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采用天然黄铁矿和有机酸的绿色太阳能光芬顿法,在原位生成 HO,用于降解卡马西平。

A green solar photo-Fenton process for the degradation of carbamazepine using natural pyrite and organic acid with in-situ generated HO.

机构信息

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, PR China; The Innovation Team for Volatile Organic Compounds Pollutants Control and Resource Utilization of Yunnan Province, Kunming 650500, PR China; The Higher Educational Key Laboratory for Odorous Volatile Organic Compounds Pollutants Control of Yunnan Province, Kunming 650500, PR China.

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, PR China.

出版信息

Sci Total Environ. 2021 Aug 25;784:147187. doi: 10.1016/j.scitotenv.2021.147187. Epub 2021 Apr 18.

Abstract

Pyrite is widely used in Fenton reaction for degradation of pollutants and exhibits great potential for environmental remediation, however, its efficiency is greatly compromised by extra HO and pH adjustment. Herein, a pyrite based green solar photo-Fenton system for carbamazepine (CBZ) treatment is constructed, involving the use of simulated sunlight and natural organic acids with in situ-generated HO and without extra pH adjustment. The addition of organic acids including tartaric acid (TA), citric acid (CA), and ascorbic acid (AA) can form complex with iron in pyrite, which promotes the Fe(II) dissolution. Upon irradiation, pyrite could be excited to produce photoelectrons, which would reduce oxygen to produce HO through a two-step route assisted by organic acids. The simulated sunlight and organic acids promoted the in-situ production of HO and Fe(II) species, sustaining an efficient Fenton reaction. This produced massive hydroxyl radical (OH), as demonstrated by the active species capture experiment. Compared with no degradation of CBZ under pure pyrite, the degradation efficiency of CBZ reached to 70%, 60%, and 53% in pyrite/TA, pyrite/CA, pyrite/AA within 30 min under simulated solar light irradiation, respectively. This work reports the first use of natural pyrite, a typical Fe-mineral semiconductor, to produce OH for CBZ degradation through natural additive assisted Fenton reaction excluding the adding extra HO and pH adjustment.

摘要

黄铁矿在芬顿反应中被广泛用于降解污染物,在环境修复方面具有很大的潜力,但其效率受到额外的 HO 和 pH 调节的极大影响。本文构建了一种基于黄铁矿的绿色太阳能光芬顿体系用于卡马西平(CBZ)的处理,涉及使用模拟太阳光和天然有机酸原位生成 HO ,无需额外的 pH 调节。添加包括酒石酸(TA)、柠檬酸(CA)和抗坏血酸(AA)在内的有机酸可以与黄铁矿中的铁形成配合物,促进 Fe(II)的溶解。在光照下,黄铁矿可以被激发产生光电子,这些光电子在有机酸的辅助下通过两步途径还原氧气产生 HO。模拟太阳光和有机酸促进了 HO 和 Fe(II)物种的原位生成,维持了高效的芬顿反应。这产生了大量的羟基自由基(OH),如活性物质捕获实验所证明的。与纯黄铁矿下 CBZ 没有降解相比,在模拟太阳光照射下,黄铁矿/TA、黄铁矿/CA、黄铁矿/AA 中 30 分钟内 CBZ 的降解效率分别达到 70%、60%和 53%。本工作首次报道了天然黄铁矿(一种典型的 Fe 矿物半导体)通过自然添加剂辅助芬顿反应产生 OH 用于 CBZ 降解,无需额外添加 HO 和 pH 调节。

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