Kim, Hyung-Jin Jung, Sung Chul Han, Young-Kyu Oh, Si Hyoung 2024-01-20T07:31:14Z 2024-01-20T07:31:14Z 2021-09-05 2015-04 2211-2855 https://pubs.kist.re.kr/handle/201004/125609 Herein, we provide critical information via first-principles calculations to solve one of the major problems of Li-O-2 batteries, namely, large overpotentials during the charge-discharge process. First, we found that PtCo exhibits remarkably low oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) overpotentials of 0.19 and 0.20 V, respectively. These are considerably lower than those of pure Pt (1.02 and 1.62V, respectively) and of high-performance Pt3Co (1.02 and 1.13V, respectively). The composition optimization of bimetallic catalysts is therefore critical in developing an optimal Li-O-2 battery catalyst with an overpotential of nearly zero. Second, our calculations demonstrate that replacing the late transition metal Co in Pt3Co with the early transition metal Ti significantly decreases overpotentials, yielding ORR and OER overpotentials of 0.34 and 0.82 V, respectively. These results are opposite to those obtained for fuel cells. Notably, our results suggest that a bimetallic catalyst with poor catalytic activity in fuel cells might show excellent activity in Li-O-2 cells. In particular, combinations of active Pt with early transition metals should be studied for development of bimetallic catalysts with high round-trip efficiency in Li-O-2 batteries. Finally, we suggest that the adsorption energies of Li and LiO2 are critical descriptors of catalytic activity and that they should be used to screen new candidate materials. This is because low ORR and OER overpotentials are closely related to strong Li and weak LiO2 adsorptions, respectively, on the catalytic surface. (C) 2015 Elsevier Ltd. All rights reserved. English ELSEVIER OXYGEN REDUCTION REACTION METAL-AIR BATTERIES ELECTROCATALYTIC ACTIVITY LI-O-2 BATTERIES ALLOY NANOPARTICLES RATE CAPABILITY ELECTROCHEMISTRY SKIN PT3NI(111) MORPHOLOGY An atomic-level strategy for the design of a low overpotential catalyst for Li - O-2 batteries Article 10.1016/j.nanoen.2015.03.030 1 NANO ENERGY, v.13, pp.679 - 686 NANO ENERGY 13 679 686 scie scopus 000358414700071 2-s2.0-84937967120 Chemistry, Physical Nanoscience & Nanotechnology Materials Science, Multidisciplinary Physics, Applied Chemistry Science & Technology - Other Topics Materials Science Physics Article OXYGEN REDUCTION REACTION METAL-AIR BATTERIES ELECTROCATALYTIC ACTIVITY LI-O-2 BATTERIES ALLOY NANOPARTICLES RATE CAPABILITY ELECTROCHEMISTRY SKIN PT3NI(111) MORPHOLOGY Electrocatalyst Nanoparticle Li-O-2 battery Sluggish kinetics Density functional calculation