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原位合成 CuS@碳纳米复合材料及其在增强 2,4-DCP 的光芬顿降解中的应用。

In-situ synthesis of CuS@carbon nanocomposites and application in enhanced photo-fenton degradation of 2,4-DCP.

机构信息

Shandong Key Laboratory of Water Pollution Control and Resource Reuse, School of Environmental Science and Engineering, Shandong University, Qingdao, 266200, PR China.

Shandong Key Laboratory of Water Pollution Control and Resource Reuse, School of Environmental Science and Engineering, Shandong University, Qingdao, 266200, PR China; Shenzhen Research Institute of Shandong University, Shenzhen, 518057, China.

出版信息

Chemosphere. 2021 May;270:129295. doi: 10.1016/j.chemosphere.2020.129295. Epub 2020 Dec 29.

Abstract

Novel CuS nanoparticles embedded into carbon nanosheets (CuS@CNs) were prepared in situ by applying wheat straw cellulose/feather protein hydrogel beads as templates and were used to photocatalytically activate HO to degrade 2,4-dichlorphenol (2,4-DCP). The photo-Fenton catalytic properties of the nanocomposite catalysts obtained under different synthetic conditions, including different Cu concentrations, S concentrations and calcination temperatures, were evaluated. The results showed that CuS@CNs with 0.1 M Cu, 0.1 M S at 800 °C presented excellent photo-Fenton degradation performance for 2,4-DCP (25 mg/L) in the presence of HO and could remove 90% of 2,4-DCP in 2.5 h. The water quality parameters (pH, Cl, HCO, HPO and SO) exhibited different effects on the photocatalytic degradation process. The catalytic activity of the CuS@CNs used in the cycle could be recovered after thermal regeneration. Radical quenching and electron paramagnetic resonance (EPR) experiments confirmed that ·OH species were main active radicals contributing to the degradation of 2,4-DCP. The photocatalytic mechanism of CuS@CNs was also explored by photoelectrochemical (PEC) measurements and UV-vis diffuse reflectance spectroscopy (DRS). Incorporation of carbon nanosheets could significantly improve the separation of photogenerated charge carriers to stimulate pollutant degradation by CuS. Based on the detected intermediates, the degradation pathway of 2,4-DCP in the CuS@CNs/HO reaction system was also proposed.

摘要

新型 CuS 纳米颗粒嵌入碳纳米片中(CuS@CNs),通过应用小麦秸秆纤维素/羽毛蛋白水凝胶珠作为模板原位制备,并用于光催化激活 HO 以降解 2,4-二氯苯酚(2,4-DCP)。评价了在不同合成条件下(包括不同的 Cu 浓度、S 浓度和煅烧温度)获得的纳米复合材料催化剂的光芬顿催化性能。结果表明,在 HO 存在下,具有 0.1 M Cu、0.1 M S 和 800°C 的 CuS@CNs 对 25mg/L 的 2,4-DCP 具有优异的光芬顿降解性能,可在 2.5 h 内去除 90%的 2,4-DCP。水质参数(pH、Cl、HCO、HPO 和 SO)对光催化降解过程表现出不同的影响。CuS@CNs 在循环使用中的催化活性可以通过热再生恢复。自由基猝灭和电子顺磁共振(EPR)实验证实·OH 是主要的活性自由基,有助于 2,4-DCP 的降解。还通过光电化学(PEC)测量和紫外可见漫反射光谱(DRS)探索了 CuS@CNs 的光催化机制。碳纳米片的掺入可以显著提高光生载流子的分离,从而刺激 CuS 对污染物的降解。根据检测到的中间产物,还提出了 2,4-DCP 在 CuS@CNs/HO 反应体系中的降解途径。

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