Engineering Research Center of Nano-Geomaterials of Ministry of Education, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, China.
Engineering Research Center of Nano-Geomaterials of Ministry of Education, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, China.
J Colloid Interface Sci. 2022 Feb;607(Pt 2):1527-1539. doi: 10.1016/j.jcis.2021.09.112. Epub 2021 Sep 22.
The traditional heterogeneous photo-Fenton reaction was mainly restricted by the fewer surface-active sites, low Fe/Fe transformation and HO activation efficiency of catalyst. This work designed and fabricated the efficient photo-Fenton Schottky catalysts via a facile electrostatic self-assembly of metallic FeN nanoparticles scattering on the surface of red g-CN (ultrathin porous oxygen-doped 2D g-CN nanosheets). The porous morphology and exceptional electrical structure of red g-CN endowed more active sites and facilitated the photoexcited charge separation. Benefitting from the Schottky effect and unique dimensional coupling structure, the strong visible light absorption and fast spatial charge transfer were realized in the Schottky junction system. More strikingly, FeN as an efficient co-catalyst was in favor of the trap and export of e, leading to the Fe/Fe transformation and HO activation during the photo-Fenton process. Accordingly, the as-prepared catalysts revealed outstanding activity in photo-Fenton like degradation of tetracycline (TC) although under 5 W white LED light irradiation. Furthermore, the reasonable degradation pathway of TC and corresponding toxicity of the intermediates, as well as the photo-Fenton catalytic mechanism were interpreted and discussed in detail. This study would be a great aid in the development of various Schottky catalysts for heterogeneous photo-Fenton-based environmental remediation systems.
传统的非均相类芬顿反应主要受到催化剂表面活性位点较少、Fe/Fe 转化和 HO 激活效率低的限制。本工作通过金属 FeN 纳米颗粒在红色 g-CN(超薄多孔氧掺杂二维 g-CN 纳米片)表面的简易静电自组装设计并制备了高效的类芬顿肖特基催化剂。红色 g-CN 的多孔形态和优异的电子结构赋予了更多的活性位点,并促进了光激发电荷分离。受益于肖特基效应和独特的维度耦合结构,在肖特基结系统中实现了强可见光吸收和快速空间电荷转移。更引人注目的是,FeN 作为一种有效的共催化剂有利于 e 的捕获和导出,从而促进了光芬顿过程中的 Fe/Fe 转化和 HO 激活。因此,尽管在 5 W 白色 LED 光照射下,所制备的催化剂在四环素(TC)的类芬顿光降解中表现出优异的活性。此外,详细解释和讨论了 TC 的合理降解途径和相应中间体的毒性以及光芬顿催化机制。这项研究将极大地有助于开发用于基于非均相类芬顿的环境修复系统的各种肖特基催化剂。