• Subramanian, Arunkumar
• Curtiss, Larry A.
• Salehi-Khojin, Amin
• Ngo, Anh T.
• Namaeighasemi, Arash
• Jaradat, Ahmad
• Ncube, Musawenkosi K.
• Berry, Vikas
• Namvar, Shahriar
• Rai, Nikhil
• Kumar, Khagesh
• Koverga, Volodymyr
• Shahbazi, Hessam
• Nemade, Roshan Y.
• Zhang, Chengji
• Seraji, Pardis
• Cabana, Jordi
• Shan, Nannan

Abstract

<jats:title>Abstract</jats:title><jats:p>Li‐CO<jats:sub>2</jats:sub> batteries with a high theoretical energy density (1876 Wh kg<jats:sup>−1</jats:sup>) have unique benefits for reversible carbon fixation for energy storage systems. However, due to lack of stable and highly active catalysts, the long‐term operation of Li‐CO<jats:sub>2</jats:sub> batteries is limited to low current densities (mainly &lt;0.2 mA cm<jats:sup>−2</jats:sup>) that are far from practical conditions. In this work, it is discovered that, with an ionic liquid‐based electrolyte, highly active and stable transition metal trichalcogenide alloy catalysts of Sb<jats:sub>0.67</jats:sub>Bi<jats:sub>1.33</jats:sub>X<jats:sub>3</jats:sub> (X = S, Te) enable operation of the Li‐CO<jats:sub>2</jats:sub> battery at a very high current rate of 1 mA cm<jats:sup>−2</jats:sup> for up to 220 cycles. It is revealed that: i) the type of chalcogenide (Te vs S) significantly affects the electronic and catalytic properties of the catalysts, ii) a coupled cation‐electron charge transfer process facilitates the carbon dioxide reduction reaction (CO<jats:sub>2</jats:sub>RR) occurring during discharge, and iii) the concentration of ionic liquid in the electrolyte controls the number of participating CO<jats:sub>2</jats:sub> molecules in reactions. A combination of these key factors is found to be crucial for a successful operation of the Li‐CO<jats:sub>2</jats:sub> chemistry at high current rates. This work introduces a new class of catalysts with potential to fundamentally solve challenges of this type of batteries.</jats:p>

Topics

• density
• impedance spectroscopy
• Carbon
• energy density