Highly Perfluorinated Covalent Triazine Frameworks Derived from a Low-Temperature Ionothermal Approach Towards
Xian Suo1, Fengtao Zhang2, Zhenzhen Yang3
1Department of Chemistry, Institute for Advanced Materials and Manufacturing, University of Tennessee, Knoxville, TN, 37996, USA.
Angewandte Chemie (International Ed. in English)
|September 28, 2021
Summary
Researchers developed a new low-temperature method to create high-fluorine content perfluorinated covalent triazine frameworks (F-CTFs). These advanced F-CTFs show excellent performance in electrocatalytic CO2 reduction to CO.
Area of Science:
- Materials Science
- Catalysis
- Electrochemistry
Background:
- Perfluorinated covalent triazine frameworks (F-CTFs) offer unique properties for separation and catalysis.
- Existing synthesis methods yield low fluorine content F-CTFs due to harsh conditions and C-F bond cleavage.
Purpose of the Study:
- To develop a low-temperature synthesis for F-CTFs with high fluorine content.
- To investigate the performance of these F-CTFs in electrocatalytic CO2 reduction.
Main Methods:
- A low-temperature (275°C) ionothermal approach using tetrafluoroterephthalonitrile (TFPN) and Lewis superacids like zinc triflimide [Zn(NTf2)2].
- Characterization of F-CTF properties including fluorine content, surface area, and pore size.
Main Results:
- Achieved F-CTFs with high fluorine content (31 wt%) and surface area (367 m²/g).
- The synthesized F-CTF-1 demonstrated high hydrophobicity and superior electrocatalytic activity for CO2 to CO reduction.
- Achieved 95.7% Faradaic efficiency at -0.8 V and a current density of -141 mA/cm².
Conclusions:
- The low-temperature ionothermal method successfully produces high-fluorine content F-CTFs.
- These F-CTFs are highly effective metal-free electrocatalysts for CO2 reduction, outperforming existing catalysts.
Keywords:
CO2 electroreductionLewis superacidcovalent triazine frameworkfluorinatedionothermal procedureMore Related Videos
Related Concept Videos
01:26Thermal and Photochemical Electrocyclic Reactions: Overview
2.5K
Electrocyclic reactions are reversible reactions. They involve an intramolecular cyclization or ring-opening of a conjugated polyene. Shown below are two examples of electrocyclic reactions. In the first reaction, the formation of the cyclic product is favored. In contrast, in the second reaction, ring-opening is favored due to the high ring strain associated with cyclobutene formation.
2.5K
01:06Interfacial Electrochemical Methods: Overview
521
Interfacial electrochemical methods focus on the phenomena occurring at the boundary between an electrode and a solution, as opposed to bulk methods that concentrate on the solution's overall properties. These interfacial methods are classified as either static or dynamic based on the presence of a nonzero current in the electrochemical cell and the consistency of analyte concentrations. Static methods, such as potentiometry, measure the cell's potential without any significant current...
521
01:17Thermal Electrocyclic Reactions: Stereochemistry
2.2K
The stereochemistry of electrocyclic reactions is strongly influenced by the orbital symmetry of the polyene HOMO. Under thermal conditions, the reaction proceeds via the ground-state HOMO.
Selection Rules: Thermal Activation
Conjugated systems containing an even number of π-electron pairs undergo a conrotatory ring closure. For example, thermal electrocyclization of (2E,4E)-2,4-hexadiene, a conjugated diene containing two π-electron pairs, gives trans-3,4-dimethylcyclobutene.
Selection Rules: Thermal Activation
Conjugated systems containing an even number of π-electron pairs undergo a conrotatory ring closure. For example, thermal electrocyclization of (2E,4E)-2,4-hexadiene, a conjugated diene containing two π-electron pairs, gives trans-3,4-dimethylcyclobutene.
2.2K