Axial Coordination Tuning Fe Single-atom Catalysts for Boosting H2O2 Activation

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Axial Coordination Tuning Fe Single-atom Catalysts for Boosting H2O2 Activation
Title:
Axial Coordination Tuning Fe Single-atom Catalysts for Boosting H2O2 Activation
Journal Title:
Applied Catalysis B: Environmental
Publication Date:
22 September 2022
Citation:
Fu, H., Wei, J., Chen, G., Xu, M., Liu, J., Zhang, J., Li, K., Xu, Q., Zou, Y., Zhang, W., Xi, S., Chen, X., Li, S., & Ling, L. (2022). Axial Coordination Tuning Fe Single-atom Catalysts for Boosting H2O2 Activation. Applied Catalysis B: Environmental, 122012. https://doi.org/10.1016/j.apcatb.2022.122012
Abstract:
Precisely regulating the coordination microenvironment of single-atom catalysts (SACs) to achieve enhanced reactivity is significant and desired but still in its infancy. Herein, a coordination-tuned and pyrolysis-free strategy is reported for the fabrication of a Fenton-like SAC containing the axial five-coordinated configuration (Fe–N5). The N species on the N-doped graphene act as anchoring points for iron phthalocyanine (a typical Fe–N4 complex) to obtain isolated Fe–N5 sites, which significantly modulates the electronic state of Fe atoms and lowers the H2O2 activation barrier for •OH production. Moreover, the enriched pyridinic N serve as contaminant adsorption sites shortening •OH diffusion distance, establishing a dual-site reaction mechanism with Fe–N5 sites. As such, the Fe–N5 catalyst exhibits exceptional Fenton activity towards catalytic oxidation of phenol (k= 0.180 min−1). Our work unravels the dependence of Fenton activity on the single-atom coordination environment and provides a platform for precise engineering of SACs.
License type:
Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0)
Funding Info:
This research / project is supported by the Ministry of Education - Academic Research Fund Tier 2
Grant Reference no. : MOE-T2EP10220-0005

This research / project is supported by the Ministry of Education - Academic Research Fund Tier 1
Grant Reference no. : RG8/20

China Scholarship Council (202106260199), the Fundamental Research Funds for Central Universities (No. 22120200178
Description:
ISSN:
0926-3373
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