an N/P ratio of 2.5. As demonstrated in Fig. 5F and fig. S41, the assembled pouch cell successfully powers various electronic devices, including a smartphone, light-emitting diode light strips, and fans, highlighting its robust energy output and stable voltage delivery under different applications. As shown in Fig. 5G, the anode-less 5 V–class pouch cell exhibits highly overlapping curves and characteristic high-discharge voltage plateau at about 4.65 V. Specifically, a capacity of 127.2 mAh g−1 with 90% of its initial capacity after 120 cycles is achieved (Fig. 5H). Impressively, a 0.37 Ah–level MX/2D-Zn-MOF-Li||LNMO pouch cell with an energy density of 538.6 Wh kg−1 (based on the active materials of both anode and cathode) is successfully assembled, showing stable cycling performance (Fig. 5I and fig. S42), which underscores its potential for practical energy storage applications.

DISCUSSION

In summary, we report a hexagonal 2D-Zn-MOF and design a lightweight MX/2D-Zn-MOF host to achieve stable anode-less 5 V–class LMBs. The hexagonal 2D-Zn-MOF–anchored Ti3C2Tx MX creates a freestanding 3D framework with capillary texture that spatially homogenizes Li plating and provides sufficient space to buffer volume fluctuations during cycling, thereby preserving structural integrity against pulverization. In parallel, the abundant N/F/Zn-rich sites with strong lithiophilicity decrease Li nucleation overpotential, ensure uniform Li deposition, and stabilize SEI. Experimental observations and DFT calculations validate that the MX/2D-Zn-MOF achieves low overpotentials, fast reaction kinetics, and uniform Li deposition. The MX/2D-Zn-MOF electrode demonstrates reversible Li plating/stripping at varied current densities and capacities and sustains stable cycling performance over 1800 hours at 1.0 mA cm−2 and 5.0 mAh cm−2. As a result, the MX/2D-Zn-MOF-Li||LNMO full cells at low N/P ratios exhibit stable cycling performance. Moreover, the anode-less 5 V–class Li metal pouch cell realizes stable cycling performance with 90% capacity retention after 120 cycles. Impressively, a 0.37 Ah–level anode-less Li metal pouch cell also achieves stable cycling performance and high energy density of 538.6 Wh kg−1 based on the active materials of both anode and cathode. This work provides an efficient strategy to design 3D multifunctional integrated electrodes for stable anode-less high-voltage 5 V–class LMBs.

MATERIALS AND METHODS

Synthesis of 2D-Zn-MOF, accordion-Zn-MOF, and dodeca-Zn-MOF

2-Methylimidazole (186 mg, Sigma-Aldrich) and zinc acetate dihydrate [50 mg, Zn(CH3COO)2·2H2O, Sigma-Aldrich] were separately dissolved in 10 ml of deionized water. The 2-methylimidazole solution was rapidly added to the zinc acetate solution and stirred for 4 hours at 35°C in a water bath. The white suspension was collected by centrifugation at decreasing speeds [from 6000 to 3000 revolutions per minute (rpm)] and washed with deionized water. The resultant product was dried overnight in a vacuum oven. Accordion-Zn-MOF and dodeca-Zn-MOF were synthesized following the identical procedure with adjusted precursor amounts while maintaining the same reaction conditions and solution volumes. For accordion-Zn-MOF, 372 mg of 2-methylimidazole and 100 mg of Zn(CH3COO)2·2H2O were used. For dodeca-Zn-MOF, the amounts of 2-methylimidazole and Zn(CH3COO)2·2H2O were 1116 and 300 mg, respectively.

Synthesis of MX@2D-Zn-MOF

LiF (800 mg) was dissolved in 7.5 ml of HCl (38 wt %) and 2.5 ml of deionized water. Five hundred milligrams of Ti3AlC2 powder (purchased from Laizhou KaiKai Ceramic Materials Co. Ltd.) was gradually added into HCl/LiF solution and stirred for 24 hours at 35°C. The product was washed using deionized water until pH up to 7, followed by the repeated hand-shaking and centrifugal (3500 rpm ) processes. The supernatant was collected to obtain a uniform MX colloidal solution containing single-/few-layer Ti3C2Tx sheets with a concentration of ~1 mg ml−1. Subsequently, 50 mg of Zn(CH3COO)2·2H2O was added into 10 ml of MX colloidal solution and stirred for 1 hour. Then, 0.186 g of 2-methylimidazole was dissolved in 10 ml of deionized water and added to the MX/Zn(CH3COO)2·2H2O mixture. The resulting solution was stirred continuously for 4 hours at 35°C. Using a vacuum filtration device, 5 ml of MX colloidal solution was first filtered onto a polyvinylidene difluoride (PVDF) water-based filter membrane. While the membrane remained sufficiently wet, 10 ml of the prepared mixture was added. The final product was washed using deionized water to remove residual impurities and lastly dried in a vacuum oven. The thickness and areal mass loading of MX/2D-Zn-MOF were around 81 μm and 1.5 mg cm−2, respectively.

Material characterizations

Morphological characterization was performed using FESEM (Thermo Fisher Scientific, Quattro ESEM & TESCAN MIRA LMS) and TEM (Thermo Fisher Scientific, Talos-F200X G2). Elemental composition and distribution were analyzed through EDX spectroscopy coupled with FESEM and TEM. XRD patterns of the samples were recorded using Bruker D2 PHASER X-ray Diffractometer with Ni-filtered Cu Kα radiation. XPS measurements were conducted on a Thermo Fisher Scientific ESCALAB 250Xi spectrometer, with spectra calibrated to the C 1s peak at 284.8 eV. The cycled electrodes were rinsed with dimethyl carbonate and transferred to an XPS chamber through a vacuum transfer device.

Electrochemical measurements

Electrochemical tests were conducted using CR2032 coin-type cells assembled in an Ar-filled glove box. One piece of Celgard 2325 with a diameter of 19 mm was used as the separator. A total of 1 M LiPF6 in a mixture of 1:3:1 wt % FEC, 3,3,3-fluoroethylmethyl carbonate, and 1,1,2,2-tetrafluoroethyl-2′,2′,2′-trifluoroethyl ether was used as electrolyte, unless otherwise specified. GITT and galvanostatic charge/discharge measurements were performed using a NEWARE battery test system (CT-4008-5V10mA-164). Cyclic voltammetry and EIS measurements were conducted on a CHI760E electrochemical workstation. To investigate the CE of Li plating/stripping, MX/2D-Zn-MOF, MX/accordion-Zn-MOF, and MX were used as the working electrodes, while Li foil was used as the counter and reference electrodes. For the cyclic stability tests, Li was preplated on these hosts to obtain MX/2D-Zn-MOF-Li, MX/accordion-Zn-MOF-Li, and MX-Li electrodes, which were then assembled into symmetric cells for evaluation. GITT tests were also performed using Li||Li symmetric cells with MX/2D-Zn-MOF-Li, MX/accordion-MOF-Li, and MX-Li electrodes. The symmetric cells were plated and stripped at 1.0 mA cm−2 for 1 hour, followed by an intermittently applied current (1.0 mA cm−2 for 6 min) and a resting period of 12 min, until a total plating/stripping capacity of 1.0 mAh cm−2. This procedure was repeated for several cycles. For the full cells, commercial 5 V–class LNMO (Canrd Technology Co. Ltd.) was used as the active material in cathode. The cathode was fabricated by mixing LNMO powder, PVDF, and Super P with a weight ratio of 90:5:5 into N-methyl-2-pyrrolidone solvent to form a slurry. The slurry was stirred for 24 hours, cast onto Al foil, and dried overnight in a vacuum oven at 130°C. The cathodes were punched into disks with a diameter of 12 mm. The full cell was operated within a voltage window of 3.5 to 5.0 V. The specific capacity in full cell was normalized by the mass of the LNMO active material. All electrochemical measurements, including CE, overpotential, and cycling performance, were performed on at least two independently assembled cells that yielded similar results to ensure reproducibility.

Acknowledgments

Funding:

X.W.L. acknowledges the funding support for the Global STEM Professorship from the Innovation, Technology and Industry Bureau (“ITIB”) and Education Bureau (“EDB”) of Hong Kong.

Author contributions:

X.W.L. and Y.T. conceived the idea. Y.T. carried out the material synthesis, characterization, and electrochemical measurements. Z.P. conducted the DFT calculation. Y.T. drafted the initial manuscript. Y.T., Z.P., D.L., and X.W.L. discussed the results and contributed to the manuscript.

Competing interests:

The authors declare that they have no competing interests.

Data and materials availability:

All data and code needed to evaluate and reproduce the results in the paper are present in the paper and/or the Supplementary Materials.

Supplementary Materials

This PDF file includes:

Supplementary Text

Figs. S1 to S42

Tables S1 to S3

sciadv.aeb1378_sm.pdf (4.3MB, pdf)

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Associated Data

This section collects any data citations, data availability statements, or supplementary materials included in this article.

Supplementary Materials

Supplementary Text

Figs. S1 to S42

Tables S1 to S3

sciadv.aeb1378_sm.pdf (4.3MB, pdf)

Data Availability Statement

All data and code needed to evaluate and reproduce the results in the paper are present in the paper and/or the Supplementary Materials.

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