Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination

© 2018 Elsevier B.V. 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-synthesize...

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Main Authors: Wang, Y., Cao, H., Chen, L., Chen, C., Duan, Xiaoguang, Xie, Y., Song, W., Sun, Hongqi, Wang, Shaobin
Format: Journal Article
Published: Elsevier BV 2018
Online Access:http://hdl.handle.net/20.500.11937/66459
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author Wang, Y.
Cao, H.
Chen, L.
Chen, C.
Duan, Xiaoguang
Xie, Y.
Song, W.
Sun, Hongqi
Wang, Shaobin
author_facet Wang, Y.
Cao, H.
Chen, L.
Chen, C.
Duan, Xiaoguang
Xie, Y.
Song, W.
Sun, Hongqi
Wang, Shaobin
author_sort Wang, Y.
building Curtin Institutional Repository
collection Online Access
description © 2018 Elsevier B.V. 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 [rad] - ) and singlet oxygen ( 1 O 2 ) were found to be responsible ROS, whereas hydroxyl radicals ([rad]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.
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spelling curtin-20.500.11937-664592020-02-24T07:33:11Z Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination Wang, Y. Cao, H. Chen, L. Chen, C. Duan, Xiaoguang Xie, Y. Song, W. Sun, Hongqi Wang, Shaobin © 2018 Elsevier B.V. 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 [rad] - ) and singlet oxygen ( 1 O 2 ) were found to be responsible ROS, whereas hydroxyl radicals ([rad]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. 2018 Journal Article http://hdl.handle.net/20.500.11937/66459 10.1016/j.apcatb.2018.02.010 Elsevier BV fulltext
spellingShingle Wang, Y.
Cao, H.
Chen, L.
Chen, C.
Duan, Xiaoguang
Xie, Y.
Song, W.
Sun, Hongqi
Wang, Shaobin
Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination
title Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination
title_full Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination
title_fullStr Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination
title_full_unstemmed Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination
title_short Tailored synthesis of active reduced graphene oxides from waste graphite: Structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination
title_sort tailored synthesis of active reduced graphene oxides from waste graphite: structural defects and pollutant-dependent reactive radicals in aqueous organics decontamination
url http://hdl.handle.net/20.500.11937/66459