1. Design of ZIF-67-derived Fe, N and F co-doped porous carbon material and evaluation of its ORR and OER performance.
- Author
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He, Xinfu, Chang, Liaobo, Wu, Hongju, Liu, Guoyang, Zhang, Yating, and Zhou, Anning
- Subjects
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POROUS materials , *STRUCTURE-activity relationships , *METAL catalysts , *OXYGEN evolution reactions , *DOPING agents (Chemistry) , *HYDROGEN evolution reactions - Abstract
Addressing the low conductivity and porosity of ZIF-67-based oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts is a top priority. Noble metal-free highly active bifunctional catalysts F-N/FeCoNC 900 with three-dimensional interconnected porous structure and high electrical conductivity were successfully prepared by co-doping Fe, F, and N on the precursor ZIF-67. In terms of ORR performance, F-N/FeCoNC 900 has a high onset potential (E onset) of 0.97 V (vs. RHE), a half-wave potential (E 1/2) of 0.87 V (vs. RHE), and an ultimate current density (J L) of 5.7 mA cm−2, superior to commercially available Pt/C (0.95 V, 0.85 V, 5.3 mA cm−2). In addition, F-N/FeCoNC 900 provides high ORR activity with constant 4 electron transfer (n = 3.91–3.99) for methanol resistance and long-lasting stability (initial current retention of 96.32% after 21600 s). In terms of OER performance, F-N/FeCoNC 900 exhibits ultra-low overpotential (273 mV) and ultra-high Faraday efficiency (93%) at constant 4 (n = 3.91–3.99) electron transfer mode. This work provides a new pathway of doped ZIFs-derived composites as efficient bifunctional non-precious metal catalysts. [Display omitted] • Exquisite structure: The F-N/FeCoNC 900 catalyst has the following structural advantages:(a) A unique three-dimensional interconnected hierarchical porous structure is formed, which promotes the diffusion of oxygen and electrolytes and improves the utilization of internal active sites. (b) High specific surface area and high electrochemical active surface area enable highly exposed active centers, while abundant pyridinic nitrogen and graphitic nitrogen content overcome reaction barriers. • The highly efficient synergistic effect between composition and structure: The F-N/FeCoNC 900 catalyst has the following structure-activity relationship: (a) In view of the positive deep synergies among Co, Fe, F, N, and C atoms in the graphite lattice of F-N/FeCoNC 900 catalyst, reflecting F-N/FeCoNC 900 contains higher charge density to have smaller electrochemical impedance. (b) Abundant M-N x species serve as active sites with high structural stability and electrochemical activity. • This work not only delivers a low-cost and high-efficient ORR and OER catalyst, but also offers a new insight to develop a well-organized carbon hybrid electrocatalyst for various energy-related applications. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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