Institute of Environmental Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China; School of Civil Engineering and Architecture, Ningbo Institute of Technology, Zhejiang University, Ningbo 315100, China.
Institute of Environmental Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China.
J Hazard Mater. 2019 Oct 15;378:120782. doi: 10.1016/j.jhazmat.2019.120782. Epub 2019 Jun 17.
Cu-based catalysts have great potential in Fenton reactions under neutral pH conditions. However, cuprous (Cu) materials are instable in the aqueous environment. Herein, using the cheap precursors, a Cu-graphitic carbon nitride complex with an efficient Fenton-like activity as well as relative stability was prepared. 99.2% removal of Rhodamine B with an initial concentration of 50 mg/L could be attained in 1 h. Several experimental techniques are employed to study the structure of this catalyst. Results show that after the addition of Cu, the graphitic carbon nitride (g-CN) network is partially destroyed and the reduced Cu is therefore firmly embedded in the fragmentary g-CN sheet. The X-ray adsorption fine spectra illustrates the chemical state and the local structure of the bonded Cu. Due to the strong orbital hybridization, Cu could be stabilized through the coordination with pyridinic N. A two-coordinate structure with a bond length of 1.90 Å is confirmed and this structure is not changed even after the Fenton-like reaction. Singlet oxygen (O) and hydroxyl radicals (HO•) are produced by the rapid interaction of bonded Cu with HO and the resulting Cu can be easily reduced to its cuprous state due to its structure stability, leading to its high activity in the Fenton-like reaction.
基于铜的催化剂在中性 pH 条件下的芬顿反应中具有很大的潜力。然而，亚铜（Cu）材料在水环境中不稳定。在此，使用廉价的前体，制备了一种具有高效类芬顿活性和相对稳定性的 Cu-石墨相氮化碳复合物。在 1 小时内，可以去除初始浓度为 50mg/L 的 Rhodamine B 的 99.2%。采用多种实验技术研究了该催化剂的结构。结果表明，加入 Cu 后，石墨相氮化碳（g-CN）网络被部分破坏，因此还原的 Cu 被牢固地嵌入到碎片状的 g-CN 片中。X 射线吸收精细光谱说明了键合 Cu 的化学状态和局部结构。由于强轨道杂化，Cu 可以通过与吡啶 N 的配位而稳定。通过与 HO 的快速相互作用，Cu 可以形成具有 1.90Å 键长的二配位结构，即使在类芬顿反应后，这种结构也不会改变。结合 Cu 与 HO 迅速产生单线态氧（O）和羟基自由基（HO•），而由于其结构稳定性，生成的 Cu 很容易被还原为亚铜状态，这导致其在类芬顿反应中具有很高的活性。
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