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[Fe-CTFs] Crystalline Dual-Porous CTFs for Efficient Electrocatalysis
Summary:
The authors from Westlake University and Lanzhou University developed a crystalline dual-porous covalent triazine framework (Fe-CTF) with in situ generated Fe-N3 single-atom active sites, achieving remarkable electrocatalytic performance in oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), as well as superior performance in Zn-air batteries.
Background:
1. Crystalline porous materials such as covalent organic frameworks (COFs) and metal–organic frameworks (MOFs) have attracted significant interest due to their high surface areas and tunable structures. However, the synthesis of crystalline covalent triazine frameworks (CTFs) with diverse structures and single-atom active sites remains challenging. Previous methods often involve harsh conditions or complex procedures, limiting their practical applications.
2. The authors proposed a novel solvent-free FeCl3-catalyzed polymerization method to synthesize a crystalline dual-porous pyridine-based CTF (Fe-CTF) with Fe-N3 single-atom active sites, achieving high catalytic performance in electrochemical applications.
Research Content:
1. Synthesis:
The authors synthesized Fe-CTF using a solvent-free FeCl3-catalyzed polymerization of 2,6-pyridinedicarbonitrile (DCP). The FeCl3 acted as both a Lewis acid catalyst and an in situ coordination source for generating Fe-N3 active sites.
2. Characterizations:
1) BET surface area of Fe-CTF was 253.8 m²/g with dual pore sizes centered at 0.64 and 1.42 nm.
2) SEM images revealed a layered structure, while TEM images showed ultrathin nanosheets with a thickness of 1.6 nm.
3) XPS and XAFS analyses confirmed the presence of Fe-N3 single-atom active sites.
3. Application:
Fe-CTF nanosheets (Fe-CTF NSs) exhibited excellent ORR performance with an onset potential of 1.02 V and a half-wave potential of 0.902 V. In Zn-air batteries, Fe-CTF NSs achieved a specific capacity of 811 mAh/g and a power density of 230 mW/cm².
4. Mechanism:
Operando XAFS and DFT calculations revealed a dynamic and reversible evolution of Fe-N3 to Fe-N2 during the ORR process, which significantly enhanced the catalytic activity by facilitating electron transfer and improving adsorption of oxygen intermediates.
Outlook:
This research provides a new method for synthesizing crystalline CTFs with single-atom active sites, offering a promising platform for high-performance electrocatalysis. The findings highlight the potential of Fe-CTF NSs in energy conversion and storage applications, such as fuel cells and metal-air batteries.
Crystalline Dual-Porous Covalent Triazine Frameworks as a New Platform for Efficient Electrocatalysis
Authors: Kai Cui, Xiaoliang Tang, Xiaopei Xu, Manchang Kou, Pengbo Lyu, Yuxi Xu
DOI: 10.1002/anie.202317664
Link: https://onlinelibrary.wiley.com/doi/10.1002/anie.202317664
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