Li-CO2 Batteries Research Articles

Enhanced Co3O4 Nanoflakes Reactivity via Integrated Al-Doping and Metal Vacancy Engineering for Large Capacity Li-CO2 Batteries

Rechargeable Li-CO2 batteries are well-regarded for their high-energy, environmental friendliness, and resourceful use of CO2, but suffer from poor cycle reversibility. Herein, Al-doped Co3O4 nanoflakes featuring abundant metal vacancies (V-ACO/CC) were synthesized via a facile approach employing Al ions as both a dopant and sacrificial agents, which serve as high-efficient cathode catalyst for Li-CO2 batteries. Experiment results demonstrate that the incorporation of Al doping and metal vacancies modulates the electronic structure of Co-center and optimizes the growth path of discharge product. The cation vacancies generated by the sacrificed part of the Al atoms change the local charge distribution, strengthen the affinity of CO2 and reaction intermediates and facilitate the reversible decomposition of discharge products. Concurrently, the formation of covalent Al-O bonds by the remaining Al species reinforces the stability of nanostructures. Notably, the V-ACO/CC-based LCBs exhibit enhanced CO2 conversion kinetics, as evidenced by a high specific capacity (12.06 mAh cm−2 at 0.05 mA cm−2), fast rate capability and impressive stability (over 420 cycles under 0.1 mA cm−2).

Multi-scale synergistic regulation of hierarchical porous Ni@NiSe cathodes with low voltage gap, high capacity and long-term cycling stability in Li–CO2 battery

Multi-scale synergistic regulation of hierarchical porous Ni@NiSe cathodes with low voltage gap, high capacity and long-term cycling stability in Li–CO2 battery

Laser Precise Synthesis of Oxidation-Free High-Entropy Alloy Nanoparticle Libraries.

High-entropy alloy nanoparticles (HEA-NPs) show exceptional properties and great potential as a new generation of functional materials, yet a universal and facile synthetic strategy in air toward nonoxidized and precisely controlled composition remains a huge challenge. Here we provide a laser scribing method to prepare single-phase solid solution HEA-NPs libraries in air with tunable composition at the atomic level, taking advantage of the laser-induced metastable thermodynamics and substrate-assisted confinement effect. The three-dimensional porous graphene substrate functions as a microreactor during the fast heating/cooling process, which is conductive to the generation of the pure alloy phase by effectively blocking the binding of oxygen and metals, but is also beneficial for realizing accurate composition control via microstructure confinement-endowed favorable vapor pressure. Furthermore, by combining an active learning approach based on an adaptive design strategy, we discover an optimal composition of quinary HEA-NP catalysts with an ultralow overpotential for Li-CO2 batteries. This method provides a simple, fast, and universal in-air route toward the controllable synthesis of HEA-NPs, potentially integrated with machine learning to accelerate the research on HEAs.

Sabatier principle guiding the design of cathode catalysts for Li-CO2 batteries

The Sabatier principle has been widely used for designing electrocatalysts for energy conversion applications, but it is rarely mentioned in the research of cathode catalyst of Li-CO2 batteries. In our work, the “volcanic” relationship between the catalytic activity and the adsorption energy of the catalyst to the intermediates is first demonstrated based on the first-principles calculation, which meets the Sabatier principle and can be used to design the cathode catalysts. The increases in the number of nitrogen-vacancy in WN shift the d-band center and increase the interaction with the reactants. The catalytic activity increases first and then decreases with the increase of adsorption energy, which was proved in the experiment. The optimal catalyst for moderate adsorption of intermediate makes the thin Li2CO3 distribute evenly. It exhibits a median voltage difference of 0.68 V and an energy efficiency of 84.33% at 20 μA cm−2 with a limited capacity of 200 μA h cm−2.

Unlock CO2 Reduction Reaction Pathways in Aprotic Li-CO2 Batteries with In Situ Isotope-Labeled Spectroscopy and Theoretical Calculations.

The CO2 reduction reaction (CO2RR) pathway significantly dictates the reversibility and overpotential of aprotic Li-CO2 batteries; however, it has remained incompletely understood due to the lack of direct in situ spectroscopic evidence. Herein, the Li-CO2RR pathways at the model Au | dimethyl sulfoxide (DMSO) interface are interrogated using a combination of in situ isotope-labeled spectroscopy techniques and theoretical calculations. This obtained direct spectroscopic evidence presents that the primary CO2RR proceeds through the CO2-to-CO pathway (i.e., 2Li+ + 2CO2 + 2e- → CO + Li2CO3) initiated at a low overpotential (ca. 2.1 V vs Li/Li+), and the CO2-to-Li2C2O4 pathway (i.e., 2Li+ + 2CO2 + 2e- → Li2C2O4) initiated at a high overpotential (ca. 1.7 V vs Li/Li+), where the potential-dependent pathways critically depend on the coverage of LiCO2 intermediates. Simultaneously, the entire Li-CO2RR process is also accompanied by parasitic reactions to form gaseous C2H4 with COOH* as the crucial intermediate, which is induced by the H+-abstraction reaction between the reactive LiCO2 intermediate and the DMSO solvent. These fundamental insights enable us to establish a molecular picture for Li-CO2RR pathways in aprotic media and will serve as a crucial guideline for reversible Li-CO2 electrochemistry.

Li1.4Al0.4Ge0.1Ti1.5(PO4)3: A stable solid electrolyte for Li-CO2 batteries

In this study, a solid electrolyte, Li1.4Al0.4Ge0.1Ti1.5(PO4)3 (LAGTP), with a sodium superionic conductor-type crystal structure, was prepared using a facile solution-based method. LAGTP exhibited exceptional ionic conductivity (1.05 × 10−3 S cm−1) and a low activation energy (0.237 eV). The LAGTP pellet was employed as a solid-state electrolyte in a Li-CO2 battery, showcasing charge-discharge characteristics via a reversible electrochemical reaction (4Li+ + 3CO2 ↔ 2Li2CO3 + C). As-synthesized multi-walled carbon nanotubes, drop-cast on carbon cloth, were used as the cathode. The battery underwent 60 cycles with a cut-off capacity of 1000 mAh g−1 at various current densities, and a full-depth charge and discharge test was conducted at 100 mA g−1. During the charge/discharge process, the particle size of the dead lithium increased on the cathode surface, leading to the blockage of active sites for conversion. Post-cycling analyses were performed to elucidate the cathode degradation mechanism. The incorporation of LAGTP significantly enhanced battery cycle life and safety, making it a suitable candidate for use in next-generation, high-performance Li-CO2 batteries.

Imidazolium bromide based dual-functional redox mediator for the construction of dendrite-free Li-CO2 batteries

Rechargeable lithium-carbon dioxide (Li-CO2) batteries have emerged as a highly promising approach to simultaneously address energy shortages and the greenhouse effect. However, certain limitations exist in Li-CO2 batteries like high charge overpotential and unstable Li metal interface, which adversely affect the energy efficiency and cycling life. The incorporation of soluble redox mediators (RMs) has proven effective in enhancing the charge transfer between lithium carbonate (Li2CO3) and cathode, thereby substantially reducing the charge overpotential. Nevertheless, the severe shuttle effect of RMs results in the reactions with Li anode, not only exacerbating the corrosion of Li anode but also leading to the depletion of RMs and electrical energy efficiency. In this work, an organic compound containing large cation group, 1-ethyl-3-methylimidazole bromide (EMIBr) is proposed as the defense donor RM for Li anode in Li-CO2 batteries to address the above problems simultaneously. During charging, Li2CO3 oxidation kinetics can be accelerated by bromide anion pair (Br3−/Br−). Meanwhile, the cations (EMI+) are preferentially adsorbed around the protruding tips of Li anode through electrostatic interaction driven by surface free energy, forming protective layers that effectively inhibit further Li deposition at these tips, which is verified by DFT calculations. Additionally, Li dendrites growth is inhibited by the electrostatic repulsion of polar groups in EMIBr, resulting in uniform Li deposition. Consequently, a lower overpotential (∼1.17 V) and a longer cycle life (∼200 cycles) have been obtained for Li-CO2 battery incorporating EMIBr.

Improving the Rechargeable Li-CO2 Battery Performances by Tailoring Oxygen Defects on Li-Ni-Co-Mn Multi-Metal Oxide Catalysts Recycled from Spent Ternary Lithium-Ion Batteries.

Rechargeable Li-CO2 batteries are considered as a promising carbon-neutral energy storage technology owing to their ultra-high energy density and efficient CO2 capture capability. However, the sluggish CO2 reduction/evolution kinetics impedes their practical application, which leads to huge overpotentials and poor cyclability. Multi-element transit metal oxides (TMOs) are demonstrated as effective cathodic catalysts for Li-CO2 batteries. But there are no reports on the integration of defect engineering on multi-element TMOs. Herein, the oxygen vacancy-bearing Li-Ni-Co-Mn multi-oxide (Re-NCM-H3) catalyst with the α-NaFeO2-type structure is first fabricated by annealing the NiCoMn precursor that derived from spent ternary LiNi0.8Co0.1Mn0.1O2 cathode, in H2 at 300°C. As demonstrated by experimental results and theory calculations, the introduction of moderate oxygen vacancy has optimized electronic state near the Fermi level (Ef), eventually improving CO2 adsorption and charge transfer. Therefore, the Li-CO2 batteries with Re-NCM-H3 catalyst deliver a high capacity (11808.9 mAh g-1), a lower overpotential (1.54V), as well as excellent stability over 216 cycles at 100mA g-1 and 165 cycles at 400mA g-1. This study not only opens up a sustainable application of spent ternary cathode, but also validates the potential of multi-element TMO catalysts with oxygen defects for high-efficiency Li-CO2 batteries.

N, S Co-doped carbon anchored Co9S8 cathode: Advancing sustainable energy through efficient Li–CO2 Mars batteries

Owing to their higher capacity and ability to address global warming, Li–CO2 batteries have potential for next-generation energy storage systems on Earth and for space applications. However, the key drawbacks of high overpotential and low cyclability of Li–CO2 batteries substantially hinder their practicality. In this study, we develop uniquely designed cobalt sulfide (Co9S8) nanoparticles anchored onto the N, S dual-doped hetero atoms graphitized mesoporous carbon (NSC) as a low-cost but highly effective cathodic catalyst for Li–CO2 batteries with a large number of active sites with enhanced conductivity. The as-developed Li–CO2 batteries under simulated Martian gas atmosphere conditions (Li–CO2 Mars) display a high discharge capacity and exceptional rate performance. The Li–CO2 Mars battery offers a high discharge capacity of 15147 mAh g−1 at 500 mA g−1 current density and maintains a stable performance over 120 cycles for a limited capacity of 500 mAh g−1. Further, the first-principle calculations provide a deeper understanding of the reaction pathways during discharging and charging. These results create new avenues for designing novel catalysts for high-performance Li–CO2 Mars batteries for their use in interplanetary missions.

Ultrafine Ru nanoparticles anchored on N-doped mesoporous hollow carbon spheres as a highly efficient bifunctional catalyst for Li–CO2 batteries

Rechargeable Li–CO2 battery is a facilitative and promising device for the conversion of CO2 to electrochemical energy. However, it remains a challenge to enhance the sluggish decomposition kinetics of lithium carbonate as the discharge product. Herein, the Ru nanoparticles anchored on N-doped mesoporous hollow carbon nanospheres (Ru-AHCNs) are designed as cathode to enhance the electrochemical performance of Li–CO2 battery. The Ru-AHCNs cathode displays a high discharge specific capacity of 11194.4 mA h g−1 at the current density of 100 mA g−1. In addition, the Ru-AHCNs cathode can stably run over 50 cycles and maintain a small overpotential (<1.38 V) with a limited capacity of 1000 mA h g−1 at 100 mA g−1. The excellent stability and catalytic activity of the cathode are ascribed to the following factors: (i) Uniform deposition of Ru nanoparticles in hollow carbon nanospheres can enhance the decomposition of Li2CO3 and provide considerable exposure to active sites. (ii) N-doped mesoporous hollow carbon nanospheres can provide abundant electron transport channels and promote the nucleation of discharge products. These results evidently prove the reversible formation and decomposition of the discharge products, indicating that Ru-AHCNs cathode possesses excellent bifunctional catalytic activity.

Nano-interface engineering of NiFe2O4/MoS2/MWCNTs heterostructure catalyst as cathodes in the Long-Life reversible Li-CO2 Mars batteries

Lithium-CO2 batteries, a potential next-generation negative emission technology, are advanced energy storage devices with considerable interest in carbon neutrality for developing a sustainable environment. Additional challenges arise from the slow kinetics with poor reversibility in cycling performance and high overpotential of these batteries, limiting the further development of this technology toward large-scale implementation. Herein, we construct a NiFe2O4/MoS2/MWCNTs heterostructure nanomaterial catalyst as a cathode for Li-CO2 batteries function in the simulated Martian atmosphere (Li-CO2 Mars). The Li-CO2 Mars batteries with the proposed cathode exhibit excellent efficiency with a high discharge capacity of 26533.5 mAh g−1, a discharge plateau at ∼ 2.68 V, and high stability over 195 and 115 cycles with a limited capacity of 500 and 1000 mAh g−1, respectively. Computational studies demonstrate that improved CO2 adsorption with favorable discharge product growth using the heterostructure catalyst promotes the exceptional performance of the Li-CO2 Mars batteries consistent with the ex-situ experimental studies. The outcome of this study offers a novel approach to the design and construction of efficient multifunctional electrocatalysts, which can be used to develop sustainable and clean energy systems for both Earth and Mars missions.

Redox Molecular Junction Metal-Covalent Organic Frameworks for Light-assisted CO2 Energy Storage.

Visible-light sensitive and bi-functionally favored CO2 reduction (CRR)/evolution (CER) photocathode catalysts that can get rid of the utilization of ultraviolet light and improve sluggish kinetics is demanded to conquer the current technique-barrier of traditional Li-CO2 battery. Here, a kind of redox molecular junction sp2c metal-covalent organic framework (i.e. Cu3-BTDE-COF) has been prepared through the connection between Cu3 and BTDE and can serve as efficient photocathode catalyst in light-assisted Li-CO2 battery. Cu3-BTDE-COF with redox-ability, visible-light-adsorption region, electron-hole separation ability and endows the photocathode with excellent round-trip efficiency (95.2 %) and an ultralow voltage hysteresis (0.18 V), outperforming the Schiff base COFs (i.e. Cu3-BTDA-COF and Cu3-DT-COF) and majority of the reported photocathode catalysts. Combined theoretical calculations with characterizations, Cu3-BTDE-COF with the integration of Cu3 centers, thiazole and cyano groups possess strong CO2 adsorption/activation and Li+ interaction/diffusion ability to boost the CRR/CER kinetics and related battery property.

Catalytic role of in-situ formed C-N species for enhanced Li2CO3 decomposition

Sluggish kinetics of the CO2 reduction/evolution reactions lead to the accumulation of Li2CO3 residuals and thus possible catalyst deactivation, which hinders the long-term cycling stability of Li-CO2 batteries. Apart from catalyst design, constructing a fluorinated solid-electrolyte interphase is a conventional strategy to minimize parasitic reactions and prolong cycle life. However, the catalytic effects of solid-electrolyte interphase components have been overlooked and remain unclear. Herein, we systematically regulate the compositions of solid-electrolyte interphase via tuning electrolyte solvation structures, anion coordination, and binding free energy between Li ion and anion. The cells exhibit distinct improvement in cycling performance with increasing content of C-N species in solid-electrolyte interphase layers. The enhancement originates from a catalytic effect towards accelerating the Li2CO3 formation/decomposition kinetics. Theoretical analysis reveals that C-N species provide strong adsorption sites and promote charge transfer from interface to *CO22− during discharge, and from Li2CO3 to C-N species during charge, thereby building a bidirectional fast-reacting bridge for CO2 reduction/evolution reactions. This finding enables us to design a C-N rich solid-electrolyte interphase via dual-salt electrolytes, improving cycle life of Li-CO2 batteries to twice that using traditional electrolytes. Our work provides an insight into interfacial design by tuning of catalytic properties towards CO2 reduction/evolution reactions.

Mild oxidation regulating the surface of Mo2CTx MXene to enhance catalytic activity for low overpotential and long cycle life Li-CO2 batteries

The lithium-carbon dioxide (Li-CO2) batteries hold promise for energy storage, given their capacity to capture and convert carbon dioxide (CO2). However, the practical application of Li-CO2 batteries continues to face substantial obstacles caused by sluggish CO2 reduction/evolution kinetics, resulting in high overpotential and short lifespan. This work presents the fabrication of a highly effective MoO2@Mo2C heterostructure hybrid catalyst using a CO2 oxidation strategy. This strategy integrated (in-situ) MoO2 onto the surface of two-dimensional (2D) Mo2C MXene, enhancing catalytic activity while preserving 2D electron/ion pathways. As a result, the MoO2@Mo2C, when used as a catalyst in Li-CO2 battery showcased a discharge capacity of 20790.8 mAh g−1 at a current density of 200 mA g−1. Notably, it achieved a long cycling life of 230 cycles at a cutoff capacity of 1000 mAh g−1 with a voltage gap as low as 1.85 V, which was significantly superior to that of a pristine Mo2CTx catalyst (3.61 V after twenty cycles). This work provides critical insights into the design of MXenes-based high-performance catalysts for advanced Li-CO2 batteries.

High-Efficiency Rechargeable Fe-CO2 Battery: A Route for Effective CO2 Conversion and Energy Storage.

Because of their high theoretical energy density, metal-CO2 batteries based on Li, Na, or K have attracted increasing attention recently for meeting the growing demands of CO2 recycling and conversion into electrical energy. However, the scarcity of active anode material resources, high cost, as well as safety concerns of Li, Na, and K create obstacles for practical applications. Herein, we demonstrate for the first time a high-efficiency (η = 77.2%) rechargeable Fe-CO2 battery that is composed of iron (Fe) anode and MoS2-catalysts deposited carbon cathode. MoS2 catalysts are crucial to the successful acceleration of reaction kinetics of Fe during charge and discharge with a minimum overpotential of the cell. The Fe-CO2 cell has a higher initial specific capacity of 12,500 mA h g-1 with an average discharge potential of 0.65 V and operates reversibly with a lower overpotential than that of Li-CO2 batteries with a cutoff capacity of 500 mA h g-1. Our Fe-CO2 battery can effectively convert CO2 greenhouse gas into electrical energy by consuming 1 ton of CO2 with usage of 1.23 tons of iron.

Revealing the Indispensable Role of In Situ Electrochemically Reconstructed Mn(II)/Mn(III) in Improving the Performance of Lithium-Carbon Dioxide Batteries.

Li-CO2 batteries are regarded as promising high-energy-density energy conversion and storage devices, but their practicability is severely hindered by the sluggish CO2 reduction/evolution reaction (CORR/COER) kinetics. Due to the various crystal structures and unique electronic configuration, Mn-based cathode catalysts have shown considerable competition to facilitate CORR/COER. However, the specific active sites and regulation principle of Mn-based catalysts remain ambiguous and limited. Herein, this work designs novel Mn dual-active sites (MOC) supported on N-doped carbon nanofibers and conduct a comprehensive investigation into the underlying relationship between different Mn active sites and their electrochemical performance in Li-CO2 batteries. Impressively, this work finds that owing to the in situ generation and stable existence of Mn(III), MOC undergoes obvious electrochemical reconstruction during battery cycling. Moreover, a series of characterizations and theoretical calculations demonstrate that the different electronic configurations and coordination environments of Mn(II) and Mn(III) are conducive to promoting CORR and COER, respectively. Benefiting from such a modulating behavior, the Li-CO2 batteries deliver a high full discharge capacity of 10.31 mAh cm-2, and ultra-long cycle life (327 cycles/1308h). This fundamental understanding of MOC reconstruction and the electrocatalytic mechanisms provides a new perspective for designing high-performance multivalent Mn-integrated hybrid catalysts for Li-CO2 batteries.

Unique Hierarchically Structured High-Entropy Alloys with Multiple Adsorption Sites for Rechargeable Li-CO2 Batteries with High Capacity.

Lithium-carbon dioxide (Li-CO2) batteries offer the possibility of synchronous implementation of carbon neutrality and the development of advanced energy storage devices. The exploration of low-cost and efficient cathode catalysts is key to the improvement of Li-CO2 batteries. Herein, high-entropy alloys (HEAs)@C hierarchical nanosheet is synthesized from the simulation of the recycling solution of waste batteries to construct a cathode for the first time. Owing to the excellent electrical conductivity of the carbon material, the unique high-entropy effect of the HEAs, and the large number of catalytically active sites exposed by the hierarchical structure, the FeCoNiMnCuAl@C-based battery exhibits a superior discharge capability of 27664 mAh g-1 and outstanding durability of 134 cycles as well as low overpotential with 1.05V at a discharge/recharge rate of 100mA g-1. The adsorption capacity of different sites on the HEAs is deeply understood through density functional theory calculations combined with experiments. This work opens up the application of HEAs in Li-CO2 batteries catalytic cathodes and provides unique insights into the study of adsorption active sites in HEAs.

Strong electronic coupling of NiCo2O4 and CeO2 regulates the nucleation and decomposition of Li2CO3 for high-rate performance Li–CO2 batteries

The sluggish CO2 reduction/evolution kinetics at the cathode severely hamper the industrial applications of Li–CO2 batteries, especially under large current densities. Herein, NiCo2O4/CeO2 with a strong electron coupling effect is prepared via solvothermal method and calcination to realize the rapid kinetics of discharge and charge processes. The electronic character of the catalyst and the growth behavior of Li2CO3 are investigated through density functional theory (DFT) and experiments, elucidating the reaction mechanism of Li–CO2 battery. The results demonstrate that the strong electronic coupling of NiCo2O4 and CeO2 enhances the intrinsic activity of the catalyst and promotes the generation of membrane-like Li2CO3 with good reversibility, thereby enhancing battery performance at a large current density. Consequently, NiCo2O4/CeO2 achieved a large specific capacity of 7767 mAh g−1 under 2000 mA g−1 and could be stably cycled more than 240 times, outperforming most reported metal-based catalysts. This work underscores the important role of strong electronic coupling in facilitating the formation and decomposition of Li2CO3, providing valuable insight for designing cathode catalysts with high-rate properties for Li–CO2 batteries.

Metal-Free Electron Donor-Acceptor Pair Enabled Long-Term Stability of Li-CO2 Battery.

The challenges of Lithium-carbon dioxide (Li-CO2) batteries for ensuring long-term cycling stability arise from the thermodynamically stable and electrically insulating discharge products (e.g., Li2CO3), which primarily rely on their interaction with the active materials. To achieve the optimized intermediates, the bifunctional electron donor-acceptor (D-A) pairs are proposed in cathode design to adjust such interactions in the case of B-O pairs. The inclusion of BC2O sites allows for the optimized redistribution of electrons via p-π conjugation. The as-obtained DO-AB pairs endow the enhanced interactions with Li+, CO2, and various intermediates, accompanied by the adjustable growth mode of Li2CO3. The shift from solvation-mediated mode into surface absorption mode in turn manipulates the morphology and decomposition kinetics of Li2CO3. Therefore, the corresponding Li-CO2 battery got twofold improved in both the capacity and reversibility. The cycling prolongs exceed 1300h and well operates at a wide temperature range (20-50°C) and different folding angles (0-180°). Such a strategy of introducing electron donor-acceptor pairs provides a distinct direction to optimize the lifetime of Li-CO2 battery from local structure regulation at the atomic scale, further inspiring in-depth understandings for developing electrochemical energy storage and carbon capture technologies.

Compositionally engineered NiCoLDH@rGO as bifunctional cathode catalyst for rechargeable Li-O2/Li-CO2 battery

Compositionally tuned nickel-cobalt layered double hydroxides (NCLDHs) and NCLDH@reduced graphene-oxide (NCLDH@rGO) were synthesized through a facile solvothermal synthesis route. The formation of the synthesized NCLDH and the NCLDH@rGO with the intercalated carbonate and nitrate anions, has been confirmed utilizing different characterization techniques. Microscopic results revealed the flaky morphology with thickness about 30 nm. Rotating ring disc electrode (RRDE) voltammetry was utilized to analyze the oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and carbon dioxide reduction reaction (CO2RR) kinetics on each of the pristine (1:1), (2:1), (3:1) and (4:1) NCLDH catalysts and the NCLDH@rGO composites. The RRDE data revealed that the electrochemical activity towards ORR/OER/CO2RR could be largely increased by tuning mole ratio of the (Ni2+/Co3+) or the amount of the rGO in the NCLDH. It turned out that among the pristine electrocatalysts, the (1:1) NCLDH catalyst exhibited enhanced ORR/OER kinetics. While the NCLDH acted as a catalyst center, the rGO provided conductive network that facilitated passable overpotential with increased current density for the ORR/OER/ CO2RR. Better adsorption of O2 and CO2 on the NCLDH@rGO catalyst also contributed for the electrocatalytic activity. Consequently, the NCLDH@rGO composites as cathode catalyst for Li-O2 battery in the CR2032 prototype coin-cell exhibited a stable open circuit voltage (OCV). Among the NCLDH@rGO composites, the NCLDH with 15 wt.% rGO (NCRGO15) exhibited a high discharge capacity of 3616 mAh g−1 at 50 Ag−1 for the Li-O2 battery and a discharge capacity of 45 mAh g−1 at a current density of 100 Ag−1 for the CR2032 coin-type Li-CO2 battery. As a practical use, a commercial 2.8 V green LED bulb was lit continuously for about 20 h using the fabricated Li-O2 battery that consisted of lithium anode and (1:1) NCLDH@rGO15 wt.% (NCRGO15) air-breathing cathode.