Xia Jiawei, Mark Gabriel, Volokh Michael, Fang Yuanxing, Chen Haiqun, Wang Xinchen, Shalom Menny
Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, Changzhou University, Changzhou, Jiangsu Province 213164, China.
Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev, Beer-Sheva 8410501, Israel.
Nanoscale. 2021 Dec 2;13(46):19511-19517. doi: 10.1039/d1nr06974h.
Intrinsic defects and structural properties are two main factors influencing the photocatalytic performance of carbon nitride (CN) materials. Here, photoactive porous CN rods are fabricated through the thermal condensation of melem-based hexagonal supramolecular assemblies. To overcome the poor solubility of melem, we exfoliate the bulk melem using hydrochloric acid. The latter allows good dispersibility of the monomer in an aqueous medium, leading to the formation of H-bond bridged supramolecular assembly with good regularity in both size and rod-like morphology. After thermal condensation, a well-ordered structure of porous CN rods with fewer defects due to the high thermal stability of the melem-based supramolecular assembly is obtained. The new CN materials have a high specific surface area, good light-harvesting properties, and enhanced charge separation and migration. The optimal CN material exhibits excellent photocatalytic activity and durability towards hydrogen evolution reaction (HER) and CO reduction reaction (CORR, with good selectivity).
本征缺陷和结构性质是影响氮化碳(CN)材料光催化性能的两个主要因素。在此,通过基于蜜勒胺的六边形超分子组装体的热缩合制备了光活性多孔CN棒。为了克服蜜勒胺溶解性差的问题,我们用盐酸对块状蜜勒胺进行剥离。后者使单体在水性介质中具有良好的分散性,导致形成尺寸和棒状形态具有良好规则性的氢键桥连超分子组装体。热缩合后,由于基于蜜勒胺的超分子组装体具有高热稳定性,获得了缺陷较少的有序多孔CN棒结构。这种新型CN材料具有高比表面积、良好的光捕获性能以及增强的电荷分离和迁移能力。最佳的CN材料对析氢反应(HER)和CO还原反应(CORR,具有良好的选择性)表现出优异的光催化活性和耐久性。