Lattice oxygen activation enabled by high-valence metal sites for enhanced water oxidation

Ning Zhang, Xiaobin Feng, Dewei Rao, Xi Deng, Lejuan Cai, Bocheng Qiu, Ran Long, Yujie Xiong, Yang Lu () and Yang Chai ()
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Ning Zhang: The Hong Kong Polytechnic University, Hung Hom, Kowloon
Xiaobin Feng: City University of Hong Kong, Kowloon
Dewei Rao: Jiangsu University
Xi Deng: University of Science and Technology of China
Lejuan Cai: The Hong Kong Polytechnic University, Hung Hom, Kowloon
Bocheng Qiu: The Hong Kong Polytechnic University, Hung Hom, Kowloon
Ran Long: University of Science and Technology of China
Yujie Xiong: University of Science and Technology of China
Yang Lu: City University of Hong Kong, Kowloon
Yang Chai: The Hong Kong Polytechnic University, Hung Hom, Kowloon

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

Abstract: Abstract Anodic oxygen evolution reaction (OER) is recognized as kinetic bottleneck in water electrolysis. Transition metal sites with high valence states can accelerate the reaction kinetics to offer highly intrinsic activity, but suffer from thermodynamic formation barrier. Here, we show subtle engineering of highly oxidized Ni4+ species in surface reconstructed (oxy)hydroxides on multicomponent FeCoCrNi alloy film through interatomically electronic interplay. Our spectroscopic investigations with theoretical studies uncover that Fe component enables the formation of Ni4+ species, which is energetically favored by the multistep evolution of Ni2+→Ni3+→Ni4+. The dynamically constructed Ni4+ species drives holes into oxygen ligands to facilitate intramolecular oxygen coupling, triggering lattice oxygen activation to form Fe-Ni dual-sites as ultimate catalytic center with highly intrinsic activity. As a result, the surface reconstructed FeCoCrNi OER catalyst delivers outstanding mass activity and turnover frequency of 3601 A gmetal−1 and 0.483 s−1 at an overpotential of 300 mV in alkaline electrolyte, respectively.

Date: 2020
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DOI: 10.1038/s41467-020-17934-7

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