Well-Defined Co<sub>2</sub> Dual-Atom Catalyst Breaks Scaling Relations of Oxygen Reduction Reaction
The 4-electron oxygen reduction reaction (ORR) under alkaline conditions is central to the development of non-noble metal-based hydrogen fuel cell technologies. However, the kinetics of ORR are constrained by scaling relations, where the adsorption free energy of *OOH is intrinsically linked to that of *OH with a nearly constant difference larger than the optimal value. In this study, a well-defined binuclear Co<sub>2</sub> complex was synthesized and adsorbed onto carbon black, serving as a model dual-atom catalyst. This catalyst achieved a record half-wave potential of 0.972 V versus the reversible hydrogen electrode in an alkaline electrolyte. Density functional theory simulations and in situ infrared spectroscopy revealed that the dual-atom site stabilizes the *OOH intermediate through bidentate coordination, thereby reducing the free energy gap between *OOH and *OH. By altering the adsorption configuration of *OOH on the dual-atom site, the scaling relations are effectively disrupted, leading to a significant enhancement in ORR activity.
Authors
- Linke Yu
- Meng-Ting Liu
- Jun Gu (ORCID: https://orcid.org/0000-0002-4902-2433)
- Yiwei Zheng (ORCID: https://orcid.org/0000-0002-6722-5883)
- Hao Ming Chen (ORCID: https://orcid.org/0000-0002-7480-9940)
- Xian Yue (ORCID: https://orcid.org/0000-0002-7264-8928)
- Xile Hu (ORCID: https://orcid.org/0000-0001-8335-1196)
- Jianzhao Peng (ORCID: https://orcid.org/0000-0002-5684-331X)
- Qidi Sun (ORCID: https://orcid.org/0000-0002-0864-9416)
- Lei Li (ORCID: https://orcid.org/0000-0003-2882-2447)
- Fuzhi Li (ORCID: https://orcid.org/0000-0003-1413-0319)
Institutions
- Sinopec (China) (CN)
- American Petroleum Institute (US)
- Petroleum University of Technology (IR)
- National Taiwan University (TW)
- City University of Hong Kong (HK)
- Southern University of Science and Technology (CN)
- Institute of Molecular Functional Materials (CN)
- Petroleum Technology Company (Norway) (NO)
- Chemical Synthesis Lab (SG)
- École Polytechnique Fédérale de Lausanne (CH)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2024-12-11
- DOI
- https://doi.org/10.1021/jacs.4c12705
- Citations
- 74
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 7.58
Funders
- National Natural Science Foundation of China
- Department of Education of Guangdong Province
- Shenzhen Science and Technology Innovation Program