Nonredox trivalent nickel catalyzing nucleophilic electrooxidation of organics

Yuandong Yan, Ruyi Wang, Qian Zheng, Jiaying Zhong, Weichang Hao, Shicheng Yan () and Zhigang Zou
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Yuandong Yan: Nanjing University
Ruyi Wang: Nanjing University
Qian Zheng: Nanjing University
Jiaying Zhong: Nanjing University
Weichang Hao: Beihang University
Shicheng Yan: Nanjing University
Zhigang Zou: Nanjing University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract A thorough comprehension of the mechanism behind organic electrooxidation is crucial for the development of efficient energy conversion technology. Here, we find that trivalent nickel is capable of oxidizing organics through a nucleophilic attack and electron transfer via a nonredox process. This nonredox trivalent nickel exhibits exceptional kinetic efficiency in oxidizing organics that possess the highest occupied molecular orbital energy levels ranging from −7.4 to −6 eV (vs. Vacuum level) and the dual local softness values of nucleophilic atoms in nucleophilic functional groups, such as hydroxyls (methanol, ethanol, benzyl alcohol), carbonyls (formamide, urea, formaldehyde, glucose, and N-acetyl glucosamine), and aminos (benzylamine), ranging from −0.65 to −0.15. The rapid electrooxidation kinetics can be attributed to the isoenergetic channels created by the nucleophilic attack and the nonredox electron transfer via the unoccupied eg orbitals of trivalent nickel (t2g6eg1). Our findings are valuable in identifying kinetically fast organic electrooxidation on nonredox catalysts for efficient energy conversions.

Date: 2023
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DOI: 10.1038/s41467-023-43649-6

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