Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 24, Pages 27166-27175Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c04814
Keywords
density functional theory; oxygen evolution reaction; Li-O-2 battery; 4d transition metal catalysts; electrochemical catalysis
Funding
- National Natural Science Foundation of China
- NSFC [21973107, 51702345, 11804351]
- Key Project of Science and Technology of Shanghai [18511109400]
- Science and Technology Commission of Shanghai Municipality [18520723000]
- Shanghai Sailing program [18YF1427300]
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The development of active electrocatalysts for enhancing Li2O2 decomposition kinetics plays an important role in reducing the overpotential of Li-O-2 batteries. However, a catalytic descriptor is not established due to the difficult characterization of the charge transfer between Li2O2 and the catalyst. Here, we employ first-principles thermodynamic calculations to study the electrocatalytic mechanism of 4d transition metals. We found that charge acceptation and donation capacities of catalysts, defined as surface electron affinity (V-SEA) and surface ionic potential (V-SIP), take cooperative responsibilities for the activation of Li-O-2 bonds and the reduction of desorption barriers of Li+ and O-2, respectively. Therefore, we define surface electronegativity V-SE (V-SE (V-SEA + V-SIP)/2), which exhibits a volcano curve with a reduced charge overpotential, as the catalytic descriptor. We identified those catalysts with surface electronegativities of 1.7-2.2 V to have highly catalytic activities in the reduction of the charge overpotential, which are well verified by previous experimental data. The present study opens a wide avenue in the development of high-activity catalysts for interfacial electrocatalysts by an effective descriptor.
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