Song Lihong, Yi Chunlin, Wu Qingfeng, Li Zhaohui, Zhang Weibin, Hong Hanlie
School of Physics and Optoelectronic Engineering, Yangtze University 1 Nanhuan Road Jingzhou Hubei 434023 China
Department of Geosciences, University of Wisconsin-Parkside 900 Wood Road, Kenosha WI 53144 USA.
RSC Adv. 2020 Oct 21;10(63):38663-38671. doi: 10.1039/d0ra07533g. eCollection 2020 Oct 15.
Natural dolomite, an inexpensive and vastly available natural material, was demonstrated as a potential heterogeneous photocatalyst for the efficient removal of diphenhydramine (DP) from aqueous solution under simulated solar light in this study. About 65% DP removal and 14% mineralization were achieved with dolomite as a catalyst after 75 min irradiation. The electron spin resonance analysis and scavenger experiments verified that O, ˙OH, and O ˙ produced in the dolomite system were the main reactive species responsible for DP degradation. Furthermore, first-principle calculations combined with deoxygenation experiments were employed to elucidate the photocatalytic mechanism. The results revealed that the dolomite changed from an insulator to a semiconductor after partial substitution of Mg by Fe, suggesting that natural dolomite could act as a semiconductor photocatalyst in photoreactions. Under irradiation, photo-excited electrons and holes separate and migrate to the surface of dolomite, and subsequently react to form reactive species resulting in the DP degradation. Product studies demonstrated that the main degradation pathways of DP included hydroxylation of the aromatic ring as well as hydroxyl radical mediated oxidation of the alkylamine side chain. This work indicated that natural dolomite could be applied in water and wastewater treatment as a promising photocatalyst.
天然白云石是一种廉价且储量丰富的天然材料,本研究表明其作为一种潜在的多相光催化剂,在模拟太阳光下可有效去除水溶液中的苯海拉明(DP)。以白云石为催化剂,光照75分钟后,DP的去除率约为65%,矿化率为14%。电子自旋共振分析和清除剂实验证实,白云石体系中产生的O、˙OH和O˙是导致DP降解的主要活性物种。此外,采用第一性原理计算结合脱氧实验来阐明光催化机理。结果表明,Fe部分取代Mg后,白云石由绝缘体转变为半导体,这表明天然白云石在光反应中可作为半导体光催化剂。在光照下,光激发电子和空穴分离并迁移到白云石表面,随后发生反应形成活性物种,导致DP降解。产物研究表明,DP的主要降解途径包括芳环羟基化以及羟基自由基介导的烷基胺侧链氧化。这项工作表明,天然白云石作为一种有前景的光催化剂可应用于水和废水处理。