Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations
Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved a...
Ausführliche Beschreibung
Gespeichert in:
| Autor*in: |
Long, Yangke [verfasserIn] |
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| Format: |
E-Artikel |
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| Sprache: |
Englisch |
| Erschienen: |
2022transfer abstract |
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| Schlagwörter: |
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| Übergeordnetes Werk: |
Enthalten in: Summer bloom of - Moreira-González, Angel R. ELSEVIER, 2020, environmental control, risk assessment, impact and management, New York, NY [u.a.] |
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| Übergeordnetes Werk: |
volume:424 ; year:2022 ; day:15 ; month:02 ; pages:0 |
| Links: |
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| DOI / URN: |
10.1016/j.jhazmat.2021.126786 |
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ELV05606733X |
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| 245 | 1 | 0 | |a Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations |
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| 520 | |a Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. | ||
| 520 | |a Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. | ||
| 650 | 7 | |a Surface atomic engineering |2 Elsevier | |
| 650 | 7 | |a Water treatment |2 Elsevier | |
| 650 | 7 | |a MOF derivatives |2 Elsevier | |
| 650 | 7 | |a Nonradical mechanism |2 Elsevier | |
| 700 | 1 | |a Dai, Jian |4 oth | |
| 700 | 1 | |a Zhao, Shiyin |4 oth | |
| 700 | 1 | |a Huang, Shixin |4 oth | |
| 700 | 1 | |a Zhang, Zuotai |4 oth | |
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10.1016/j.jhazmat.2021.126786 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001719.pica (DE-627)ELV05606733X (ELSEVIER)S0304-3894(21)01753-2 DE-627 ger DE-627 rakwb eng 333.7 610 VZ 43.12 bkl 43.13 bkl 44.13 bkl Long, Yangke verfasserin aut Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations 2022transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. Surface atomic engineering Elsevier Water treatment Elsevier MOF derivatives Elsevier Nonradical mechanism Elsevier Dai, Jian oth Zhao, Shiyin oth Huang, Shixin oth Zhang, Zuotai oth Enthalten in Science Direct Moreira-González, Angel R. ELSEVIER Summer bloom of 2020 environmental control, risk assessment, impact and management New York, NY [u.a.] (DE-627)ELV005292484 volume:424 year:2022 day:15 month:02 pages:0 https://doi.org/10.1016/j.jhazmat.2021.126786 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA SSG-OPC-GGO 43.12 Umweltchemie VZ 43.13 Umwelttoxikologie VZ 44.13 Medizinische Ökologie VZ AR 424 2022 15 0215 0 |
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10.1016/j.jhazmat.2021.126786 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001719.pica (DE-627)ELV05606733X (ELSEVIER)S0304-3894(21)01753-2 DE-627 ger DE-627 rakwb eng 333.7 610 VZ 43.12 bkl 43.13 bkl 44.13 bkl Long, Yangke verfasserin aut Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations 2022transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. Surface atomic engineering Elsevier Water treatment Elsevier MOF derivatives Elsevier Nonradical mechanism Elsevier Dai, Jian oth Zhao, Shiyin oth Huang, Shixin oth Zhang, Zuotai oth Enthalten in Science Direct Moreira-González, Angel R. ELSEVIER Summer bloom of 2020 environmental control, risk assessment, impact and management New York, NY [u.a.] (DE-627)ELV005292484 volume:424 year:2022 day:15 month:02 pages:0 https://doi.org/10.1016/j.jhazmat.2021.126786 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA SSG-OPC-GGO 43.12 Umweltchemie VZ 43.13 Umwelttoxikologie VZ 44.13 Medizinische Ökologie VZ AR 424 2022 15 0215 0 |
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10.1016/j.jhazmat.2021.126786 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001719.pica (DE-627)ELV05606733X (ELSEVIER)S0304-3894(21)01753-2 DE-627 ger DE-627 rakwb eng 333.7 610 VZ 43.12 bkl 43.13 bkl 44.13 bkl Long, Yangke verfasserin aut Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations 2022transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. Surface atomic engineering Elsevier Water treatment Elsevier MOF derivatives Elsevier Nonradical mechanism Elsevier Dai, Jian oth Zhao, Shiyin oth Huang, Shixin oth Zhang, Zuotai oth Enthalten in Science Direct Moreira-González, Angel R. ELSEVIER Summer bloom of 2020 environmental control, risk assessment, impact and management New York, NY [u.a.] (DE-627)ELV005292484 volume:424 year:2022 day:15 month:02 pages:0 https://doi.org/10.1016/j.jhazmat.2021.126786 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA SSG-OPC-GGO 43.12 Umweltchemie VZ 43.13 Umwelttoxikologie VZ 44.13 Medizinische Ökologie VZ AR 424 2022 15 0215 0 |
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10.1016/j.jhazmat.2021.126786 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001719.pica (DE-627)ELV05606733X (ELSEVIER)S0304-3894(21)01753-2 DE-627 ger DE-627 rakwb eng 333.7 610 VZ 43.12 bkl 43.13 bkl 44.13 bkl Long, Yangke verfasserin aut Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations 2022transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. Surface atomic engineering Elsevier Water treatment Elsevier MOF derivatives Elsevier Nonradical mechanism Elsevier Dai, Jian oth Zhao, Shiyin oth Huang, Shixin oth Zhang, Zuotai oth Enthalten in Science Direct Moreira-González, Angel R. ELSEVIER Summer bloom of 2020 environmental control, risk assessment, impact and management New York, NY [u.a.] (DE-627)ELV005292484 volume:424 year:2022 day:15 month:02 pages:0 https://doi.org/10.1016/j.jhazmat.2021.126786 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA SSG-OPC-GGO 43.12 Umweltchemie VZ 43.13 Umwelttoxikologie VZ 44.13 Medizinische Ökologie VZ AR 424 2022 15 0215 0 |
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10.1016/j.jhazmat.2021.126786 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001719.pica (DE-627)ELV05606733X (ELSEVIER)S0304-3894(21)01753-2 DE-627 ger DE-627 rakwb eng 333.7 610 VZ 43.12 bkl 43.13 bkl 44.13 bkl Long, Yangke verfasserin aut Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations 2022transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. Surface atomic engineering Elsevier Water treatment Elsevier MOF derivatives Elsevier Nonradical mechanism Elsevier Dai, Jian oth Zhao, Shiyin oth Huang, Shixin oth Zhang, Zuotai oth Enthalten in Science Direct Moreira-González, Angel R. ELSEVIER Summer bloom of 2020 environmental control, risk assessment, impact and management New York, NY [u.a.] (DE-627)ELV005292484 volume:424 year:2022 day:15 month:02 pages:0 https://doi.org/10.1016/j.jhazmat.2021.126786 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA SSG-OPC-GGO 43.12 Umweltchemie VZ 43.13 Umwelttoxikologie VZ 44.13 Medizinische Ökologie VZ AR 424 2022 15 0215 0 |
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Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations |
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Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. |
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Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. |
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Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as CoNC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation. |
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