Modulating the potential-determining step in oxygen evolution reaction by regulating the cobalt valence in NiCo2O4 via Ru substitution

[Display omitted] •NiCo2O4 nano-flakes with different dopant concentrations of Ruthenium (NiCo2-xRuxO4) are synthesized.•Ru dopant changes the valance state of Co, and adjust the ratio of Co2+/Co3+.•The free energy of the potential-determining step is reduced.•The optimized Ru-doped NiCo2O4 exhibits...

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Published inApplied surface science Vol. 544; p. 148897
Main Authors Peng, Cailing, Liu, Huan, Chen, Jifang, Zhang, Yuanxi, Zhu, Liuyang, Wu, Qingmei, Zou, Wei, Wang, Jianlin, Fu, Zhengping, Lu, Yalin
Format Journal Article
LanguageEnglish
Published Elsevier B.V 01.04.2021
Subjects
Electrocatalysis
Oxygen evolution reaction
Oxygen intermediate
Ruthenium doping
Spinel oxides
Valance regulation
Electrocatalysis
Oxygen intermediate
Spinel oxides
Oxygen evolution reaction
Ruthenium doping
Valance regulation
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Abstract [Display omitted] •NiCo2O4 nano-flakes with different dopant concentrations of Ruthenium (NiCo2-xRuxO4) are synthesized.•Ru dopant changes the valance state of Co, and adjust the ratio of Co2+/Co3+.•The free energy of the potential-determining step is reduced.•The optimized Ru-doped NiCo2O4 exhibits excellent OER activities and smaller charge transfer resistance. Spinel oxide has a unique open structure, the existence of numerous empty interstitial sites is conducive to cation migration, so the valence of transition metal in spinel oxide is modifiable. Optimizing the valence state on the spinel surface has always been the focus of research because it is key for realizing efficient oxygen evolution reaction. In this paper, we introduced metal Ru into spinel oxide NiCo2O4 to adjust the valence state of the cations on the spinel surface, achieving a suitable ion ratio of Co2+/Co3+. The catalytic performance is the best when the doping concentration of Ru is 5.7% (NiCo1.7Ru0.3O4). In 1.0 M KOH, NiCo1.7Ru0.3O4 required only 280 mV overpotential to drive the current of 10 mA·cm−2. The incorporation of Ru induces more Co2+ on the octahedral site and changes the valence state of Co, optimizing the adsorption of the oxygen intermediate. In addition, the coordinated charge transfer between Ru, Co, and Ni will also accelerate the reaction. These results confirm that the Ru doping process can not only change the electrochemical performance of spinel oxides but also provide new insights into the design of OER (Oxygen evolution reaction) catalysts.
AbstractList [Display omitted] •NiCo2O4 nano-flakes with different dopant concentrations of Ruthenium (NiCo2-xRuxO4) are synthesized.•Ru dopant changes the valance state of Co, and adjust the ratio of Co2+/Co3+.•The free energy of the potential-determining step is reduced.•The optimized Ru-doped NiCo2O4 exhibits excellent OER activities and smaller charge transfer resistance. Spinel oxide has a unique open structure, the existence of numerous empty interstitial sites is conducive to cation migration, so the valence of transition metal in spinel oxide is modifiable. Optimizing the valence state on the spinel surface has always been the focus of research because it is key for realizing efficient oxygen evolution reaction. In this paper, we introduced metal Ru into spinel oxide NiCo2O4 to adjust the valence state of the cations on the spinel surface, achieving a suitable ion ratio of Co2+/Co3+. The catalytic performance is the best when the doping concentration of Ru is 5.7% (NiCo1.7Ru0.3O4). In 1.0 M KOH, NiCo1.7Ru0.3O4 required only 280 mV overpotential to drive the current of 10 mA·cm−2. The incorporation of Ru induces more Co2+ on the octahedral site and changes the valence state of Co, optimizing the adsorption of the oxygen intermediate. In addition, the coordinated charge transfer between Ru, Co, and Ni will also accelerate the reaction. These results confirm that the Ru doping process can not only change the electrochemical performance of spinel oxides but also provide new insights into the design of OER (Oxygen evolution reaction) catalysts.
ArticleNumber 148897
Author Chen, Jifang
Liu, Huan
Zou, Wei
Lu, Yalin
Wu, Qingmei
Zhang, Yuanxi
Peng, Cailing
Zhu, Liuyang
Wang, Jianlin
Fu, Zhengping
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  givenname: Huan
  surname: Liu
  fullname: Liu, Huan
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  givenname: Wei
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  givenname: Jianlin
  surname: Wang
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  givenname: Zhengping
  orcidid: 0000-0002-7896-1333
  surname: Fu
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  givenname: Yalin
  surname: Lu
  fullname: Lu, Yalin
  email: yllu@ustc.edu.cn
  organization: Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, PR China
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Keywords Electrocatalysis
Oxygen intermediate
Spinel oxides
Oxygen evolution reaction
Ruthenium doping
Valance regulation
Language English
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Snippet [Display omitted] •NiCo2O4 nano-flakes with different dopant concentrations of Ruthenium (NiCo2-xRuxO4) are synthesized.•Ru dopant changes the valance state of...
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StartPage 148897
SubjectTerms Electrocatalysis
Oxygen evolution reaction
Oxygen intermediate
Ruthenium doping
Spinel oxides
Valance regulation
Title Modulating the potential-determining step in oxygen evolution reaction by regulating the cobalt valence in NiCo2O4 via Ru substitution
URI https://dx.doi.org/10.1016/j.apsusc.2020.148897
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