Spin‐Polarized PdCu–Fe<sub>3</sub>O<sub>4</sub> In‐Plane Heterostructures with Tandem Catalytic Mechanism for Oxygen Reduction Catalysis
Alloying has significantly upgraded the oxygen reduction reaction (ORR) of Pd-based catalysts through regulating the thermodynamics of oxygenated intermediates. However, the unsatisfactory activation ability of Pd-based alloys toward O<sub>2</sub> molecules limits further improvement of ORR kinetics. Herein, the precise synthesis of nanosheet assemblies of spin-polarized PdCu-Fe<sub>3</sub>O<sub>4</sub> in-plane heterostructures for drastically activating O<sub>2</sub> molecules and boosting ORR kinetics is reported. It is demonstrated that the deliberate-engineered in-plane heterostructures not only tailor the d-band center of Pd sites with weakened adsorption of oxygenated intermediates but also endow electrophilic Fe sites with strong ability to activate O<sub>2</sub> molecules, which make PdCu-Fe<sub>3</sub>O<sub>4</sub> in-plane heterostructures exhibit the highest ORR specific activity among the state-of-art Pd-based catalysts so far. In situ electrochemical spectroscopy and theoretical investigations reveal a tandem catalytic mechanism on PdCu-Fe<sub>3</sub>O<sub>4</sub>─Fe sites that initially activate molecular O<sub>2</sub> and generate oxygenated intermediates being transferred to Pd sites to finish the subsequent proton-coupled electron transfer steps.
Authors
- Fangxu Lin (ORCID: https://orcid.org/0009-0008-4589-6302)
- Guanghui Han (ORCID: https://orcid.org/0000-0001-8556-5497)
- Xiaoxing Ke (ORCID: https://orcid.org/0000-0003-2004-6906)
- Shaojun Guo (ORCID: https://orcid.org/0000-0003-4427-6837)
- Linke Fu (ORCID: https://orcid.org/0000-0001-6733-9031)
- Lu Li (ORCID: https://orcid.org/0000-0003-2105-1352)
- Chenhui Zhou (ORCID: https://orcid.org/0000-0002-5624-7577)
- Bingjun Xu (ORCID: https://orcid.org/0000-0002-2303-257X)
- Yongsheng Yu (ORCID: https://orcid.org/0000-0001-6626-5747)
- Fenyang Tian (ORCID: https://orcid.org/0000-0001-7114-849X)
- Shipeng Zhang (ORCID: https://orcid.org/0000-0003-4973-5086)
- Tao Lü (ORCID: https://orcid.org/0000-0001-5385-1034)
- Lin He (ORCID: https://orcid.org/0000-0001-9231-2615)
- Menggang Li (ORCID: https://orcid.org/0000-0003-1354-2645)
- Weiwei Yang (ORCID: https://orcid.org/0000-0002-7583-9682)
- Mingchuan Luo (ORCID: https://orcid.org/0000-0003-4936-238X)
Institutions
- Peking University (CN)
- Harbin Institute of Technology (CN)
- Beijing University of Technology (CN)
Publication Details
- Journal
- Advanced Materials
- Published
- 2024-10-23
- DOI
- https://doi.org/10.1002/adma.202412004
- Citations
- 29
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 2.97
Funders
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- Natural Science Foundation of Beijing Municipality
- National Key Research and Development Program of China
- National Science Fund for Distinguished Young Scholars