Fukushima Tomohiro, Ashizawa Daiki, Murakoshi Kei
Department of Chemistry, Faculty of Science, Hokkaido University Japan
RSC Adv. 2022 Apr 28;12(21):12967-12970. doi: 10.1039/d2ra01676a.
Understanding molecular processes at nanoparticle surfaces is essential for designing active photocatalytic materials. Here, we utilize nuclear magnetic resonance (NMR) spectroscopy to track photocatalytic hydrogen evolution using donor molecules and water isotopologues. Pt-TiO catalysts were prepared and used for isotopic hydrogen evolution reactions using alcohols as electron donors. H NMR monitoring revealed that evolution of the H and HD species is accompanied by the oxidation of donor molecules. The isotopic selectivity in the hydrogen evolution reaction gives rise to formal overpotential. Based on a comparison of the rates of hydrogen evolution and donor oxidation, we propose the use of ethanol as an efficient electron donor for the hydrogen evolution reaction without re-oxidation of radical intermediates.
了解纳米颗粒表面的分子过程对于设计活性光催化材料至关重要。在此，我们利用核磁共振（NMR）光谱法，通过供体分子和水同位素分子来追踪光催化析氢过程。制备了Pt-TiO催化剂，并以醇类作为电子供体用于同位素析氢反应。1H NMR监测表明，H和HD物种的析出伴随着供体分子的氧化。析氢反应中的同位素选择性导致了形式过电位。基于析氢速率和供体氧化速率的比较，我们提出使用乙醇作为析氢反应的有效电子供体，且不会使自由基中间体再氧化。
