标题: Biphase Co@C core-shell catalysts for efficient Fenton-like catalysis

作者: Ma, YS (Ma, Yongsong); Du, KF (Du, Kaifa); Guo, YF (Guo, Yifan); Tang, MY (Tang, Mengyi); Yin, HY (Yin, Huayi); Mao, XH (Mao, Xuhui); Wang, DH (Wang, Dihua)

来源出版物: JOURNAL OF HAZARDOUS MATERIALS 卷: 429 文献号: 128287 DOI: 10.1016/j.jhazmat.2022.128287 出版年: MAY 5 2022

摘要: Despite the vital roles of Co nanoparticles catalytic oxidation in the Fenton-like system for eliminating pollutants, contributions of Co phases are typically overlooked. Herein, a biphase Co@C core-shell catalyst was synthesized by the electrochemical co-reduction of CaCO3 and Co3O4 in molten carbonate. Unlike the traditional pyrolysis method that is performed over 700 degrees C, the electrolysis was deployed at 450 degrees C, at which biphase structures, i.e., face-centered cubic (FCC) and hexagonal close-packed (HCP) structures, can be obtained. The biphase Co@C shows excellent catalytic oxidation performance of diethyl phthalate (DEP) with a high turnover frequency value (TOF, 28.14 min(-1)) and low catalyst dosage (4 mg L--(1)). Furthermore, density functional theory (DFT) calculations confirm that the synergistic catalytic effect of biphase Co@C is the enhancement for the breaking of the peroxide O-O bond and the charge transfer from catalysts to PMS molecule for the activation. Moreover, the results of radicals quenching experiments and electron paramagnetic resonance (EPR) tests confirm that SO4 center dot-, center dot OH, O-2(center dot-), and O-1(2) co-degrade DEP. Remarkably, 100% removals of three model contaminants, including DEP, sulfamethoxazole (SMX) and 2,4-dichlorophen (2,4-DCP), were achieved, either in pure water or actual river water. This paper provides an electrochemical pathway to leverage the phase of catalysts and thereby mediate their catalytic capability for remediating refractory organic contaminants.

作者关键词: Refractory organic contaminants; Peroxymonosulfate; Biphase Co@C core-shell catalyst; CaCO3 reduction; Catalytic oxidation

地址: [Ma, Yongsong; Du, Kaifa; Guo, Yifan; Tang, Mengyi; Yin, Huayi; Mao, Xuhui; Wang, Dihua] Wuhan Univ, Hubei Int Sci & Technol Cooperat Base Sustainable, Sch Resource & Environm Sci, Wuhan 430072, Peoples R China.

[Ma, Yongsong; Wang, Dihua] Wuhan Univ, State Key Lab Water Resources & Hydropower Engn S, Wuhan 430072, Peoples R China.

[Yin, Huayi] Northeastern Univ, Sch Met, Minist Educ, Key Lab Ecol Met Multimet Mineral, Shenyang 110819, Peoples R China.

通讯作者地址: Wang, DH (通讯作者)，Wuhan Univ, Hubei Int Sci & Technol Cooperat Base Sustainable, Sch Resource & Environm Sci, Wuhan 430072, Peoples R China.

Wang, DH (通讯作者)，Wuhan Univ, State Key Lab Water Resources & Hydropower Engn S, Wuhan 430072, Peoples R China.

电子邮件地址: wangdh@whu.edu.cn

影响因子：10.588