A High‐Rate Li–CO<sub>2</sub> Battery Enabled by 2D Medium‐Entropy Catalyst
Ahmad Jaradat, Chengji Zhang, Sanket Shashikant Sutar, Nannan Shan, Shuxi Wang, Sachin Kumar Singh, Taimin Yang, Khagesh Kumar, Kartikey Sharma, Shahriar Namvar, Alireza Ahmadiparidari, Tomás Rojas, Vikas Berry, Jordi Cabana, Zhehao Huang, Arunkumar Subramanian, Anh T. Ngo, Larry A. Curtiss, Amin Salehi‐Khojin
Abstract
Abstract Lithium‐air batteries based on CO 2 reactant (Li–CO 2 ) have recently been of interest because it has been found that reversible Li/CO 2 electrochemistry is feasible. In this study, a new medium‐entropy cathode catalyst, (NbTa) 0.5 BiS 3 , 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–CO 2 battery that operates at high current density of 5000 mA g −1 and capacity of 5000 mAh g −1 for 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) 0.5 BiS 3 catalyst 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) 0.5 BiS 3 and transmission electron microscopystudies showing the structure being retained after cycling. In addition, the calculations indicate that Nb‐terminated surface promotes Li–CO 2 electrochemistry resulting in Li 2 CO 3 and carbon formation, consistent with the products found in the cell. These results open new direction to design and develop high‐performance Li–CO 2 batteries.