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1. Improved cycle performance of Li-CO2 batteries with nickel manganite supported carbon nanotube NiMn2O4 @CNT cathode

   Wang, Jianda ; Powell, Matthew ; Alcala, Ryan ; Fetrow, Christopher ; Zhou, Xiao-Dong ; Wei, Shuya ( October 2023 , Journal of the Electrochemical Society)

   Doron Aurbach (Ed.)

   Rechargeable Li-CO2 batteries have emerged as promising candidates for next generation batteries due to their low cost, high theoretical capacity, and ability to capture the greenhouse gas CO2. However, these batteries still face challenges such as slow reaction kinetic and short cycle performance due to the accumulation of discharge products. To address this issue, it is necessary to design and develop high efficiency electrocatalysts that can improve CO2 reduction reaction. In this study, we report the use of NiMn2O4 electrocatalysts combined with multiwall carbon nanotubes as a cathode material in the Li-CO2 batteries. This combination proved effective in decomposing discharge products and enhancing cycle performance. The battery shows stable discharge–charge cycles for at least 30 cycles with a high limited capacity of 1000 mAh/g at current density of 100 mA/g. Furthermore, the battery with the NiMn2O4@CNT catalyst exhibits a reversible discharge capacity of 2636 mAh/g. To gain a better understanding of the reaction mechanism of Li-CO2 batteries, spectroscopies and microscopies were employed to identify the chemical composition of the discharge products. This work paves a pathway to increase cycle performance in metal-CO2 batteries, which could have significant implications for energy storage and the reduction of greenhouse gas emissions. 

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2. A Long‐Cycle‐Life Lithium–CO 2 Battery with Carbon Neutrality

   https://doi.org/10.1002/adma.201902518  

   Ahmadiparidari, Alireza ; Warburton, Robert E. ; Majidi, Leily ; Asadi, Mohammad ; Chamaani, Amir ; Jokisaari, Jacob R. ; Rastegar, Sina ; Hemmat, Zahra ; Sayahpour, Baharak ; Assary, Rajeev S. ; et al ( August 2019 , Advanced Materials)

   Lithium–CO₂batteries are attractive energy‐storage systems for fulfilling the demand of future large‐scale applications such as electric vehicles due to their high specific energy density. However, a major challenge with Li–CO₂batteries is to attain reversible formation and decomposition of the Li₂CO₃and carbon discharge products. A fully reversible Li–CO₂battery is developed with overall carbon neutrality using MoS₂nanoflakes as a cathode catalyst combined with an ionic liquid/dimethyl sulfoxide electrolyte. This combination of materials produces a multicomponent composite (Li₂CO₃/C) product. The battery shows a superior long cycle life of 500 for a fixed 500 mAh g⁻¹capacity per cycle, far exceeding the best cycling stability reported in Li–CO₂batteries. The long cycle life demonstrates that chemical transformations, making and breaking covalent CO bonds can be used in energy‐storage systems. Theoretical calculations are used to deduce a mechanism for the reversible discharge/charge processes and explain how the carbon interface with Li₂CO₃provides the electronic conduction needed for the oxidation of Li₂CO₃and carbon to generate the CO₂on charge. This achievement paves the way for the use of CO₂in advanced energy‐storage systems.

    

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3. Rechargeable Li/Cl 2 Battery Down to −80 °C

   https://doi.org/10.1002/adma.202307192  

   Liang, Peng ; Zhu, Guanzhou ; Huang, Cheng‐Liang ; Li, Yuan‐Yao ; Sun, Hao ; Yuan, Bin ; Wu, Shu‐Chi ; Li, Jiachen ; Wang, Feifei ; Hwang, Bing‐Joe ; et al ( December 2023 , Advanced Materials)

   Low temperature rechargeable batteries are important to life in cold climates, polar/deep‐sea expeditions, and space explorations. Here, this work reports 3.5–4 V rechargeable lithium/chlorine (Li/Cl₂) batteries operating down to −80 °C, employing Li metal negative electrode, a novel carbon dioxide (CO₂) activated porous carbon (KJCO₂) as the positive electrode, and a high ionic conductivity (≈5–20 mS cm⁻¹from −80 °C to room‐temperature) electrolyte comprised of aluminum chloride (AlCl₃), lithium chloride (LiCl), and lithium bis(fluorosulfonyl)imide (LiFSI) in low‐melting‐point (−104.5 °C) thionyl chloride (SOCl₂). Between room‐temperature and −80 °C, the Li/Cl₂battery delivers up to ≈29 100–4500 mAh g⁻¹first discharge capacity (based on carbon mass) and a 1200–5000 mAh g⁻¹reversible capacity over up to 130 charge–discharge cycles. Mass spectrometry and X‐ray photoelectron spectroscopy probe Cl₂trapped in the porous carbon upon LiCl electro‐oxidation during charging. At −80 °C, Cl₂/SCl₂/S₂Cl₂generated by electro‐oxidation in the charging step are trapped in porous KJCO₂carbon, allowing for reversible reduction to afford a high discharge voltage plateau near ≈4 V with up to ≈1000 mAh g⁻¹capacity for SCl₂/S₂Cl₂reduction and up to ≈4000 mAh g⁻¹capacity at ≈3.1 V plateau for Cl₂reduction.

    

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4. Enabling Uniform and Accurate Control of Cycling Pressure for All‐Solid‐State Batteries

   https://doi.org/10.1002/aenm.202304327  

   Chen, Yu‐Ting ; Jang, Jihyun ; Oh, Jin_An_Sam ; Ham, So‐Yeon ; Yang, Hedi ; Lee, Dong‐Ju ; Vicencio, Marta ; Lee, Jeong_Beom ; Tan, Darren_H_S ; Chouchane, Mehdi ; et al ( May 2024 , Advanced Energy Materials)

   All‐solid‐state batteries are emerging as potential successors in energy storage technologies due to their increased safety, stemming from replacing organic liquid electrolytes in conventional Li‐ion batteries with less flammable solid‐state electrolytes. However, all‐solid‐state batteries require precise control over cycling pressure to maintain effective interfacial contacts between materials. Traditional uniaxial cell holders, often used in battery research, face challenges in accommodating electrode volume changes, providing uniform pressure distribution, and maintaining consistent pressure over time. This study introduces isostatic pouch cell holders utilizing air as pressurizing media to achieve uniform and accurately regulated cycling pressure. LiNi_0.8Co_0.1Mn_0.1O₂| Li₆PS₅Cl | Si pouch cells are fabricated and tested under 1 to 5 MPa pressures, revealing improved electrochemical performance with higher cycling pressures, with 2 MPa as the minimum for optimal operation. A bilayer pouch cell with a theoretical capacity of 100 mAh, cycled with an isostatic pouch cell holder, demonstrated a first‐cycle Coulombic efficiency of 76.9% and a discharge capacity of 173.6 mAh g⁻¹(88.1 mAh), maintaining 83.6% capacity after 100 cycles. These findings underscore the effectiveness of isostatic pouch cell holders in enhancing the performance and practical application of all‐solid‐state batteries.

    

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5. A High‐Rate Li–CO 2 Battery Enabled by 2D Medium‐Entropy Catalyst

   https://doi.org/10.1002/adfm.202300814  

   Jaradat, Ahmad ; Zhang, Chengji ; Shashikant Sutar, Sanket ; Shan, Nannan ; Wang, Shuxi ; Singh, Sachin Kumar ; Yang, Taimin ; Kumar, Khagesh ; Sharma, Kartikey ; Namvar, Shahriar ; et al ( April 2023 , Advanced Functional Materials)

   Lithium‐air batteries based on CO₂reactant (Li–CO₂) have recently been of interest because it has been found that reversible Li/CO₂electrochemistry is feasible. In this study, a new medium‐entropy cathode catalyst, (NbTa)_0.5BiS₃, that enables the reversible electrochemistry to operate at high rates is presented. This medium entropy cathode catalyst is combined with an ionic liquid‐based electrolyte blend to give a Li–CO₂battery that operates at high current density of 5000 mA g⁻¹and capacity of 5000 mAh g⁻¹for up to 125 cycles, far exceeding reported values in the literature for this type of battery. The higher rate performance is believed to be due to the greater stability of the multi‐element (NbTa)_0.5BiS₃catalyst because of its higher entropy compared to previously used catalysts with a smaller number of elements with lower entropies. Evidence for this comes from computational studies giving very low surface energies (high surface stability) for (NbTa)_0.5BiS₃and transmission electron microscopystudies showing the structure being retained after cycling. In addition, the calculations indicate that Nb‐terminated surface promotes Li–CO₂electrochemistry resulting in Li₂CO₃and carbon formation, consistent with the products found in the cell. These results open new direction to design and develop high‐performance Li–CO₂batteries.

    

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