Gholami Peyman, Khataee Alireza, Bhatnagar Amit, Vahid Behrouz
Research Laboratory of Advanced Water and Wastewater Treatment Processes, Department of Applied Chemistry, Faculty of Chemistry, University of Tabriz, 51666-16471 Tabriz, Iran.
Department of Environmental and Biological Sciences, University of Eastern Finland, P.O. Box 1627, FI-70211 Kuopio, Finland.
ACS Appl Mater Interfaces. 2021 Mar 24;13(11):13072-13086. doi: 10.1021/acsami.0c21076. Epub 2021 Mar 15.
Synthesis of three-dimensional photocatalysts offers great potential for chemical conversion and hydrogen generation as appropriate solutions for environmental protection and energy shortage challenges. In this study, the magnetic WO@mesoporous carbon (M-WO@MC) was synthesized through the evaporation-induced self-assembly method applying diatom frustules as a natural template. Then, plasma modification was used to prepare the N-doped M-WO@MC (NM-WO@MC) with enhanced photocatalytic activity and durable performance. The WO was embedded in the conductive MC, which was also partially reduced by the carbon precursor within the heat-treatment procedure. The obtained M-WO@MC was treated by the plasma under an N atmosphere for the production of the final photocatalyst containing both the N-doped WO and MC. As a result, the NM-WO@MC had larger surface area (208.4 m g), narrower band gap (2.3 eV), more visible light harvesting, and confined electron-hole pairs recombination. The H generation rates of net WO nanorods and NM-WO@MC nanocomposite were estimated as 532 and 2765 μmol g h, respectively. Additionally, more than 90% of antibiotics (cephalexin, cefazolin and cephradine) degradation and 76% of total organic carbon elimination were obtained after 120 and 240 min of photocatalytic process under visible light irradiation. Eventually, more than eight intermediates were detected for each antibiotic degradation using the gas chromatography-mass spectrometer method, and based on the obtained results, the possible degradation pathways were suggested.
三维光催化剂的合成对于化学转化和制氢具有巨大潜力,有望成为应对环境保护和能源短缺挑战的合适解决方案。在本研究中,以硅藻壳作为天然模板,通过蒸发诱导自组装法合成了磁性WO@介孔碳(M-WO@MC)。然后,采用等离子体改性制备了具有增强光催化活性和持久性能的氮掺杂M-WO@MC(NM-WO@MC)。WO嵌入导电的MC中,在热处理过程中,MC也被碳前驱体部分还原。在氮气气氛下,对获得的M-WO@MC进行等离子体处理,以制备同时包含氮掺杂WO和MC的最终光催化剂。结果表明,NM-WO@MC具有更大的表面积(208.4 m²/g)、更窄的带隙(2.3 eV)、更强的可见光捕获能力以及受限的电子-空穴对复合。纯WO纳米棒和NM-WO@MC纳米复合材料的产氢速率分别估计为532和2765 μmol g⁻¹ h⁻¹。此外,在可见光照射下进行120和240分钟的光催化过程后,抗生素(头孢氨苄、头孢唑林和头孢拉定)的降解率超过90%,总有机碳的去除率达到76%。最终,使用气相色谱-质谱法对每种抗生素降解检测到了八种以上的中间体,并根据所得结果提出了可能的降解途径。