Salati Martina, Dorchies Florian, Wang Jia-Wei, Ventosa Marta, González-Carrero Soranyel, Bozal-Ginesta Carlota, Holub Jan, Rüdiger Olaf, DeBeer Serena, Gimbert-Suriñach Carolina, Durrant James R, Ertem Mehmed Z, Gil-Sepulcre Marcos, Llobet Antoni
Institute of Chemical Research of Catalonia (ICIQ), Barcelona Institute of Science and Technology (BIST), Tarragona, 43007, Spain.
Department of Chemistry, Centre for Processable Electronics, Imperial College London, Wood Lane, London, W12 0BZ, UK.
Small. 2025 Feb;21(7):e2406375. doi: 10.1002/smll.202406375. Epub 2024 Sep 5.
Light-induced water splitting (hν-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 hν-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 and TONs in the range of 220 using sodium persulfate as a sacrificial electron acceptor.
光诱导水分解（hν-WS）用于生产作为太阳能燃料的氢气，被认为是一种有前景的替代化石燃料的可持续策略。一个高效的hν-WS系统涉及一种光活性材料，该材料在光照下能够将电荷分离并转移到用于析氢和析氧过程的催化剂上。共价三嗪基框架（CTF）是一类有趣的二维有机光吸收材料，由于其可调的结构、光学和形态特性，最近才出现。通常，催化剂（Cat）是金属前驱体经光电还原后原位生成的金属纳米颗粒，或直接滴铸在CTF材料顶部以生成Cat-CTF组件。在这项工作中，报道了一种新型杂化材料Ru-CTF的合成、表征和光催化性能，该材料基于一种具有悬挂吡啶基的CTF结构，该结构允许Ru-tda（tda是[2,2':6',2''-三联吡啶]-6,6''-二羧酸）水氧化催化剂（WOC）单元通过共价键进行配位。Ru-CTF分子杂化材料在中性pH值下能够高效地进行光诱导水氧化反应，以过硫酸钠作为牺牲电子受体时，最大TOF值达到17 h，TONs在220范围内。
