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石墨相氮化碳(g-CN)作为一种高效的无金属类芬顿催化剂用于降解有机污染物:被忽视的非光催化活性。

Graphitic carbon nitride (g-CN) as an efficient metal-free Fenton-like catalyst for degrading organic pollutants: the overlooked non-photocatalytic activity.

机构信息

School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, China E-mail:

School of Ecology and Environment, Zhengzhou University, Zhengzhou 450001, China.

出版信息

Water Sci Technol. 2020 Feb;81(3):518-528. doi: 10.2166/wst.2020.129.

DOI:10.2166/wst.2020.129
PMID:32385205
Abstract

Graphitic carbon nitride (g-CN) has attracted a large amount of research, mainly being used as a photocatalyst, but its Fenton-like catalytic performance has been overlooked. In this paper, the dark Fenton-like catalytic performance of g-CN was evaluated by degrading rhodamine B over a wide pH range. The results showed that the g-CN, which was synthesized by conventional urea pyrolysis without any modification, was an efficient metal-free heterogeneous Fenton-like catalyst. The highest activity occurred under a weakly alkaline condition of about pH 10. The experiment of catalyst recycling indicated that g-CN had long-term stability. The reactive oxidizing species of HO·, generated by the g-CN activating HO, was identified by EPR and further supported by a scavenging experiment of HO· using isopropanol as the scavenger. The HNO oxidation of g-CN resulted in catalytic deactivation, implying the catalytic activity originated from the surface reduced groups of g-CN. The structure of synthesized g-CN before and after the HNO oxidation was characterized by X-ray diffraction, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy, and a possible catalytic mechanism was proposed.

摘要

石墨相氮化碳(g-CN)引起了大量研究,主要用作光催化剂,但它类似芬顿的催化性能却被忽视了。本文通过在较宽的 pH 范围内降解罗丹明 B 来评估 g-CN 的暗芬顿类似催化性能。结果表明,通过常规尿素热解合成而未经任何修饰的 g-CN 是一种高效的无金属异相芬顿类似催化剂。在约 pH 10 的弱碱性条件下活性最高。催化剂回收实验表明 g-CN 具有长期稳定性。通过电子顺磁共振(EPR)鉴定了 g-CN 激活 HO 产生的反应性氧化物种 HO·,并通过使用异丙醇作为清除剂的 HO·清除实验进一步证实了这一点。g-CN 的 HNO 氧化导致催化失活,这表明催化活性源于 g-CN 的表面还原基团。通过 X 射线衍射、傅里叶变换红外光谱和 X 射线光电子能谱对合成前后 g-CN 的结构进行了表征,并提出了可能的催化机制。

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