Aminated N-doped graphene hydrogel for long-term catalytic oxidation in strong acidic environment
[Display omitted] •Aminated N-doped graphene hydrogel is synthesized with free-standing and porous structure.•The ANGH has high activity and long lifetime for PMS activation under strong-acidic condition.•The active sites of ANGH will transform from N containing groups into oxygenous groups.•ANGH ca...
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| Published in | Journal of hazardous materials Vol. 401; p. 123742 |
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| Main Authors | , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Elsevier B.V
05.01.2021
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| Subjects | |
| Online Access | Get full text |
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| Abstract | [Display omitted]
•Aminated N-doped graphene hydrogel is synthesized with free-standing and porous structure.•The ANGH has high activity and long lifetime for PMS activation under strong-acidic condition.•The active sites of ANGH will transform from N containing groups into oxygenous groups.•ANGH can be reused for rhodamine B degradation on a large scale after phenol degradation.
Metal-based catalysts in advanced oxidation processes (AOPs) are not stable under strong acidic condition due to the remarkable leaching, which will also lead to a secondary pollution. In this study, an aminated N-doped graphene hydrogel (ANGH) is synthesized from graphene oxide and ethylenediamine (EDA) via an in-situ hydrothermal process. The ANGH shows a free-standing structure and has high catalytic activity especially in phenol degradation under strong-acidic condition because of a non-radical dominated mechanism determined in this process. On the large scale, a longer lifetime of ∼1700 min for ANGH is obtained under strong-acidic condition on a dynamic amplifying device, 2.9 times longer than that at neutral condition. It is proposed that amine N can be protected by hydrogen ions from being oxidized, thus leading to the better stability. Meanwhile, the active sites of ANGH can transform from N containing groups into oxygenous groups, and the deactivated material can be reutilized 10 times for rhodamine B degradation on a large scale. The ANGH synthesized facilely and could be recycled repeatedly, which is also very stable in the strong acidic environment, thus should have great potential in wastewater remediation. |
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| AbstractList | Metal-based catalysts in advanced oxidation processes (AOPs) are not stable under strong acidic condition due to the remarkable leaching, which will also lead to a secondary pollution. In this study, an aminated N-doped graphene hydrogel (ANGH) is synthesized from graphene oxide and ethylenediamine (EDA) via an in-situ hydrothermal process. The ANGH shows a free-standing structure and has high catalytic activity especially in phenol degradation under strong-acidic condition because of a non-radical dominated mechanism determined in this process. On the large scale, a longer lifetime of ∼1700 min for ANGH is obtained under strong-acidic condition on a dynamic amplifying device, 2.9 times longer than that at neutral condition. It is proposed that amine N can be protected by hydrogen ions from being oxidized, thus leading to the better stability. Meanwhile, the active sites of ANGH can transform from N containing groups into oxygenous groups, and the deactivated material can be reutilized 10 times for rhodamine B degradation on a large scale. The ANGH synthesized facilely and could be recycled repeatedly, which is also very stable in the strong acidic environment, thus should have great potential in wastewater remediation. [Display omitted] •Aminated N-doped graphene hydrogel is synthesized with free-standing and porous structure.•The ANGH has high activity and long lifetime for PMS activation under strong-acidic condition.•The active sites of ANGH will transform from N containing groups into oxygenous groups.•ANGH can be reused for rhodamine B degradation on a large scale after phenol degradation. Metal-based catalysts in advanced oxidation processes (AOPs) are not stable under strong acidic condition due to the remarkable leaching, which will also lead to a secondary pollution. In this study, an aminated N-doped graphene hydrogel (ANGH) is synthesized from graphene oxide and ethylenediamine (EDA) via an in-situ hydrothermal process. The ANGH shows a free-standing structure and has high catalytic activity especially in phenol degradation under strong-acidic condition because of a non-radical dominated mechanism determined in this process. On the large scale, a longer lifetime of ∼1700 min for ANGH is obtained under strong-acidic condition on a dynamic amplifying device, 2.9 times longer than that at neutral condition. It is proposed that amine N can be protected by hydrogen ions from being oxidized, thus leading to the better stability. Meanwhile, the active sites of ANGH can transform from N containing groups into oxygenous groups, and the deactivated material can be reutilized 10 times for rhodamine B degradation on a large scale. The ANGH synthesized facilely and could be recycled repeatedly, which is also very stable in the strong acidic environment, thus should have great potential in wastewater remediation. Metal-based catalysts in advanced oxidation processes (AOPs) are not stable under strong acidic condition due to the remarkable leaching, which will also lead to a secondary pollution. In this study, an aminated N-doped graphene hydrogel (ANGH) is synthesized from graphene oxide and ethylenediamine (EDA) via an in-situ hydrothermal process. The ANGH shows a free-standing structure and has high catalytic activity especially in phenol degradation under strong-acidic condition because of a non-radical dominated mechanism determined in this process. On the large scale, a longer lifetime of ∼1700 min for ANGH is obtained under strong-acidic condition on a dynamic amplifying device, 2.9 times longer than that at neutral condition. It is proposed that amine N can be protected by hydrogen ions from being oxidized, thus leading to the better stability. Meanwhile, the active sites of ANGH can transform from N containing groups into oxygenous groups, and the deactivated material can be reutilized 10 times for rhodamine B degradation on a large scale. The ANGH synthesized facilely and could be recycled repeatedly, which is also very stable in the strong acidic environment, thus should have great potential in wastewater remediation.Metal-based catalysts in advanced oxidation processes (AOPs) are not stable under strong acidic condition due to the remarkable leaching, which will also lead to a secondary pollution. In this study, an aminated N-doped graphene hydrogel (ANGH) is synthesized from graphene oxide and ethylenediamine (EDA) via an in-situ hydrothermal process. The ANGH shows a free-standing structure and has high catalytic activity especially in phenol degradation under strong-acidic condition because of a non-radical dominated mechanism determined in this process. On the large scale, a longer lifetime of ∼1700 min for ANGH is obtained under strong-acidic condition on a dynamic amplifying device, 2.9 times longer than that at neutral condition. It is proposed that amine N can be protected by hydrogen ions from being oxidized, thus leading to the better stability. Meanwhile, the active sites of ANGH can transform from N containing groups into oxygenous groups, and the deactivated material can be reutilized 10 times for rhodamine B degradation on a large scale. The ANGH synthesized facilely and could be recycled repeatedly, which is also very stable in the strong acidic environment, thus should have great potential in wastewater remediation. |
| ArticleNumber | 123742 |
| Author | Hongwei, He Qing, Xia Yongsheng, Xu Wenchao, Peng Yuexiao, Song Xintong, Li |
| Author_xml | – sequence: 1 givenname: Xu surname: Yongsheng fullname: Yongsheng, Xu – sequence: 2 givenname: Li surname: Xintong fullname: Xintong, Li – sequence: 3 givenname: He surname: Hongwei fullname: Hongwei, He – sequence: 4 givenname: Song surname: Yuexiao fullname: Yuexiao, Song – sequence: 5 givenname: Xia surname: Qing fullname: Qing, Xia – sequence: 6 givenname: Peng surname: Wenchao fullname: Wenchao, Peng email: wenchao.peng@tju.edu.cn |
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| Keywords | Amination Active sites Regulation Hydrogel Large scale Strong Acidic condition N-doped graphene |
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•Aminated N-doped graphene hydrogel is synthesized with free-standing and porous structure.•The ANGH has high activity and long lifetime for... Metal-based catalysts in advanced oxidation processes (AOPs) are not stable under strong acidic condition due to the remarkable leaching, which will also lead... |
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| SubjectTerms | Acidic condition Active sites Amination catalytic activity ethylenediamines graphene graphene oxide Hydrogel hydrogels hydrogen Large scale N-doped graphene oxidation phenol pollution Regulation remediation rhodamines Strong wastewater |
| Title | Aminated N-doped graphene hydrogel for long-term catalytic oxidation in strong acidic environment |
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