期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 34, 页码 13605-13615出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c04682
关键词
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资金
- National Natural Science Foundation of China [21802065]
- Entrepreneurial Research Team Program [2016ZT06N500]
- Shenzhen Peacock Plan [KQTD2016022620054656]
- Shenzhen Clean Energy Research Institute [CERI-KY-2019-003]
- DOE Office of Science [DE-AC02-06CH11357]
The study presents a novel design of iridium single atoms on Ni2P catalyst with excellent activity in OER. Experimental results and computational simulations highlight the crucial role of the optimized Ir-O-P/Ni-O-P bonding environment in enhancing OER activity. Additionally, the dynamic top-down evolution of the structure ensures the stability of the catalyst.
Single-atom catalysts (SACs) with 100% active sites have excellent prospects for application in the oxygen evolution reaction (OER). However, further enhancement of the catalytic activity for OER is quite challenging, particularly for the development of stable SACs with overpotentials <180 mV. Here, we report an iridium single atom on Ni2P catalyst (Ir-SA-Ni2P) with a record low overpotential of 149 mV at a current density of 10 mA.cm(-2) in 1.0 M KOH. The Ir-SA-Ni2P catalyst delivers a current density up to similar to 28-fold higher than that of the widely used IrO2 at 1.53 V vs RHE. Both the experimental results and computational simulations indicate that Ir single atoms preferentially occupy Ni sites on the top surface. The reconstructed Ir-O-P/Ni-O-P bonding environment plays a vital role for optimal adsorption and desorption of the OER intermediate species, which leads to marked enhancement of the OER activity. Additionally, the dynamic top-down evolution of the specific structure of the Ni@Ir particles is responsible for the robust single-atom structure and, thus, the stability property. This Ir-SA-Ni2P catalyst offers novel prospects for simplifying decoration strategies and further enhancing OER performance.
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