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氮掺杂还原氧化石墨烯作为一种双功能材料去除双酚:吸附与催化协同作用。

Nitrogen-Doped Reduced Graphene Oxide as a Bifunctional Material for Removing Bisphenols: Synergistic Effect between Adsorption and Catalysis.

机构信息

†Key Laboratory of Catalysis and Materials Science of the State Ethnic Affairs Commission and Ministry of Education, College of Resources and Environmental Science, South-Central University for Nationalities, Wuhan 430074, P. R. China.

‡College of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China.

出版信息

Environ Sci Technol. 2015 Jun 2;49(11):6855-64. doi: 10.1021/acs.est.5b01059. Epub 2015 May 19.

DOI:10.1021/acs.est.5b01059
PMID:25943004
Abstract

Nitrogen modified reduced graphene oxide (N-RGO) was prepared by a hydrothermal method. The nitrogen modification enhanced its adsorption and catalysis ability. For an initial bisphenol concentration of 0.385 mmol L(-1), the adsorption capacity of N-RGO was evaluated as 1.56 and 1.43 mmol g(-1) for bisphenol A (BPA) and 1.43 mmol g(-1) for bisphenol F (BPF), respectively, both of which were about 1.75 times that (0.90 and 0.84 mmol g(-1)) on N-free RGO. N-RGO could activate persulfate, producing strong oxidizing sulfate radicals. The apparent degradation rate constant of BPA on N-RGO was 0.71 min(-1), being about 700 times that (0.001 min(-1)) on N-free RGO. In mixtures of various phenols, the degradation rate constant of each phenol was linearly increased with its adsorption capacity. A simultaneous use of N-RGO and persulfate yielded fast and efficient removal of bisphenols. The use of N-RGO (120 mg L(-1)) and persulfate (0.6 mmol L(-1)) almost completely removed the added bisphenols (0.385 mmol L(-1)) at pH 6.6 within 17 min. A mechanism study indicated that the adsorption enriched the pollutant, and the catalytically generated sulfate radicals rapidly degrade the adsorbed pollutant, accelerating in turn the adsorption of residual pollutant.

摘要

氮修饰还原氧化石墨烯(N-RGO)是通过水热法制备的。氮修饰增强了其吸附和催化能力。对于初始双酚浓度为 0.385mmol/L,N-RGO 的吸附容量分别为 1.56 和 1.43mmol/g 用于双酚 A(BPA)和 1.43mmol/g 用于双酚 F(BPF),分别约为 N-无 RGO 的 1.75 倍(0.90 和 0.84mmol/g)。N-RGO 可以激活过硫酸盐,产生强氧化硫酸根自由基。N-RGO 上 BPA 的表观降解速率常数为 0.71min-1,约为 N-无 RGO 的 700 倍(0.001min-1)。在各种酚类混合物中,每种酚类的降解速率常数与其吸附容量呈线性增加。同时使用 N-RGO 和过硫酸盐可以快速有效地去除双酚类物质。使用 N-RGO(120mg/L)和过硫酸盐(0.6mmol/L)在 pH6.6 下 17min 内几乎完全去除添加的双酚类物质(0.385mmol/L)。机理研究表明,吸附富集了污染物,催化生成的硫酸根自由基迅速降解吸附的污染物,从而加速了残留污染物的吸附。

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