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氧在石墨相氮化碳上诱导的富电子铜活性位点的高效过硫酸盐非自由基活化

Efficient persulfate non-radical activation of electron-rich copper active sites induced by oxygen on graphitic carbon nitride.

作者信息

Song Hui, Liu Zhuang, Guan Zeyu, Yang Fan, Xia Dongsheng, Li Dongya

机构信息

School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, PR China.

School of Electronic and Electrical Engineering, Wuhan Textile University, Wuhan 430073, PR China.

出版信息

Sci Total Environ. 2021 Mar 25;762:143127. doi: 10.1016/j.scitotenv.2020.143127. Epub 2020 Oct 17.

DOI:10.1016/j.scitotenv.2020.143127
PMID:33162135
Abstract

Peroxymonosulfate (PMS) non-radical reactions possess high catalytic activity for specific pollutants under complex water environments. However, the synthesis of high-performance catalysts and the discussion of non-radical reaction mechanisms are still unsatisfactory. Here, a novel and efficient non-radical catalyst (O-CuCN) was successfully assembled using the scheme of Copper (Cu) and oxygen (O) co-doping. The O element with great electronegativity induces graphite carbon nitride (g-CN) to act as a medium to change the phase properties and electron density distribution of g-CN and provides a support for the targeting of Cu. Cu is introduced into g-CN as an active site in the phase structure, and an electron-rich center with the Cu site is formed, which forms a metastable intermediate after the adsorption of PMS by Cu as the active site. The new catalyst O-CuCN has outstanding activity in the PMS system, and its degradation rate for bisphenol A (BPA) is increased by more than 20 times compared to that of g-CN, and it has excellent environmental tolerance and stability. This work demonstrates that the formation of metastable intermediates and the initiation of effective non-radical reactions can be achieved by constructing differentiated electron density structures.

摘要

过一硫酸盐(PMS)非自由基反应在复杂水环境下对特定污染物具有高催化活性。然而,高性能催化剂的合成以及非自由基反应机理的探讨仍不尽人意。在此,通过铜(Cu)和氧(O)共掺杂的方案成功组装了一种新型高效非自由基催化剂(O-CuCN)。具有高电负性的O元素诱导石墨相氮化碳(g-CN)作为介质改变g-CN的相性质和电子密度分布,并为Cu的靶向提供支撑。Cu作为相结构中的活性位点引入到g-CN中,形成具有Cu位点的富电子中心,该富电子中心在作为活性位点的Cu吸附PMS后形成亚稳中间体。新型催化剂O-CuCN在PMS体系中具有出色的活性,其对双酚A(BPA)的降解速率比g-CN提高了20倍以上,并且具有优异的环境耐受性和稳定性。这项工作表明,通过构建差异化的电子密度结构可以实现亚稳中间体的形成和有效的非自由基反应的引发。

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