Lithium Carbon Dioxide Research Articles

Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO2 and Li-Air Batteries.

Lithium-carbon dioxide (Li-CO2) and Li-air batteries hold great potential in achieving carbon neutral given their ultrahigh theoretical energy density and eco-friendly features. However, these Li-gas batteries still suffer from low discharging-charging rate and poor cycling life due to sluggish decomposition kinetics of discharge products especially Li2CO3. Here we report the theory-guided design and preparation of unconventional phase metal heteronanostructures as cathode catalysts for high-performance Li-CO2/air batteries. The assembled Li-CO2 cells with unconventional phase 4H/face-centered cubic (fcc) ruthenium-nickel heteronanostructures deliver a narrow discharge-charge gap of 0.65 V, excellent rate capability and long-term cycling stability over 200 cycles at 250 mA g-1. The constructed Li-air batteries can steadily run for above 150 cycles in ambient air. Electrochemical mechanism studies reveal that 4H/fcc Ru-Ni with high-electroactivity facets can boost redox reaction kinetics and tune discharge reactions towards Li2C2O4 path, alleviating electrolyte/catalyst failures induced by the aggressive singlet oxygen from solo decomposition of Li2CO3.

Li2CO3/LiF-Rich Solid Electrolyte Interface Stabilized Lithium Metal Anodes for Durable Li-CO2 Batteries

Lithium carbon dioxide (Li-CO2) batteries are considered a promising next-generation energy storage device due to their high theoretical energy density and potential carbon neutralization. Despite numerous iterative advancements in cathode catalysts for Li-CO2 batteries, the cycling stability still to be hindered by the growth of lithium dendrites during cycling, primarily due to uneven deposition and the side reaction of sufficient CO2 with the Li metal anode. In this work, bisalt electrolyte (BE) consisting of LiPF6 and LiTFSI is used as a localized anode surface stabilizer to achieve durable Li-CO2 batteries. The introduction of PF6− promotes the decomposition and reduction of TFSI−, leading to the formation of LiF-rich inorganic SEI (Li2CO3/LiF-rich) with enhanced Li+ affinity and good electronic insulating properties. This effectively inhibits lithium dendrite formation while also insulating CO2 and electrolytes from contacting the lithium anode. Consequently, the Li symmetric battery incorporating the novel BE exhibits a long cycling life of 912 hours (∼3.8 times of the cell with a single-salt electrolyte (SE)). The BE based Li-CO2 battery achieves an ultra-long cyclelife of 2720 hours (∼2.6 times of SE battery) and outstanding rate capability. In addition, the assembled belt-shaped Li-CO2 batteries could stably power a digital watch for 1267 hours.

Creating CoRu Dual Active Sites Codecorated Stable Porous Ceria Support for Enhanced Li-CO2 Batteries Cathodes.

Lithium-carbon dioxide (Li-CO2) battery represents a high-energy density energy storage with excellent real-time CO2 enrichment and conversion, but its practical utilization is hampered by the development of an excellent catalytic cathode. Here, the synergistic catalytic strategy of designing CoRu bimetallic active sites achieves the electrocatalytic conversion of CO2 and the efficient decomposition of the discharge products, which in turn realizes the smooth operation of the Li-CO2 battery. Moreover, obtained support based on metal-organic frameworks precursors facilitates the convenient diffusion and adsorption of CO2, resulting in higher reaction concentration and lower mass transfer resistance. Meanwhile, the optimization of the interfacial electronic structure and the effective transfer of electrons are achieved by virtue of the strong interaction of CoRu at the support interface. As a result, the Li-CO2 cell assembled based on bimetallic CoRu active sites achieved a discharge capacity of 19,111mAhg-1 and a steady-state discharge voltage of 2.58V as well as a cycle life of >175 cycles at a rate of 100mAg-1. Further experiments combined with density-functional theory calculations achieve a deeply view of the connection between cathode and electrochemical performance and pave a way for the subsequent development of advanced Li-CO2 catalytic cathodes.

Approaching Splendid Catalysts for Li-CO2 Battery from the Theory to Practical Designing: A Review.

Lithium carbon dioxide (Li-CO2) batteries, noted for their high discharge voltage of approximately 2.8V and substantial theoretical specific energy of 1876Wh kg-1, represent a promising avenue for new energy sources and CO2 emission reduction. However, the practical application of these batteries faces significant hurdles, particularly at high current densities and over extended cycle lives, due to their complex reaction mechanisms and slow kinetics. This paper delves into the recent advancements in cathode catalysts for Li-CO2 batteries, with a specific focus on the designing philosophy from composition, geometry, and homogeneity of the catalysts to the proper test conditions and real-world application. It surveys the possible catalytic mechanisms, giving readers a brief introduction of how the energy is stored and released as well as the critical exploration of the relationship between material properties and performances. Specifically, optimization and standardization of test conditions for Li-CO2 battery research is highlighted to enhance data comparability, which is also critical to facilitate the practical application of Li-CO2 batteries. This review aims to bring up inspiration from previous work to advance the design of more effective and sustainable cathode catalysts, tailored to meet the practical demands of Li-CO2 batteries.

Restrained interfacial resistance Co5.47N@C derived from metal-organic frameworks for advanced Li–CO2 batteries cathodes

Lithium–carbon dioxide (Li–CO2) batteries are novel high energy density energy storage devices that can simultaneously enrich and convert CO2, but their widespread implementation is hindered by the continuous accumulation of lithium carbonate at the cathode. Herein, we developed non-precious metal cobalt-based nitride matrix composite Co[Formula: see text]N@C based on metal-organic frameworks precursor for the catalytic cathode of advanced Li–CO2 batteries. The highly stable Co[Formula: see text]N achieves favorable adsorption and catalysis of CO2 molecules by virtue of the excellent electronic structure on the surface, while the nanoscale high dispersion also effectively promotes interfacial electron transfer. As expected, the assembled Li–CO2 battery exhibits excellent electrochemical performance in the discharge capacity of 10,000 mAh g[Formula: see text] and a cycling capability of about 400 h. Further density functional theory (DFT) calculations explored the relationship between electronic structure and electrochemical activity. This work promotes the development of catalytic materials for Li–CO2 batteries cathode.

Activity evaluation and reaction mechanisms of highly efficient dual-atom transition metal catalysts in Li-CO2 batteries

Lithium-carbon dioxide (Li-CO2) batteries have received increased attention due to their high energy density and fixing CO2 as a major greenhouse gas. At the same time, there are challenges including low activity of cathode and high overpotential in Li-CO2 batteries. Herein, 45 dual-atom catalysts (DACs) composed of 9 transition metal (TM) atoms doped in nitrogen-doped graphene (M1M2-N-G, M1, M2 = Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn), as cathode catalysts of Li-CO2 batteries, have been studied by using first-principles calculations. According to the thermodynamic stability of the DACs and the ability of CO2 activation, 25 catalysts candidates were screened out. Then, the reaction activity and selectivity of DACs were evaluated by thermodynamical reaction energy and overpotential. Finally, TiMn-N-G displayed the smallest total electrode overpotential 1.83 V during the pathway of Li2CO3 and CrNi-N-G exhibited the smallest total electrode overpotential 0.08 V during the in Li2C2O4 pathway, respectively, which proved that they possessed better catalytic activity tendency in Li-CO2 batteries. This work provides not only a rational design to identify promising graphene-based catalysts, but also a general screen rule for atomic catalysts in 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.

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.

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.

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.

Enabling All-Solid-State Lithium-Carbon Dioxide Battery Operation in a Wide Temperature Range.

Flexible all-solid-state lithium-carbon dioxide batteries (FASSLCBs) are recognized as a next-generation energy storage technology by solving safety and shuttle effect problems. However, the present FASSLCBs rely heavily on high-temperature operation due to sluggish solid-solid-gas multiphase mass transfer and unclear capacity degradation mechanism. Herein, we designed bicontinuous hierarchical porous structures (BCHPSs) for both solid polymer electrolyte and cathode for FASSLCBs to facilitate the mass transfer in all connected directions. The formed large Lewis acidic surface effectively promotes the lithium salt dissociation and the CO2 conversion. Furthermore, it is unraveled that the battery capacity degradation originates from the "dead Li2CO3" formation, which is inhibited by the fast decomposition of Li2CO3. Accordingly, the assembled FASSLCBs exhibit an excellent cycling stability of 133 cycles at 60 °C, which is 2.7 times longer than that without BCHPSs, and the FASSLCBs can be operated repeatedly even at room temperature. This BCHPS method and fundamental deactivation mechanism provide a perspective for designing FASSLCBs with long cycling life.

Realizing long-cycling solid-state Li–CO2 batteries using Zn-doped LATP ceramic electrolytes

Lithium–carbon dioxide (Li–CO2) batteries with high theoretical energy density and carbon dioxide conversion ability are considered as the next generation of energy storage devices for solving electric vehicle range anxiety and reducing the greenhouse effect. However, the volatilization and leakage of traditional liquid organic electrolytes and the short circuit caused by the penetration of the lithium dendrite anode induce serious cycle and safety problems, hindering the commercial application of Li–CO2 batteries. Herein, a Zn-doped Li1.3Al0.3Ti1.7(PO4)3 (LATP) solid-state ceramic electrolyte stabilized in CO2 was designed and prepared. The additive Zn2+ ions make the crystal structure of the electrolyte denser with strong mechanical properties, providing an optimized network channel for Li+ ions transmission and further improving its ionic conductivity at room temperature. The optimized Zn-doped LATP exhibited an ionic conductivity of 2.45 × 10-3 S cm−1, much higher than that of LATP (2.67 × 10-4 S cm−1). The assembled Li–CO2 battery provides a high discharge capacity of 16,585 mAh/g and more than 180 stable cycles with charge/discharge overpotential less than 1.4 V. Due to the Zn-doped structure, the reduction effect of Ti4+ ions in LATP contact with Li was proved to be effectively suppressed. This doping strategy provides a feasible method for achieving high-performance solid-state Li–CO2 batteries.

A Force‐Assisted Li−O2 Battery Based on Piezoelectric Catalysis and Band Bending of MoS2/Pd Cathode

AbstractThe high overpotential caused by the slow kinetics of oxygen reduction (ORR) and oxygen evolution (OER) has greatly limited the practical application of lithium‐oxygen (Li−O2) batteries. The adoption of force‐field‐assisted system based on a newly developed piezocatalysis is promising in reducing the overpotential. Herein, a force‐assisted Li−O2 battery is first established by employing MoS2/Pd nanocomposite cathode, in which the piezoelectric polarization as well as built‐in electric field are formed in MoS2 piezoelectric catalyst under ultrasound activation, leading to the continuously separated electrons and holes to enhance the ORR and OER kinetics. Moreover, the introduction of Pd can promote the electrons transfer and further inhibit the complexation of electron–hole pairs, contributing to enhanced catalytic activity in the decomposition/generation of discharge products, resulting in reduced discharge/charge overpotentials. Thus, the force‐assisted MoS2/Pd‐based Li−O2 battery is capable of adjusting the output and input energies by the assisted ultrasonic wave. An ultra‐low charging platform of 2.86 V and a high discharging platform of 2.77 V are achieved. The proposed unique force‐assisted strategy can also be applied to lithium carbon dioxide battery system through the effective reduction and separation of CO2 and CO32−, providing significant insights in achieving efficient energy conversion for metal−air batteries.

Revealing the CO2 Conversion at Electrode/Electrolyte Interfaces in Li–CO2 Batteries via Nanoscale Visualization Methods

AbstractLithium–carbon dioxide (Li–CO2) battery technology presents a promising opportunity for carbon capture and energy storage. Despite tremendous efforts in Li–CO2 batteries, the complex electrode/electrolyte/CO2 triple‐phase interfacial processes remain poorly understood, in particular at the nanoscale. Here, using in situ atomic force microscopy and laser confocal microscopy‐differential interference contrast microscopy, we directly observed the CO2 conversion processes in Li–CO2 batteries at the nanoscale, and further revealed a laser‐tuned reaction pathway based on the real‐time observations. During discharge, a bi‐component composite, Li2CO3/C, deposits as micron‐sized clusters through a 3D progressive growth model, followed by a 3D decomposition pathway during the subsequent recharge. When the cell operates under laser (λ=405 nm) irradiation, densely packed Li2CO3/C flakes deposit rapidly during discharge. Upon the recharge, they predominantly decompose at the interfaces of the flake and electrode, detaching themselves from the electrode and causing irreversible capacity degradation. In situ Raman shows that the laser promotes the formation of poorly soluble intermediates, Li2C2O4, which in turn affects growth/decomposition pathways of Li2CO3/C and the cell performance. Our findings provide mechanistic insights into interfacial evolution in Li–CO2 batteries and the laser‐tuned CO2 conversion reactions, which can inspire strategies of monitoring and controlling the multistep and multiphase interfacial reactions in advanced electrochemical devices.

Recycled Tandem Catalysts Promising Ultralow Overpotential Li-CO2 Batteries.

Lithium-carbon dioxide (Li-CO2 ) batteries are regarded as a prospective technology to relieve the pressure of greenhouse emissions but are confronted with sluggish CO2 redox kinetics and low energy efficiency. Developing highly efficient and low-cost catalysts to boost bidirectional activities is craved but remains a huge challenge. Herein, derived from the spent lithium-ion batteries, a tandem catalyst is subtly synthesized and significantly accelerates the CO2 reduction and evolution reactions (CO2 RR and CO2 ER) kinetics with an in-built electric field (BEF). Combining with the theoretical calculations and advanced characterization techniques, this work reveals that the designed interface-induced BEF regulates the adsorption/decomposition of the intermediates during CO2 RR and CO2 ER, endowing the recycled tandem catalyst with excellent bidirectional activities. As a result, the spent electronics-derived tandem catalyst exhibits remarkable bidirectional catalytic performance, such as an ultralow voltage gap of 0.26V and an ultrahigh energy efficiency of 92.4%. Profoundly, this work affords new opportunities to fabricate low-cost electrocatalysts from recycled spent electronics and inspires fresh perceptions of interfacial regulation including but not limited to BEF to engineer better Li-CO2 batteries.

Revealing the CO2 Conversion at Electrode/Electrolyte Interfaces in Li-CO2 Batteries via Nanoscale Visualization Methods.

Lithium-carbon dioxide (Li-CO2 ) battery technology presents a promising opportunity for carbon capture and energy storage. Despite tremendous efforts in Li-CO2 batteries, the complex electrode/electrolyte/CO2 triple-phase interfacial processes remain poorly understood, in particular at the nanoscale. Here, using in situ atomic force microscopy and laser confocal microscopy-differential interference contrast microscopy, we directly observed the CO2 conversion processes in Li-CO2 batteries at the nanoscale, and further revealed a laser-tuned reaction pathway based on the real-time observations. During discharge, a bi-component composite, Li2 CO3 /C, deposits as micron-sized clusters through a 3D progressive growth model, followed by a 3D decomposition pathway during the subsequent recharge. When the cell operates under laser (λ=405 nm) irradiation, densely packed Li2 CO3 /C flakes deposit rapidly during discharge. Upon the recharge, they predominantly decompose at the interfaces of the flake and electrode, detaching themselves from the electrode and causing irreversible capacity degradation. In situ Raman shows that the laser promotes the formation of poorly soluble intermediates, Li2 C2 O4 , which in turn affects growth/decomposition pathways of Li2 CO3 /C and the cell performance. Our findings provide mechanistic insights into interfacial evolution in Li-CO2 batteries and the laser-tuned CO2 conversion reactions, which can inspire strategies of monitoring and controlling the multistep and multiphase interfacial reactions in advanced electrochemical devices.

A highly reversible force-assisted Li − CO2 battery based on piezoelectric effect of Bi0.5Na0.5TiO3 nanorods

The use of light-assisted cathode is regarded as an effective approach to reduce the overpotential of lithium carbon dioxide (Li − CO2) batteries. However, the inefficient electron-hole separation and the complex discharge–charge reactions hamper the efficiency of CO2 photocatalytic reaction in battery. Herein, a highly reversible force-assisted Li − CO2 battery has been established for the first time by employing a Bi0.5Na0.5TiO3 nanorods piezoelectric cathode. The high-energy electron and holes generated by the piezoelectric cathode with ultrasonic force can effectively enhance the carbon dioxide reduction reaction (CDRR) and carbon dioxide evolution reaction (CDER) kinetics, thereby reducing the overpotentials during the discharge–charge processes. Moreover, the morphology of the discharge product (Li2CO3) can be modified via the dense surface electrons of the piezoelectric cathode, resulting in the promoted decomposition kinetics of Li2CO3 in charging progress. Thus, the force-assisted Li − CO2 battery with the unique piezoelectric cathode can adjust the output and input energy by ultrasonic wave, and provides an ultra-low charging platform of 3.52 V, and exhibits excellent cycle stability (a charging platform of 3.42 V after 100 h cycles). The investigation of the force-assisted process described herein provides significant insights to solve overpotential in the Li − CO2 batteries system.

Revisiting the Role of Discharge Products in Li-CO2 Batteries.

Rechargeable lithium-carbon dioxide (Li-CO2 ) batteries are promising devices for CO2 recycling and energy storage. However, thermodynamically stable and electrically insulating discharge products (DPs) (e.g., Li2 CO3 ) deposited at cathodes require rigorous conditions for completed decomposition, resulting in large recharge polarization and poor battery reversibility. Although progresses have been achieved in cathode design and electrolyte optimization, the significance of DPs is generally underestimated. Therefore, it is necessary to revisit the role of DPs in Li-CO2 batteries to boost overall battery performance. Here, we report for the first time, a critical and systematic review of DPs in Li-CO2 batteries. We appraise fundamentals of reactions for formation and decomposition of DPs and demonstrate impacts on battery performance including, overpotential, capacity and stability, and highlight the necessity of discharge product management. We assess practical in-situ/operando technologies to characterize reaction intermediates and the corresponding DPs for mechanism investigation. Additionally, achievable control measures to boost the decomposition of DPs are evidenced to provide battery design principles and improve the battery performance. Findings from this work will deepen the understanding of electrochemistry of Li-CO2 batteries and promote practical applications. This article is protected by copyright. All rights reserved.

Recent Progress in Hot Spot Regulated Strategies for Catalysts Applied in Li-CO2 Batteries.

As a high energy density power system, lithium-carbon dioxide (Li-CO2 ) batteries play an important role in addressing the fossil fuel crisis issues and alleviating the greenhouse effect. However, the sluggish transformation kinetic of CO2 and the difficult decomposition of discharge products impede the achievement of large capacity, small overpotential, and long life span of the batteries, which require exploring efficient catalysts to resolve these problems. In this review, the main focus is on the hot spot regulation strategies of the catalysts, which include the modulation of the active sites, the designing of microstructure, and the construction of composition. The recent progress of promising catalysis with hot spot regulated strategies is systematically addressed. Critical challenges are also presented and perspectives to provide useful guidance for the rational design of highly efficient catalysts for practical advanced Li-CO2 batteries are proposed.