An Energy-Dense and High-Power Li-Cl2 Battery by Reversible Interhalogen Bonds

doi:10.21203/rs.3.rs-2108521/v1

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An Energy-Dense and High-Power Li-Cl2 Battery by Reversible Interhalogen Bonds

https://doi.org/10.21203/rs.3.rs-2108521/v1

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Anionic redox reactions would achieve a high capacity than typical transition-metal-oxide cathodes, offering a low-cost chemistry to advance the energy storage capability of lithium-ion batteries. Li-Cl₂ chemistry using anionic redox reactions of Cl^0/−1 shows superior operation voltage (~ 3.8 V) and capacity (756 mAh g^− 1). However, a redox-active and reversible chlorine cathode has not been developed in organic electrolytes-based lithium-ion batteries. Chlorine ions bonded by ionic bonding hardly dissolve in organic electrolyte, imposing a thermodynamic barrier for redox reactions. Meanwhile, chlorine gas is easily formed during oxidation. Herein, we report an interhalogen compound, iodine trichloride (ICl₃), as the cathode to address these two issues. In-situ and ex-situ spectroscopy data and calculations reveal that reduced Cl⁻ ions are partially dissolved in the electrolyte, and oxidized Cl⁰ is anchored by forming interhalogen bonds with I. A reversible Li-Cl₂ at room temperature is developed, which delivers a specific capacity of 302 mAh g^− 1 at 425 mA g^− 1, and a 73.8% capacity retention at 1250 mA g^− 1. The demonstration of reversible interhalogen bonds enabled rechargeable Li-Cl₂ battery opens a new avenue to develop halogen compound cathodes.

Li-Cl2 batteries

high energy density

high voltage

interhalogen bonds

high reversibility

The past ten years have witnessed tremendous progress in the development of the energy density of lithium-ion batteries¹. However, the pace of advance slows down because conventional ways to improve energy densities are meeting their fundamental limits^2–10. Charges are stored by intercalating lithium ions into crystalline materials, but the amount of stored charges is approaching the theoretical maximum^11–15. Even worse, many electrode materials contain expensive elements, nickel and/or cobalt, for instance, which impedes the construction of grid-level energy storage stations and therefore plagues the transition to renewable energies^16–19. Alternative ways to further boost up energy density of lithium-ion batteries are being intensively investigated. For instance, conversion chemistries of chalcogenides (e.g., S, Se) and halogens (e.g., I₂, Br₂, Cl₂) that use redox reaction of compounds show high theoretical capacity, from 221 to 756 mAh g^− 1, up to ཞ4 times higher than that of the typical intercalation cathode materials (~ 200 mAh g^− 1 for NMC811). Notably, these materials are abundant and cheap, becoming a strong competitor^{4, 20–22}.

In principle, halogens Cl, Br, and I, are all suitable for high-energy batteries because the conversion reaction of halogens allows for a large amount of charge transfer. Br and I have been widely investigated^23–27 but the development of Cl-based lithium batteries is plagued though it may deliver the highest theoretical capacity and voltage among these three halogens. Typically, thermodynamically unstable gaseous Cl₂ is used as the cathode^{2, 28}, and thus cannot discharge on the electrode, posing a significant limitation to the general utility of the battery.

Challenges toward reversible Cl^0/−1 redox reaction at the cathode side are manifold. The ideal case for the Cl₂ redox (dimethoxyethane (DME) and dioxolane (DOL) electrolyte as an example) is shown in Fig. 1a. First, Cl⁻ ions should be abundant and highly mobile in the electrolyte, facilitating the Cl^− 1/0 redox reaction. Second, free oxidized Cl⁰ needs to be bonded to the electrode-electrolyte interface by using adsorbents and/or chemical/physical fixations, otherwise the Cl₂ generation will occur, resulting in the irreversibility. These two challenges post very high requirements on the electrode/electrolyte design. In terms of the mobile chlorine ions, inorganic chloride compounds, such as lithium chloride (LiCl) or sodium chloride (NaCl), are almost completely insoluble in organic electrolytes (Figs. 1b, S1, and S2). In addition, the solid-state mass transfer from chloride compounds to Cl⁰ is thermodynamically unrealistic^29–31. A clear demonstration showing the inactivity of inorganic chloride compounds is exhibited in Fig. 1c. No oxidation peak of Cl⁻ occurs during the cyclic voltammetry (CV) test, and neither does the reduction peak. Only a capacitive behavior can be identified. Some organic chloride compounds, such as tetrabutylammonium chloride (TBACl), can partially dissolve in the electrolyte and provide Cl⁻ for redox reactions. However, unbonded Cl⁰ generates gaseous Cl_2, resulting in the loss of active materials and limited reversibility (Fig. 1d). Correspondingly, an intense oxidation polarization could be observed in the CV curve as the current density after 3.8 V increases dramatically (Fig. 1e). As a result, a reduction peak is still missing, implying the escape of Cl⁰.

Graphite has been used as an anchoring material to stabilize Cl⁰ with the assistance of other halogen ions^{32, 33}. Another example of the reversible Cl^0/−1 reaction in a battery is to deposit inorganic chloride compounds from the electrolyte during the first discharge in a carbon host³⁴. The formation of a thin inorganic chloride layer is crucial for reversibility, but it is relatively inert and cannot fully release the Cl^0/−1 reaction capacity. So far, an intermediate material is needed for the reversible reaction of Cl^0/−1, which limits the prospect of Cl cathodes to some extent. It is expected to realize fast oxidation relying on an unblocked mass transfer path in organic electrolytes.

Here, we report the iodine trichloride (ICl₃) as a cathode for a Li-Cl₂ battery. Reduced Cl⁻ is partially soluble in the organic electrolyte, facilitating oxidation via a liquid-solid pathway. The Cl⁰ is efficiently and chemically anchored by forming interhalogen bonds with I and hence allows for the Cl^0/−1 reaction in a highly reversible manner. The rich chemistry of ICl₃ makes it possible to achieve multiple electron reaction and, therefore high capacity. The ICl₃ cathode exhibits outstanding performances with a specific capacity of 302 mAh g^− 1 (based on the ICl₃ mass throughout this paper unless otherwise specified) at 425 mA g^− 1 and an excellent rate capability (73.8% capacity retention at 1250 mA g^− 1).

We use activated carbon (YP50) with a large Brunauer-Emmett-Teller (BET) surface area (1742 m² g^− 1, Figure S3) to host the ICl₃, which offers abundant sites for the Cl^− 1/0 redox reaction³⁵. SEM images and the corresponding elemental mapping (Figure S4) demonstrate evenly distributed ICl₃ in micropores of the YP50. The open circuit voltage (OCV) of the ICl₃ cathode is about 3.5 V. No peaks are observed during the first anodic sweep from the (OCV) to 4.0 V (Figure S5) because I and Cl atoms are strongly bonded by halogen bonds, showing no reactivity as a compound. Figure 2a shows the stabilized CV curve. During the cathodic sweep, three prominent peaks at 2.9, 3.3, 3.8 V and a shoulder peak at 3.2 V are recognized. By contrast, the pure I₂ electrode only shows a cathodic peak at around 2.8 V (Figure S6), which is attributed to the reduction of I₃⁻ to I^− 36. This peak is also found in Fig. 2a, indicating that the redox reaction of I⁻ ions is also activated. Correspondingly, the other three peaks are attributed to the Cl-induced reactions. The galvanostatic charge/discharge profile (Fig. 2b) shows three discharge plateaus at 3.85, 3.4 and 3.0 V, respectively, consistence with three prominent peaks in the CV curve. In specific, the ICl₃ electrode delivers a capacity of 302 mAh g^− 1. The reduction of I₃⁻ to I⁻ (plateau at 3.0 V) contributes about 1/6 of the capacity, while the other two main plateaus offer about 2/3 of the capacity, showing the Cl-induced reactions are the primary source of the capacity.

First-principle density-functional theory (DFT) calculations were employed to predict the conversion path and structural evolution of the ICl₃ (Figs. 2c and S7-10)^{37, 38}. As the last cathodic peak (2.8 V) is identified as the reduction of I₃⁻ to I⁻, the end products are I⁻ and Cl⁻, implying that the halogen bonds by sharing the lone-pair electrons of I and Cl in the ICl₃ compound are broken. We calculated the Gibbs free-energy (ΔG) for extracting Cl⁻ from ICl₃^39–41. Either forming ICl or ICl₂⁻ is possible for the first reduction step. From the thermodynamic point of view, forming ICl₂⁻ is more likely because its ΔG (-9.07 eV) is much larger than for the ICl formation. The electrostatic potential of the ICl₂⁻ is balanced (Figure S7), supporting the existence of ICl₂ intermediate products. The extracted Cl from ICl₃ accepts one electron, generating the first reduction peak. Next, the formation of I₂Cl⁻ is preferable as the ΔG for I₂Cl- is larger than that of I₂. A fast transition to I₃⁻ would be expected as the ΔG from I₂Cl⁻ to I₃⁻ is very small (-0.93 eV). Furthermore, the electrostatic potential structure of I₂Cl⁻ is less stable than I₃⁻ (Figure S10), which also supports the assumption of the fast change to I₃⁻. This prediction can be evidenced by the shoulder peak corresponding to the transition from I₂Cl⁻ to I₃⁻ at 3.2 V in Fig. 2a. Through the reduction from ICl₂⁻ to I₃⁻, two more Cl⁻ ions are released from the ICl₃, indicating Cl atoms accept two more electrons. The final step is a typical reduction reaction of I₃⁻ and I⁻. In short, the discharging process of the ICl₃ electrode is speculated as four steps:

step 1: ICl₃ + 2e⁻ → ICl₂⁻ + Cl⁻ (1)

step 2: ICl₂⁻ + Cl⁻ + e⁻ → 1/2 I₂Cl⁻ + 5/2 Cl⁻ (2)

step 3: 1/2 I₂Cl⁻ + 5/2 Cl⁻ + 1/3 e⁻ → 1/3 I₃⁻ + 3 Cl⁻ (3)

step 4: 1/3 I₃⁻ + 3 Cl⁻ + 2/3 e⁻ → I⁻ + 3 Cl⁻ (4)

In situ Raman measurements were performed to further explore the conversion mechanism (Fig. 3a and 3b). Figure 3a shows the G- and D-band change of the YP50 during the CV measurement at a scan rate of 0.5 mV s^− 1 (Fig. 3c). As the voltage increases, the widths of the G- and D-band of the YP50 increase, which can be explained by a superposition of charge transfer^{42, 43}. The intensive reaction in the YP50 host is further characterized by detecting various I and Cl species (Figures S11, S12). I₃⁻ species show a characteristic stretching band at 110 cm^− 1 (Fig. 3b)^44–46. During the anodic sweep, I₃⁻ species are detected after the voltage reaches 3.0 V. The first anodic peak in the voltage range of 3.0 to 3.2 V is attributed to the oxidation of I⁻ to I₃⁻. I₃⁻ species disappear when the voltage exceeds 3.5 V, implying that the second anodic peak from 3.5 to 3.8 V stems from the interhalogen reformation. From 3.5 to 4.0 V, we found a new stretching band at 174 cm^− 1 (Fig. 3d). The same stretching band was detected by dissolving ICl₃ into 1 M LiTFSI in DOL/DME (Figure S13), which therefore corresponds to the interhalogen bond between I and Cl. Figures 3e and 3f show a clear sequence of halogen oxidation. The intensity of the I₃⁻ band increases when the battery is charged from 2.5 V to 3.15 V, at which it reaches the highest value. As the charging process continues, I₃⁻ band intensity gradually decreases and almost disappears at 3.48 V due to the formation of the I-Cl interhalogen bond at 3.54 V (Fig. 3f). The intensity of the I-Cl band increases with charging, indicating that free Cl⁻ species are bound to I via interhalogen bonds. Anchoring the oxidized Cl⁻ to I is crucial for redox reversibility because, otherwise, the oxidized Cl- would form a gas and thus escape, as shown in Fig. 1c. The reformation of ICl₃ due to the strong interhalogen bond induces the highly reversible Cl^0/−1 redox reaction.

The interhalogen bonds between I and Cl are further evidenced by X-ray photoelectron spectroscopy (XPS), which reveals the valence state change of I and Cl at different voltages. I, Cl, and C are identified (Figure S14). I 3d peaks (Fig. 4a) are much stronger than that of Cl 2p at a fully discharged state of 2.0 V (Fig. 4b). This suggests that Cl is largely dissolved in the electrolyte, approaching the ideal case for the Cl^0/−1 redox reaction that Cl^− 1 is mobile for efficient utilization. Figure 4a also confirms the final discharge product of I⁻ as I3d_3/2 (630.1 eV) and I3d_5/2 (618.6 eV) are assigned to I^− 47. Meanwhile, we also observe residual bonded Cl with I: ICl at about 200.5 eV and ICl₃ at about 199.0 eV (Fig. 4b)⁴⁸. On the one hand, the residual ICl and ICl₃ indicate strong interhalogen bonding, which facilitates Cl fixation during oxidation. After charging to 3.2 V, I in a neutral valance state is observed, and its position is stable in the subsequent charge process (Fig. 4c)^{49, 50}. The formation of I in the neutral valance state is consistent with the interpretation from the Raman spectra that the first oxidation peak is attributed to the oxidation of I⁻ species. As the charging continues, a pair of strong peaks stemming from the interhalogen bonded I, and Cl (ICl and ICl₃) is observed (Fig. 4d). At the same time, the relative intensity of I is weakened, indicating the dominance of the interhalogen compounds after the reaction. Both results suggest the reformation of interhalogen compounds during the second oxidation peak. All in all, Raman and XPS spectra demonstrate the reversibility of breakage and reformation of interhalogen bonds, which allows for the mobile Cl⁻ for efficient redox reaction and inhibits the escape of Cl⁰ in the form of Cl₂ gas.

A full cell is assembled using the ICl₃ (in YP50) as the cathode and a lithium foil as the anode in a coin cell. The polypropylene/polyethylene/polypropylene (PP/PE/PP) three-layer separator (Celgard 2325) soaked with LiTFSI in the ether-solvent-based electrolyte is sandwiched by the two electrodes. Figure 5a shows CV curves at various scan rates, from 0.2 to 5 mV s^− 1. When the scan rate is less than 1 mV s^− 1, three prominent and one shoulder peaks are observed. However, the shoulder peak merges into a broad peak at around 3.3 V at the scan rate larger than 1 mV s^− 1, indicating the limited I₃⁻ formation. As a result, the reduction peak assigned to I₃⁻ reduction becomes weaker as the scan rates increase. In specific, at 1 mV s^− 1, the capacity contribution of I₃⁻ reduction (2.8 V) is 0.35, whereas the contribution decreases to 0.26 at 2 mV s^− 1. In addition, the position of cathodic peaks shifts to lower potentials. On the other hand, two anodic peaks are always observable while their positions move to higher potentials as scan rate increases. The expansion of the potential difference between cathodic and anodic peaks demonstrates the kinetic limitation of the reversible halogen conversions. Oxidation peak currents exhibit good linearity with the square root of scan rates (Figure S15). Thereby, the oxidation process is controlled by the diffusion of halogen ions in the pores of the YP50. The diffusion-controlled process can also be identified for the first cathodic peak (3.85 V)⁵¹. Nevertheless, the kinetics of the following reduction process is complex because the linear relationship deviates substantially at high scan rates.

Figure 5b shows the galvanostatic charge/discharge profiles at different current densities. At a low current density (425 mA g^− 1), a high specific capacity of 302 mAh g^− 1 is achieved. When the current density increases by around 3 times (1250 mA g^− 1), the capacity is retained at 223 mAh g^− 1, indicating excellent rate performance. More importantly, three characteristic discharge plateaus are observed at all current densities. Figure 5c compares the capacity contributions of these three discharge plateaus at different current densities. The overall capacity is normalized to 1. A noticeable decrease in capacity contribution from the 3.85 V plateau is observed when the current density reaches 625 mA g^− 1, revealing that the kinetic extraction of first Cl from ICl₃ is slower than the other reactions. As the current density increases to 1250 mA g^− 1, the I₃⁻ reduction is limited. By contrast, the intermediate processes (3.4 V plateau) are relatively independent of the current density. This suggests that the process from ICl₂⁻ to I₃⁻ is fast both kinetically and thermodynamically. The cycling of Li-ICl₃ full cell is carried out at a current density of 750 mA g^− 1 (Fig. 5d). A reversible discharge capacity of 271 mAh g^− 1 is obtained, and 64% of this initial capacity is retained over 200 cycles.

We compare the power and energy density of the ICl₃ electrode to other reported cathode materials (Fig. 5e and Table S1). The I₂ based lithium-ion batteries show a good rate performance as the energy density is stable while the power density increases. However, owing to the limited one-electron transfer, its energy density is much lower than the ICl₃ based batteries. Although the Br₂ based lithium-ion batteries can deliver an energy density close to our ICl₃ based batteries, their power density is about one order of magnitude lower. At a high power density of 4225 W kg^− 1, the energy density of ICl₃ can reach 754 Wh kg^− 1. Moreover, as shown in Fig. 5f, the maximum working voltage of the ICl₃ battery is about 3.85 V, much higher than the I₂ (3.0 V) and Br₂ (3.3 V) based batteries. Besides the improved performance against conventional halogen-based lithium-ion batteries (I₂ and Br₂)^{52, 53}, the ICl₃ demonstrates superior performance beyond the conventional cathode materials of lithium-ion batteries. The maximum energy density of 1024 Wh kg^− 1 of ICl₃ cannot be achieved by intercalation-type cathode materials (LiCoO₂ and NMC)^54–56. Furthermore, the achievable power density of ICl₃ is almost two orders of magnitude higher at the same energy density of intercalated cathode materials, such as the NMC. In addition to the power and energy density, the ICl₃ marks the highest attainable working voltage among cathode materials for lithium-ion batteries (Fig. 5f). It is worth noting that the voltage of the ICl₃ based batteries is even slightly higher than for LiMn₂O₄, which is well-known for its high operating voltage.

In summary, for the first time, we demonstrate a direct halogen cathode showing high reversibility without using an intermediary material in the cathode. The ICl₃ cathode approaches the ideal cathode for Li-Cl₂ batteries due to the partial solubility of Cl⁻ in the ether or ester electrolytes from reduced ICl₃ and the effective fixation of oxidized Cl⁰ by interhalogen bonds to I. More importantly, the breakage and reformation of interhalogen bonds between I and Cl are highly reversible, thus allowing for good cycling stability of 200 cycles. The rechargeable Li-Cl₂ battery delivers a capacity of 302 mAh g^− 1 at 425 mA g^− 1 and therefore, a high energy density of 1024 Wh kg^− 1. At a high current density of 1250 mA g^− 1, corresponding to a high power of 4225 W kg^− 1, an energy density of 754 Wh kg^− 1 remains. The successful use of ICl₃ in a rechargeable lithium-ion battery paves a new way to develop energy-dense and high-power halogen-based cathode materials. New electrolyte and electrode compositions are expected to optimize the reaction kinetics further, thus unleashing the full capacity of ICl₃ (459 mAh g^− 1).

Chemicals and battery components. All chemicals are used directly without any post-treatment. Iodine trichloride (ICl₃, 97%, Aladdin), Lithium chloride (LiCl, 99.9%, Aladdin), Tetrabutylammonium chloride (TBACl, ≥ 99.0%, Aladdin), Sodium chloride (NaCl, 99.9%, Aladdin), iodine (I₂, 99.5%, Aladdin), activated carbon (YP50, Kuraray Chemical), bis (trifluoromethane) sulfonimide lithium salt (LiTFSI, 99%, Aladdin), ethanol (C₂H₅OH, 99.5%, Aladdin), dimethoxyethane (DME, 99%, Aladdin), dioxolane (DOL, 99%, Aladdin), Ethylene carbonate (EC, 99%, Aladdin), Dimethyl carbonate (DMC, 99%, Aladdin), Ethyl Methyl Carbonate (EMC, 99%, Aladdin), poly (vinylidene 470 fluoride) (PVDF, average Mw ~ 400000, Aladdin), nmethyl-2-pyrrolidone (NMP, 99%, Aladdin), ketjenblack (KB, ECP-600JD, Lion Corporation).

Preparation of ICl ₃ electrode and electrolytes. For the ICl₃ cathode, YP50 powder, ketjenblack (KB), and PVDF were mixed in N-Methylpyrrolidone solvent with a mass ratio of 8:1:1, followed by vigorously stirring for 20 minutes. Next, the slurry was coated on a titanium foil, and dried at 70 ºC in a vacuum oven for 24 h. Then YP50 disks and ICl₃ were put into a glass reactor in a glove box filled with Ar atmosphere. The reactor was then sealed for static adsorption for 12 h. ICl₃ loading (~ 70 wt%) was measured by subtracting the mass of pure YP50 from the YP50 with ICl₃ loading.

The ether electrolyte was fabricated by dissolving 1 M lithium LiTFSI salts and trace LiCl (< 0.05M) into the mixture of DOL and DME solvents with a volume ratio of 1:1 in a glove box filled with Ar atmosphere. The ether electrolyte used was fabricated by dissolving 1 M lithium LiPF₆ salts into the mixture of EC, DMC and EMC solvents with a volume ratio of 1:1:1 in a glove box filled with Ar atmosphere.

Preparation of TBACl, LiCl and NaCl electrodes. The YP50 disks were prepared as above. For Air sensitive TBACl or LiCl, TBACl or LiCl was dissolved in alchohol and the solution was dropped onto the YP50 electrodes using a pipet. Filling TBACl/LiCl was repeated several times. The electrodes were then heated at 150°C for 1 h. For the NaCl cathode, NaCl, ketjenblack (KB) and PVDF were mixed in N-Methylpyrrolidone solvent with a mass ratio of 8:1:1, followed by vigorously stirring for 20 minutes. Then the slurry was coated to a titanium foil and dried at 70 ºC in a vacuum oven for 24 h.

Preparation of I ₂ electrode. I₂@AC was prepared through a melt-diffusion method. The YP50 was mixed with acetylene black and poly (vinylidene fluoride) at a weight ratio of 8:1:1 and then coated onto carbon cloth (CC). After drying in a vacuum oven, the YP50 disk and iodine were put into a stainless reactor. Then the reactor was then sealed and heated to 135°C for 12 h.

Electrochemical measurements. The CR2032 coin-type battery was assembled for electrochemical measurements. Galvanostatic charge/discharge profiles were recorded by LAND CT2001A battery testing device. CHI 760E multichannel electrochemical workstation was employed to record the cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) data. Li foil was used as the anode. Specific capacities were calculated based on the mass of iodine trichloride.

Materials Characterization. The morphology and microstructure were characterized by the cold field emission scanning electron microscope (SEM; SU4800, Hitachi). Raman spectroscopy (WITec alpha300 access) equipped with a laser of 532 nm wavelength was performed to record the chemical changes. A coin cell with a quartz window on the positive shell was used for in situ Raman spectroscopy analysis. X-ray photoelectron spectroscopy (XPS; ESCALAB 250) was conducted to analyze surface compositions. Nitrogen adsorption measurement was conducted at 77 K using a Micromeritics ASAP 2460 instrument (Micromeritics Instrument Corp., America). Pore volume was calculated at a relative pressure P/P0 = 0.990, the specific surface area was obtained by Brunauer-Emmett-Teller (BET) analyses of the adsorption isotherm and the pore size distribution was calculated using density functional theory (DFT).

Density functional theory (DFT) calculations. All the computations were conducted based on the density functional theory (DFT) using the Cambridge Sequential Total Energy Package (CASTEP) code of the Materials Studio software. The generalized gradient approximation (GGA) with the Perdew-Burke-Ernzerhof (PBE) functional were used to describe the electronic exchange and correlation effects. The kinetic-energy cutoff was set as 500 eV. The geometry optimization within the conjugate gradient method was performed with forces on each atom less than 0.05 eV/Å. Additionally, the converge thresholds for energy and force were set to 10^− 5 eV and 0.02 eV/Å, respectively. Brillouin zone was sampled by a y a k-point mesh of 1 × 1 × 1. We computed the Gibbs free energy change (∆G) of intermediates to predict the reaction path. The ∆G was calculated as:

ΔG = E(gse) \(+\) E(zpe) \(–\) T∆S

where E(gse), E(zpe) and TΔS were the ground-state energy, zero-point energy and entropy term, respectively, with the latter two taking vibration frequencies from the density functional theory (DFT) calculation. T is set to 298.15 K. The free-energy (ΔG) of different intermediates were also defined as:

ΔG = E(intermediate) – E(reactant)

where the E(intermediate) was the energy of intermediates and E(reactant) was the total energy of reactants ICl₃.

Data availability

The data that support the findings of this study are available within the text including the Methods, and Supplementary information. Raw datasets related to the current work are available from the corresponding author on reasonable request.

Acknowledgments

This research was supported by GRF under Project CityU 11304921.

Author contributions

C.Z. and M. Z. conceived the idea and designed the experiments. C.Z. and P.L. directed the research. X.L., A.C., R.Z., Y.H., and H.C. conducted the material characterization and electrochemical measurements. Z.H., Y.W., Z.C., J. Z., and P.L. assisted with the electrochemical measurements and data analysis. P.L. and Y.G. conducted the DFT calculations. P.L., C.Z. and M. Z. co-wrote the manuscript. All authors discussed and analyzed the results.

Competing Interests

The authors declare no conflicts.

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An Energy-Dense and High-Power Li-Cl2 Battery by Reversible Interhalogen Bonds

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