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Photocatalytic degradation of diphenhydramine in aqueous solution by natural dolomite

机译:天然白云岩水溶液中二苯胺的光催化降解

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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 ~(1) O _(2) , ˙OH, and O _(2) ~(?) ˙ 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 ~(2+) by Fe ~(2+) , 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.
机译:天然白云石,廉价和广大的天然材料,被证明为潜在的异质光催化剂,用于在本研究中的模拟太阳能光下的水溶液中有效地除去二合一羟胺(DP)。在75分钟照射后,用白云石在催化剂中获得约65%的DP去除和14%的矿化。电子旋转共振分析和清除剂实验验证了〜(1)o _(2),˙OH和o _(2)〜(2)〜(?)〜在白云石体系中产生的是负责DP降解的主要反应物种。此外,使用与脱氧实验相结合的第一原理计算来阐明光催化机制。结果表明,通过Fe〜(2+)在部分取代Mg〜(2+)之后从绝缘体变为半导体的白云石,表明天然白云石可以用作光致抗蚀的半导体光催化剂。在照射下,光激发电子和孔分离并迁移到白云石的表面,随后反应形成反应性物质,导致DP降解。产品研究表明,DP的主要降解途径包括芳环的羟基化以及羟基根自由基介导的烷基胺侧链的氧化。这项工作表明,天然白云石可以应用于水和废水处理中作为有前途的光催化剂。

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