Light-induced water splitting (h nu-WS) for the production of hydrogen as a solar fuel is considered a promising sustainable strategy for the replacement of fossil fuels. An efficient system for h nu-WS involves a photoactive material that, upon shining light, is capable of separating and transferring charges to catalysts for the hydrogen and oxygen evolution processes. Covalent triazine-based frameworks (CTFs) represent an interesting class of 2D organic light-absorbing materials that have recently emerged thanks to their tunable structural, optical and morphological properties. Typically, catalysts (Cat) are metallic nanoparticles generated in situ after photoelectroreduction of metal precursors or directly drop-casted on top of the CTF material to generate Cat-CTF assemblies. In this work, the synthesis, characterization and photocatalytic performance of a novel hybrid material, Ru-CTF, is reported, based on a CTF structure featuring dangling pyridyl groups that allow the Ru-tda (tda is [2,2 ‘:6 ‘,2 ‘-terpyridine]-6,6 ‘-dicarboxylic acid) water oxidation catalyst (WOC) unit to coordinate via covalent bond. The Ru-CTF molecular hybrid material can carry out the light-induced water oxidation reaction efficiently at neutral pH, reaching values of maximum TOF of 17 h-1 and TONs in the range of 220 using sodium persulfate as a sacrificial electron acceptor. A CTF (Covalent Triazine Framework) functionalized with Ru(tda) based catalyst (tda is [2,2 ‘:6 ‘,2 ‘-terpyridine]-6,6 ‘-dicarboxylic acid) achieves light-induced water oxidation to dioxygen in the presence of sodium persulfate as sacrificial electron acceptor (SEA) reaching turnover numbers of 220 and turnover frequencies of 17 h-1, in the absence of Ag. This work puts forward the synergy between molecules and materials. image
Covalent Triazine-Based Frameworks with Ru-tda Based Catalyst Anchored via Coordination Bond for Photoinduced Water Oxidation
Small 2024, DOI: 10.1002/smll.202406375.