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Peer-reviewedCC BY-NC 3.0Chemical Science

Synergistic Ce–Ce dimerization regulates electronic hybridization for enhanced oxygen reduction

  • Xue Bai1
  • Jingru Sun1
  • Fuquan Bai2
  • Lina Li3
  • Jingqi Guan1
  1. 1Institute of Physical Chemistry, National Demonstration Center for Experimental Chemistry Education, College of Chemistry, Jilin University 2519 Jiefang Road Changchun 130021 P. R. China
  2. 2Laboratory of Theoretical and Computational Chemistry, Institute of Theoretical Chemistry, College of Chemistry Changchun 130023 P. R. China
  3. 3Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute Shanghai 201204 P. R. China
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Abstract

Compared with 3d transition metals, rare-earth elements, particularly cerium, exhibit more markedly sluggish Fenton-like reaction kinetics, making them more stable under oxidative oxygen reduction reaction (ORR) conditions. Here, a dual-atom cerium catalyst is fabricated on nitrogen-doped graphene (Ce2-NG) through an ultrafast Joule-heating strategy. This rapid synthesis enables the construction of Ce–Ce dimers within milliseconds, effectively suppressing aggregation and ensuring the atomic-level stabilization. Ce2-NG demonstrates remarkable ORR performance, reaching a half-wave potential of 0.906 V, along with superior durability and strong resistance to methanol crossover. When employed as the cathode catalyst in a zinc–air battery (ZAB), the device exhibits an elevated open-circuit voltage and excellent long-term operational stability, clearly surpassing those of Pt/C + RuO2 counterparts. Operando spectroscopy combined with density functional theory supports the Ce2–N6 moiety as the active center, where dual-atom cerium cooperation drives charge redistribution, enhances *OH binding, and lowers the free energy change of the potential-determining step. This study introduces a controllable synthesis method for constructing rare-earth dual-atom catalysts, broadening the compositional landscape of atomically dispersed electrocatalysts for sustainable energy conversion.

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Cite

BibTeXRIS
BibTeX
@article{bai2026synergistic,
  title = {{Synergistic Ce–Ce dimerization regulates electronic hybridization for enhanced oxygen reduction}},
  author = {Xue Bai and Jingru Sun and Fuquan Bai and Lina Li and Jingqi Guan},
  journal = {Chemical Science},
  year = {2026},
  month = aug,
  doi = {10.1039/d6sc05909k},
  url = {https://doi.org/10.1039/d6sc05909k},
  note = {CC BY-NC 3.0},
}
RIS
TY  - JOUR
TI  - Synergistic Ce–Ce dimerization regulates electronic hybridization for enhanced oxygen reduction
AU  - Xue Bai
AU  - Jingru Sun
AU  - Fuquan Bai
AU  - Lina Li
AU  - Jingqi Guan
PY  - 2026
DA  - 2026/08/31
JO  - Chemical Science
DO  - 10.1039/d6sc05909k
UR  - https://doi.org/10.1039/d6sc05909k
AB  - Compared with 3d transition metals, rare-earth elements, particularly cerium, exhibit more markedly sluggish Fenton-like reaction kinetics, making them more stable under oxidative oxygen reduction reaction (ORR) conditions. Here, a dual-atom cerium catalyst is fabricated on nitrogen-doped graphene (Ce2-NG) through an ultrafast Joule-heating strategy. This rapid synthesis enables the construction of Ce–Ce dimers within milliseconds, effectively suppressing aggregation and ensuring the atomic-level stabilization. Ce2-NG demonstrates remarkable ORR performance, reaching a half-wave potential of 0.906 V, along with superior durability and strong resistance to methanol crossover. When employed as the cathode catalyst in a zinc–air battery (ZAB), the device exhibits an elevated open-circuit voltage and excellent long-term operational stability, clearly surpassing those of Pt/C + RuO2 counterparts. Operando spectroscopy combined with density functional theory supports the Ce2–N6 moiety as the active center, where dual-atom cerium cooperation drives charge redistribution, enhances *OH binding, and lowers the free energy change of the potential-determining step. This study introduces a controllable synthesis method for constructing rare-earth dual-atom catalysts, broadening the compositional landscape of atomically dispersed electrocatalysts for sustainable energy conversion.
SN  - 2041-6520
SN  - 2041-6539
ER  -