College of Safety and Environmental Engineering, Shandong University of Science and Technology, Qingdao, 266590, PR China; Environment Research Institute, Shandong University, Qingdao, 266237, PR China; Institute of Yellow River Delta Earth Surface Processes and Ecological Integrity, Shandong University of Science and Technology, PR China.
College of Safety and Environmental Engineering, Shandong University of Science and Technology, Qingdao, 266590, PR China.
Environ Res. 2022 May 1;207:112623. doi: 10.1016/j.envres.2021.112623. Epub 2022 Jan 4.
Metal-free photocatalysts for high efficient photocatalytic degradation of pollutants have attracted growing concern in recent years. Herein, relying on density functional theory (DFT) calculations, boron and phosphorus doped CN layers were explored for the potential of utilization as photocatalysts for 4, 5-dichloroguaiacol (4, 5-DCG) removal. Our computations revealed that the adsorption energy of 4, 5-DCG on B@N-doped CN layers were 26.56 kcal mol, and the ΔG of initial reactions of 4, 5-DCG with OH were also reduced onto the B@N-doped CN substrates. The band gap of B@N-doped CN was 2.27 eV. The obtained results showed that the doping of boron atom into CN layer narrows bandgap, and retains well catalytic performance and adsorption properties. Hence, B@N-doped CN layer is a promising photocatalyst for organic pollutants removal. Possible degradation pathways of 4, 5-DCG and aquatic toxicity assessment during degradation were also carried out. Products with higher toxicity would be formed and the transformation products were still toxic to three nutrient levels of aquatic organisms (green algae, fish, and daphnia).
近年来，无金属光催化剂在高效光催化降解污染物方面受到了越来越多的关注。在此，我们借助密度泛函理论（DFT）计算，研究了硼和磷掺杂 CN 层作为光催化剂用于去除 4,5-二氯愈创木酚（4,5-DCG）的潜力。我们的计算表明，4,5-DCG 在 B@N 掺杂 CN 层上的吸附能为 26.56 kcal/mol，并且 4,5-DCG 与 OH 的初始反应的 ΔG 也降低到 B@N 掺杂 CN 基底上。B@N 掺杂 CN 的能带隙为 2.27 eV。研究结果表明，硼原子掺杂到 CN 层中可以缩小带隙，同时保持良好的催化性能和吸附性能。因此，B@N 掺杂 CN 层是一种很有前途的用于去除有机污染物的光催化剂。还进行了 4,5-DCG 的可能降解途径和降解过程中的水生毒性评估。会形成毒性更高的产物，并且转化产物对三种水生生物（藻类、鱼类和水蚤）的营养水平仍具有毒性。
