Turning main-group element magnesium into a highly active electrocatalyst for oxygen reduction reaction

Shuai Liu, Zedong Li, Changlai Wang, Weiwei Tao, Minxue Huang, Ming Zuo, Yang Yang, Kang Yang, Lijuan Zhang, Shi Chen, Pengping Xu and Qianwang Chen ()
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Shuai Liu: University of Science and Technology of China
Zedong Li: University of Science and Technology of China
Changlai Wang: University of Science and Technology of China
Weiwei Tao: Boston University
Minxue Huang: University of Science and Technology of China
Ming Zuo: University of Science and Technology of China
Yang Yang: University of Science and Technology of China
Kang Yang: University of Science and Technology of China
Lijuan Zhang: Shanghai Institute of Applied Physics
Shi Chen: University of Science and Technology of China
Pengping Xu: University of Science and Technology of China
Qianwang Chen: University of Science and Technology of China

Nature Communications, 2020, vol. 11, issue 1, 1-11

Abstract: Abstract It is known that the main-group metals and their related materials show poor catalytic activity due to a broadened single resonance derived from the interaction of valence orbitals of adsorbates with the broad sp-band of main-group metals. However, Mg cofactors existing in enzymes are extremely active in biochemical reactions. Our density function theory calculations reveal that the catalytic activity of the main-group metals (Mg, Al and Ca) in oxygen reduction reaction is severely hampered by the tight-bonding of active centers with hydroxyl group intermediate, while the Mg atom coordinated to two nitrogen atoms has the near-optimal adsorption strength with intermediate oxygen species by the rise of p-band center position compared to other coordination environments. We experimentally demonstrate that the atomically dispersed Mg cofactors incorporated within graphene framework exhibits a strikingly high half-wave potential of 910 mV in alkaline media, turning a s/p-band metal into a highly active electrocatalyst.

Date: 2020
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DOI: 10.1038/s41467-020-14565-w

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