Facile Method for the Preparation of Covalent Triazine Framework coated Monoliths as Catalyst Support: Applications in C1 Catalysis

Abstract

A quasi chemical vapor deposition method for the manufacture of well-defined covalent triazine framework (CTF) coatings on cordierite monoliths is reported. The resulting supported porous organic polymer is an excellent support for the immobilization of two different homogeneous catalysts: (1) an IrCp*-based catalyst for the hydrogen production from formic acid and (2) a Pt-based catalyst for the direct activation of methane via Periana chemistry. The immobilized catalysts display a much higher activity in comparison with the unsupported CTF operated in slurry because of improved mass transport. Our results demonstrate that CTF-based catalysts can be further optimized by engineering at different length scales.

Covalent Triazine‐based Frameworks—Tailor‐made Catalysts and Catalyst Supports for Molecular and Nanoparticulate Species

“… Schematic illustration of the coating procedure by Bavykina et al . (top) and SEM images (bottom) of (A) the bare cordierite, (B–E) the CTF‐coated monolith and (F) close‐up of the wall of the CTF‐coated monolith.…”

“…Just recently,B avykina et al developed am ethodt od esign CTFbased catalysts on both micro-and macroscopic level via a facile dip-coating approach (Figure2). [95] In this approach, cordierite monoliths (2 MgO·2 Al 2 O 3 ·5 SiO 2 ,6 00 cells per square inch, channel diameter 0.93 mm, wall thickness 0.11mm, open frontal area 80 %, wall porosity 0.33) are dipped into as olution of monomer and ZnCl 2 in acetone and stirred overnight to obtain ac oating, which was dried and subjected to ionother-mal polymerization conditions (500 8C, 10 h). After washing with HCl, NH 4 OH and THF to remove ZnCl 2 and organic residues, approximately 15 wt %o fC TF coating on the monolith was achieved, as indicated by thermogravimetric analysis (TGA).…”

Development of Covalent Triazine Frameworks as Heterogeneous Catalytic Supports

“…However, the porosity of the CTFs could not be completely preserved upon formulation. To address this issue, and the diffusion limitations derived from heterogenization, Gascon and co-workers introduced a well-defined CTF coated on cordierite monoliths, prepared by quasi chemical vapor deposition (Figure 5) [45]. These coatings are stable, easy to handle, and can be used in the same way as the parent material to coordinate metal complexes.…”

“…( Left ) Representation of the coating procedure step. ( Right ) SEM micrograph of ( A ) CTF powders ( B–E ), CTF-coated monolith ( F ) view on the wall of a CTF-coated monolith (Adapted with permission from [45]. Copyright 2017, American Chemical Society).…”

Continuous Hydrogenation of Carbon Dioxide to Formic Acid and Methyl Formate by a Molecular Iridium Complex Stably Heterogenized on a Covalent Triazine Framework

“…Analytical techniques such as IR [16d] and EDX [18] have been used to detect the presence of the metal complex on the CTF, suggesting its direct coordination. In literature, X-ray photoelectron spectroscopy (XPS) has been widely employed to study the chemical state of the metal center, carbon and/or nitrogen.…”