Oxygen Evolution Reaction of Amorphous/Crystalline Composites of NiFe(OH)<sub><i>x</i></sub>/NiFe<sub>2</sub>O<sub>4</sub>
Orbital structures are strongly correlated with catalytic performance, whereas their regulation strategy is still in pursuit. Herein, the Fe 3<i>d</i> and O 2<i>p</i> orbital hybridization was optimized by controlling the content of amorphous NiFe(OH)<sub><i>x</i></sub> (a-NiFe(OH)<sub><i>x</i></sub>), which was grown in situ on crystalline NiFe<sub>2</sub>O<sub>4</sub> (c-NiFe<sub>2</sub>O<sub>4</sub>) using an ultrasonic reduction method. The results of electron energy loss spectroscopy (EELS) and X-ray absorption spectra (XAS) revealed that the Fe-O<sub>a</sub> orbital hybridization in a-NiFe(OH)<sub><i>x</i></sub> is effectively strengthened by jointing with the adjacent oxygen (O<sub>c</sub>) in c-NiFe<sub>2</sub>O<sub>4</sub>, which is further confirmed by the higher antibonding orbital energies based on density functional theory (DFT) calculations. The resultant O<sub>a</sub>-Fe-O<sub>c</sub> at the composite interface leads to balanced adsorption and desorption energies. Accordingly, the optimal composite with strong Fe 3<i>d</i>-O 2<i>p</i> hybridization results in enhanced OER performance, and the overpotential is 150 mV, lower than that of the pristine sample. This work represents a promising approach to orbital hybridization via the introduction of an amorphous phase to construct highly efficient catalysts.
Authors
- Qian Zhu (ORCID: https://orcid.org/0000-0002-2806-3041)
- Songbo Li (ORCID: https://orcid.org/0000-0001-7603-3042)
- Na Liang (ORCID: https://orcid.org/0000-0001-8654-0531)
- Minmin Cai (ORCID: https://orcid.org/0000-0003-4048-6423)
- Keke Huang (ORCID: https://orcid.org/0000-0002-8995-2176)
- Zhibin Geng (ORCID: https://orcid.org/0009-0009-7719-736X)
- Huazheng Sai (ORCID: https://orcid.org/0000-0002-0514-4885)
- Ying Wang (ORCID: https://orcid.org/0000-0002-5437-8741)
- Yuan Zhang (ORCID: https://orcid.org/0000-0003-0670-2428)
- Lu Yao (ORCID: https://orcid.org/0000-0003-2743-758X)
- Xiaofeng Wu (ORCID: https://orcid.org/0000-0002-0044-896X)
- Shouhua Feng (ORCID: https://orcid.org/0000-0002-1070-1148)
- Mei Han
- Jianguo Cheng (ORCID: https://orcid.org/0000-0002-6510-8827)
- Yuan Fang (ORCID: https://orcid.org/0000-0002-7010-4740)
Institutions
- Mongolian University of Science and Technology (MN)
- Jilin University (CN)
- Chinese Academy of Sciences (CN)
- Inner Mongolia University of Science and Technology (CN)
- Changchun Institute of Applied Chemistry (CN)
- Jilin Medical University (CN)
- State Key Laboratory of Inorganic Synthesis and Preparative Chemistry
- State Key Laboratory of Rare Earth Resources Utilization
Publication Details
- Journal
- ACS Nano
- Published
- 2025-01-29
- DOI
- https://doi.org/10.1021/acsnano.4c18951
- Citations
- 21
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 15.34
Funders
- Education Department of Inner Mongolia Autonomous Region
- National Natural Science Foundation of China
- Baotou Science and Technology Bureau
- Hefei Science Center, Chinese Academy of Sciences