Baranowska Daria, Zielinkiewicz Klaudia, Mijowska Ewa, Zielinska Beata
Department of Nanomaterials Physicochemistry, Faculty of Chemical Technology and Engineering, West Pomeranian University of Technology in Szczecin, Piastow Ave. 42, 71-065, Szczecin, Poland.
Center for Advanced Materials and Manufacturing Process Engineering (CAMMPE), West Pomeranian University of Technology, Szczecin, Poland.
Sci Rep. 2024 Jan 23;14(1):1998. doi: 10.1038/s41598-024-52593-4.
Photocatalytic hydrogen evolution holds great promise for addressing critical energy and environmental challenges, making it an important area in scientific research. One of the most popular photocatalysts is graphitic carbon nitride (gCN), which has emerged as a noteworthy candidate for hydrogen generation through water splitting. However, ongoing research aims to enhance its properties for practical applications. Herein, we introduce a green approach for the fabrication of porous few-layered gCN with surface modifications (such as oxygen doping, carbon deposition, nitrogen defects) with promoted performance in the hydrogen evolution reaction. The fabrication process involves a one-step solvothermal treatment of bulk graphitic carbon nitride (bulk-gCN) in the presence of different sugars (glucose, sucrose, and fructose). Interestingly, the conducted time-dependent process revealed that porous gCN exfoliated in the presence of fructose at 180 °C for 6 h (fructose_6h) exhibits a remarkable 13-fold promotion of photocatalytic hydrogen evolution compared to bulk-gCN. The studied materials were extensively characterized by microscopic and spectroscopic techniques, allowing us to propose a reaction mechanism for hydrogen evolution during water-splitting over fructose_6h. Furthermore, the study highlights the potential of employing a facile and environmentally friendly fructose-assisted solvothermal process to improve the efficiency and stability of catalysts based on graphitic carbon nitride.
光催化析氢在应对关键的能源和环境挑战方面具有巨大潜力，使其成为科学研究的一个重要领域。最受欢迎的光催化剂之一是石墨相氮化碳（gCN），它已成为通过水分解制氢的一个值得关注的候选材料。然而，目前的研究旨在改善其性能以用于实际应用。在此，我们介绍一种绿色方法来制备具有表面改性（如氧掺杂、碳沉积、氮缺陷）的多孔少层gCN，其在析氢反应中具有提升的性能。制备过程涉及在不同糖类（葡萄糖、蔗糖和果糖）存在下对块状石墨相氮化碳（块状gCN）进行一步溶剂热处理。有趣的是，进行的时间依赖性过程表明，在180℃下果糖存在6小时（果糖_6h）时剥落的多孔gCN与块状gCN相比，光催化析氢性能显著提高了13倍。通过显微镜和光谱技术对所研究的材料进行了广泛表征，这使我们能够提出在果糖_6h上进行水分解析氢过程的反应机理。此外，该研究突出了采用简便且环境友好的果糖辅助溶剂热过程来提高基于石墨相氮化碳的催化剂的效率和稳定性的潜力。
