Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination
Wang, Yuxian1,2; Cao, Hongbin1; Chen, Lulu3; Chen, Chunmao2; Duan, Xiaoguang4; Xie, Yongbing1; Song, Weiyu3; Sun, Hongqi5; Wang, Shaobin4
2018-08-05
发表期刊APPLIED CATALYSIS B-ENVIRONMENTAL
ISSN0926-3373
卷号229页码:71-80
摘要Anode graphite was recovered from a spent lithium ion battery (LIB) and reutilized as a carbon precursor to obtain graphene-based materials. Characterization results revealed that impurities were removed from the obtained graphite powder by cleansing processes. The as-synthesized reduced graphene oxide (rGO) from the purified graphite (LIB-rGO) demonstrated excellent catalytic ozonation activity against organic pollutants removal. To probe potential catalytic active sites, LIB-rGOs with different defective levels but similar oxygen contents were synthesized. Catalytic ozonation tests revealed that a higher defective level resulted in a greater catalytic activity. Density functional theory (DFT) calculation further demonstrated that ozone molecules could spontaneously decompose into active oxygen species on graphene structural vacancies and edges, which consolidated the role of defective structure in catalytic ozonation activity. Meanwhile, we discovered the pollutant structure -dependent behavior of dominant reactive oxygen species (ROS) with the aid of radical scavenging tests and electron paramagnetic resonance (EPR) spectra. For phenolic pollutants vulnerable to direct ozone attacking, superoxide radicals (O-2 center dot(-)) and singlet oxygen (O-1(2)) were found to be responsible ROS, whereas hydroxyl radicals (center dot OH) were identified as the principle ROS for aliphatic organic pollutants destruction. This study not only put forward a possible way for reutilization of waste LIB anode, but also stepped further for investigating the catalytic ozonation mechanism towards the graphene-based materials including the active sites and the generation of ROS.
关键词Reduced Graphene Oxide Catalytic Ozonation Defects Density Functional Theory Reactive Oxygen Species
文章类型Article
WOS标题词Science & Technology ; Physical Sciences ; Technology
DOI10.1016/j.apcatb.2018.02.010
收录类别SCI
语种英语
关键词[WOS]EFFICIENT CATALYTIC OZONATION ; WALLED CARBON NANOTUBES ; HYDROGEN-PEROXIDE ; OXYGEN REDUCTION ; WATER-TREATMENT ; OXIDATION ; MECHANISM ; OZONE ; ACTIVATION ; PHENOL
WOS研究方向Chemistry ; Engineering
WOS类目Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical
项目资助者National Science Fund for Distinguished Young Scholars of China(51425405) ; National Natural Science Foundation of China(21606253) ; Science Foundation of China University of Petroleum, Beijing(2462016YJRC013) ; Beijing Natural Science Foundation(8172043)
WOS记录号WOS:000428488600009
引用统计
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/24139
专题湿法冶金清洁生产技术国家工程实验室
作者单位1.Chinese Acad Sci, Inst Proc Engn, Div Environm Technol & Engn, Beijing 100190, Peoples R China
2.China Univ Petr, Dept Chem Engn, State Key Lab Heavy Oil Proc, 18 Fuxue Rd, Beijing 102249, Peoples R China
3.China Univ Petr, Coll Sci, State Key Lab Heavy Oil Proc, 18 Fuxue Rd, Beijing 102249, Peoples R China
4.Curtin Univ, Dept Chem Engn, GPO Box U1987, Perth, WA 6845, Australia
5.Edith Cowan Univ, Sch Engn, 270 Joondalup Dr, Joondalup, WA 6027, Australia
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Wang, Yuxian,Cao, Hongbin,Chen, Lulu,et al. Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2018,229:71-80.
APA Wang, Yuxian.,Cao, Hongbin.,Chen, Lulu.,Chen, Chunmao.,Duan, Xiaoguang.,...&Wang, Shaobin.(2018).Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination.APPLIED CATALYSIS B-ENVIRONMENTAL,229,71-80.
MLA Wang, Yuxian,et al."Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination".APPLIED CATALYSIS B-ENVIRONMENTAL 229(2018):71-80.
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