期刊
CHEMICAL ENGINEERING JOURNAL
卷 440, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.135956
关键词
Electrocatalytic CO2 reduction; Ni single-atom catalyst; Coordination environment; Metal nanoparticles; Density functional theory calculation
资金
- National Natural Science Foundation of China [22178116, 21978097]
- Shanghai Pujiang Program [21PJD019]
- Fundamental Research Funds for the Central Universities [222201817001, 50321041918013, 50321042017001]
This study successfully develops Ni SACs with well-defined low-coordination nickel-nitrogen sites via a facile sacrificial template method. The Ni single atoms coordinated by three N atoms exhibit excellent activity and selectivity for electrocatalytic CO2 reduction, suggesting a new approach for efficient CO2 conversion.
Single-atom catalysis has been considered as a powerful approach for CO2 reduction reaction (CO2RR) to achieve efficient resource conversion and carbon neutrality. The electrocatalytic activity of single-atom catalysts (SACs) is closely related to the local coordination environment. Herein, Ni SACs with well-defined low-coordination nickel-nitrogen sites (denoted as Ni-SA@N-3-C) have been successfully developed via a facile sacrificial template method. XAS results reveal that the coordination environment of the atomically dispersed Ni active sites can be controlled by the pyrolysis temperature. Significantly, Ni-SA@N-3-C displays remarkably excellent activity toward electrocatalytic CO2RR with CO Faradaic efficiency (FECO) of 96.0% at -0.83 V vs. RHE and remains high FECO exceeding 90% over a broad potential range from -0.63 to -0.93 V vs. RHE, outperforming those of Ni-SA@N-4-C and Ni-NP@NC. More importantly, Ni-SA@N-3-C exhibits an excellent CO selectivity of 99.2% with a considerable current density of -160 mA cm(-2) in the flow cell reactor. Density functional theory (DFT) calculations further suggest that the Ni single atoms coordinated by three N atoms possesses a suitable free energy barrier for *COOH formation and *CO desorption, thereby exhibiting the most excellent CO2RR performance. This study sheds a new light on the design of SACs with controllable coordination structures for CO2RR.
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