Rapid Surface Reconstruction of Pentlandite by High-Spin State Iron for Efficient Oxygen Evolution Reaction
Zhengyan Du
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
These authors contributed equally to this work.
Search for more papers by this authorZeshuo Meng
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
These authors contributed equally to this work.
Search for more papers by this authorXiliang Gong
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
Search for more papers by this authorZeyu Hao
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
Search for more papers by this authorXin Li
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
Search for more papers by this authorCorresponding Author
Haoteng Sun
Department of Chemistry, Brown University, Providence, RI 02912 USA
Search for more papers by this authorCorresponding Author
Prof. Xiaoying Hu
College of Science and Laboratory of Materials Design and Quantum Simulation, Changchun University, Changchun, 130022 China
Search for more papers by this authorCorresponding Author
Prof. Shansheng Yu
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
Search for more papers by this authorCorresponding Author
Prof. Hongwei Tian
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
Search for more papers by this authorZhengyan Du
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
These authors contributed equally to this work.
Search for more papers by this authorZeshuo Meng
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
These authors contributed equally to this work.
Search for more papers by this authorXiliang Gong
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
Search for more papers by this authorZeyu Hao
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
Search for more papers by this authorXin Li
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
Search for more papers by this authorCorresponding Author
Haoteng Sun
Department of Chemistry, Brown University, Providence, RI 02912 USA
Search for more papers by this authorCorresponding Author
Prof. Xiaoying Hu
College of Science and Laboratory of Materials Design and Quantum Simulation, Changchun University, Changchun, 130022 China
Search for more papers by this authorCorresponding Author
Prof. Shansheng Yu
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
Search for more papers by this authorCorresponding Author
Prof. Hongwei Tian
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun, 130012 China
Search for more papers by this authorAbstract
Triggering rapid reconstruction reactions holds the potential to approach the theoretical limits of the oxygen evolution reaction (OER), and spin state manipulation has shown great promise in this regard. In this study, the transition of Fe spin states from low to high was successfully achieved by adjusting the surface electronic structure of pentlandite. In situ characterization and kinetic simulations confirmed that the high-spin state of Fe promoted the accumulation of OH− on the surface and accelerated electron transfer, thereby enhancing the kinetics of the reconstruction reaction. Furthermore, theoretical calculations revealed that the lower d-band center of high-spin Fe optimized the adsorption of active intermediates, thereby enhancing the reconstruction kinetics. Remarkably, pentlandites with high-spin Fe exhibited ultra-low overpotential (245 mV @ 10 mA cm−2) and excellent stability. These findings provided new insights for the design and fabrication of highly active OER electrocatalysts.
Conflict of interest
The authors declare no conflict of interest.
Open Research
Data Availability Statement
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