Stable cuprous active sites in Cu+-graphitic carbon nitride: Structure analysis and performance in Fenton-like reactions
Stable cuprous active sites in Cu+-graphitic carbon nitride: Structure analysis and performance in Fenton-like reactions
复制标题
铜石墨氮化碳中稳定的亚铜活性位点：类芬顿反应中的结构分析和性能
DOI：
10.1016/j.jhazmat.2019.120782
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发表时间：
2019-10-15
影响因子：
13.6
通讯作者：
Wen, Yuezhong
中科院分区：
文献类型：
--
作者：
Ma, Jianqing;Jia, Nanzhengfang;Wen, Yuezhong
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-C3N4) network is partially destroyed and the reduced Cu is therefore firmly embedded in the fragmentary g-C3N4 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 angstrom is confirmed and this structure is not changed even after the Fenton-like reaction. Singlet oxygen (O-1(2)) and hydroxyl radicals (HO center dot) are produced by the rapid interaction of bonded Cu+ with H2O2 and the resulting Cu2+ can be easily reduced to its cuprous state due to its structure stability, leading to its high activity in the Fenton-like reaction.
