Cu-doped Ni-LDH with abundant oxygen vacancies for enhanced methyl 4-hydroxybenzoate degradation via peroxymonosulfate activation: key role of superoxide radicals
[Display omitted] •Cu doping facilitated the formation of oxygen vacancies (OVs) in NixCu-LDHs.•OVs introduction enhanced the catalytic activation of PMS by NixCu-LDHs.•O2•− and 1O2 worked as the main ROSs in Ni15Cu-LDHs/PMS system.•DO or adsorbed oxygen could acquire electron from OVs to generate O...
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| Published in | Journal of colloid and interface science Vol. 610; pp. 504 - 517 |
|---|---|
| Main Authors | , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
Elsevier Inc
15.03.2022
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| Subjects | |
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| Abstract | [Display omitted]
•Cu doping facilitated the formation of oxygen vacancies (OVs) in NixCu-LDHs.•OVs introduction enhanced the catalytic activation of PMS by NixCu-LDHs.•O2•− and 1O2 worked as the main ROSs in Ni15Cu-LDHs/PMS system.•DO or adsorbed oxygen could acquire electron from OVs to generate O2•−.•Synergy among Mn+/M(n+1)+ and active oxygen species ensured ROS generation.
Oxygen vacancies (OVs) were introduced into Ni-based layered double hydroxides (LDHs) through Cu doping, and the catalytic performance of the resulting NixCu-LDHs were investigated for peroxymonosulfate (PMS) activation and methyl 4-hydroxybenzoate (MeP) degradation. Compared with that of Ni-LDH, the catalytic performance of NixCu-LDHs were significantly enhanced and increased with increasing OV content in the catalysts, indicating that Cu doping introduced OVs into NixCu-LDHs and greatly improved their catalytic activity with PMS. Quenching experiments and EPR analyses confirmed that oxidation processes dominated by superoxide radicals (O2•−) and singlet oxygen (1O2), rather than sulfate radicals (SO4•−) or hydroxyl radicals (•OH) used by traditional LDH catalysts, were responsible for MeP degradation by Ni15Cu-LDHs. In addition, quenching experiments with different systems showed the fate of reduced SO4•−and •OH, and demonstrated that O2•− and 1O2 concentrations grew with increasing OV content, confirming that the presence of OVs affected the process of PMS activation. Notably, O2•− mainly originated from adsorbed oxygen or dissolved oxygen (DO) by acquiring electrons from OVs in Ni15Cu-LDHs, since OVs possess abundant localized electrons. Consequently, an OV-mediated oxidative mechanism was proposed for Ni15Cu-LDHs/PMS. This study provides new clues for enhancing the catalytic performance of LDH catalysts by introducing OVs via metal doping in PMS-based AOPs systems. |
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| AbstractList | Oxygen vacancies (OVs) were introduced into Ni-based layered double hydroxides (LDHs) through Cu doping, and the catalytic performance of the resulting Ni
Cu-LDHs were investigated for peroxymonosulfate (PMS) activation and methyl 4-hydroxybenzoate (MeP) degradation. Compared with that of Ni-LDH, the catalytic performance of Ni
Cu-LDHs were significantly enhanced and increased with increasing OV content in the catalysts, indicating that Cu doping introduced OVs into Ni
Cu-LDHs and greatly improved their catalytic activity with PMS. Quenching experiments and EPR analyses confirmed that oxidation processes dominated by superoxide radicals (O
) and singlet oxygen (
O
), rather than sulfate radicals (SO
) or hydroxyl radicals (•OH) used by traditional LDH catalysts, were responsible for MeP degradation by Ni
Cu-LDHs. In addition, quenching experiments with different systems showed the fate of reduced SO
and •OH, and demonstrated that O
and
O
concentrations grew with increasing OV content, confirming that the presence of OVs affected the process of PMS activation. Notably, O
mainly originated from adsorbed oxygen or dissolved oxygen (DO) by acquiring electrons from OVs in Ni
Cu-LDHs, since OVs possess abundant localized electrons. Consequently, an OV-mediated oxidative mechanism was proposed for Ni
Cu-LDHs/PMS. This study provides new clues for enhancing the catalytic performance of LDH catalysts by introducing OVs via metal doping in PMS-based AOPs systems. Oxygen vacancies (OVs) were introduced into Ni-based layered double hydroxides (LDHs) through Cu doping, and the catalytic performance of the resulting NiₓCu-LDHs were investigated for peroxymonosulfate (PMS) activation and methyl 4-hydroxybenzoate (MeP) degradation. Compared with that of Ni-LDH, the catalytic performance of NiₓCu-LDHs were significantly enhanced and increased with increasing OV content in the catalysts, indicating that Cu doping introduced OVs into NiₓCu-LDHs and greatly improved their catalytic activity with PMS. Quenching experiments and EPR analyses confirmed that oxidation processes dominated by superoxide radicals (O₂•⁻) and singlet oxygen (¹O₂), rather than sulfate radicals (SO₄•⁻) or hydroxyl radicals (•OH) used by traditional LDH catalysts, were responsible for MeP degradation by Ni₁₅Cu-LDHs. In addition, quenching experiments with different systems showed the fate of reduced SO₄•⁻and •OH, and demonstrated that O₂•⁻ and ¹O₂ concentrations grew with increasing OV content, confirming that the presence of OVs affected the process of PMS activation. Notably, O₂•⁻ mainly originated from adsorbed oxygen or dissolved oxygen (DO) by acquiring electrons from OVs in Ni₁₅Cu-LDHs, since OVs possess abundant localized electrons. Consequently, an OV-mediated oxidative mechanism was proposed for Ni₁₅Cu-LDHs/PMS. This study provides new clues for enhancing the catalytic performance of LDH catalysts by introducing OVs via metal doping in PMS-based AOPs systems. Oxygen vacancies (OVs) were introduced into Ni-based layered double hydroxides (LDHs) through Cu doping, and the catalytic performance of the resulting NixCu-LDHs were investigated for peroxymonosulfate (PMS) activation and methyl 4-hydroxybenzoate (MeP) degradation. Compared with that of Ni-LDH, the catalytic performance of NixCu-LDHs were significantly enhanced and increased with increasing OV content in the catalysts, indicating that Cu doping introduced OVs into NixCu-LDHs and greatly improved their catalytic activity with PMS. Quenching experiments and EPR analyses confirmed that oxidation processes dominated by superoxide radicals (O2•-) and singlet oxygen (1O2), rather than sulfate radicals (SO4•-) or hydroxyl radicals (•OH) used by traditional LDH catalysts, were responsible for MeP degradation by Ni15Cu-LDHs. In addition, quenching experiments with different systems showed the fate of reduced SO4•-and •OH, and demonstrated that O2•- and 1O2 concentrations grew with increasing OV content, confirming that the presence of OVs affected the process of PMS activation. Notably, O2•- mainly originated from adsorbed oxygen or dissolved oxygen (DO) by acquiring electrons from OVs in Ni15Cu-LDHs, since OVs possess abundant localized electrons. Consequently, an OV-mediated oxidative mechanism was proposed for Ni15Cu-LDHs/PMS. This study provides new clues for enhancing the catalytic performance of LDH catalysts by introducing OVs via metal doping in PMS-based AOPs systems.Oxygen vacancies (OVs) were introduced into Ni-based layered double hydroxides (LDHs) through Cu doping, and the catalytic performance of the resulting NixCu-LDHs were investigated for peroxymonosulfate (PMS) activation and methyl 4-hydroxybenzoate (MeP) degradation. Compared with that of Ni-LDH, the catalytic performance of NixCu-LDHs were significantly enhanced and increased with increasing OV content in the catalysts, indicating that Cu doping introduced OVs into NixCu-LDHs and greatly improved their catalytic activity with PMS. Quenching experiments and EPR analyses confirmed that oxidation processes dominated by superoxide radicals (O2•-) and singlet oxygen (1O2), rather than sulfate radicals (SO4•-) or hydroxyl radicals (•OH) used by traditional LDH catalysts, were responsible for MeP degradation by Ni15Cu-LDHs. In addition, quenching experiments with different systems showed the fate of reduced SO4•-and •OH, and demonstrated that O2•- and 1O2 concentrations grew with increasing OV content, confirming that the presence of OVs affected the process of PMS activation. Notably, O2•- mainly originated from adsorbed oxygen or dissolved oxygen (DO) by acquiring electrons from OVs in Ni15Cu-LDHs, since OVs possess abundant localized electrons. Consequently, an OV-mediated oxidative mechanism was proposed for Ni15Cu-LDHs/PMS. This study provides new clues for enhancing the catalytic performance of LDH catalysts by introducing OVs via metal doping in PMS-based AOPs systems. [Display omitted] •Cu doping facilitated the formation of oxygen vacancies (OVs) in NixCu-LDHs.•OVs introduction enhanced the catalytic activation of PMS by NixCu-LDHs.•O2•− and 1O2 worked as the main ROSs in Ni15Cu-LDHs/PMS system.•DO or adsorbed oxygen could acquire electron from OVs to generate O2•−.•Synergy among Mn+/M(n+1)+ and active oxygen species ensured ROS generation. Oxygen vacancies (OVs) were introduced into Ni-based layered double hydroxides (LDHs) through Cu doping, and the catalytic performance of the resulting NixCu-LDHs were investigated for peroxymonosulfate (PMS) activation and methyl 4-hydroxybenzoate (MeP) degradation. Compared with that of Ni-LDH, the catalytic performance of NixCu-LDHs were significantly enhanced and increased with increasing OV content in the catalysts, indicating that Cu doping introduced OVs into NixCu-LDHs and greatly improved their catalytic activity with PMS. Quenching experiments and EPR analyses confirmed that oxidation processes dominated by superoxide radicals (O2•−) and singlet oxygen (1O2), rather than sulfate radicals (SO4•−) or hydroxyl radicals (•OH) used by traditional LDH catalysts, were responsible for MeP degradation by Ni15Cu-LDHs. In addition, quenching experiments with different systems showed the fate of reduced SO4•−and •OH, and demonstrated that O2•− and 1O2 concentrations grew with increasing OV content, confirming that the presence of OVs affected the process of PMS activation. Notably, O2•− mainly originated from adsorbed oxygen or dissolved oxygen (DO) by acquiring electrons from OVs in Ni15Cu-LDHs, since OVs possess abundant localized electrons. Consequently, an OV-mediated oxidative mechanism was proposed for Ni15Cu-LDHs/PMS. This study provides new clues for enhancing the catalytic performance of LDH catalysts by introducing OVs via metal doping in PMS-based AOPs systems. |
| Author | Zhou, Wenjun Zhu, Jingyi Zhu, Yixin |
| Author_xml | – sequence: 1 givenname: Jingyi surname: Zhu fullname: Zhu, Jingyi organization: Department of Environmental Science, Zhejiang University, Hangzhou, Zhejiang 310058, China – sequence: 2 givenname: Yixin surname: Zhu fullname: Zhu, Yixin organization: Department of Environmental Science, Zhejiang University, Hangzhou, Zhejiang 310058, China – sequence: 3 givenname: Wenjun surname: Zhou fullname: Zhou, Wenjun email: wenjunzhou@zju.edu.cn organization: Department of Environmental Science, Zhejiang University, Hangzhou, Zhejiang 310058, China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/34838311$$D View this record in MEDLINE/PubMed |
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| Keywords | Cu-doped Ni-LDH Oxygen vacancies Superoxide radicals Peroxymonosulfate |
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•Cu doping facilitated the formation of oxygen vacancies (OVs) in NixCu-LDHs.•OVs introduction enhanced the catalytic activation of PMS by... Oxygen vacancies (OVs) were introduced into Ni-based layered double hydroxides (LDHs) through Cu doping, and the catalytic performance of the resulting Ni... Oxygen vacancies (OVs) were introduced into Ni-based layered double hydroxides (LDHs) through Cu doping, and the catalytic performance of the resulting... |
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| SubjectTerms | 4-hydroxybenzoic acid catalytic activity Cu-doped Ni-LDH dissolved oxygen oxidation Oxygen Oxygen vacancies Parabens Peroxides Peroxymonosulfate singlet oxygen sulfates Superoxide radicals Superoxides |
| Title | Cu-doped Ni-LDH with abundant oxygen vacancies for enhanced methyl 4-hydroxybenzoate degradation via peroxymonosulfate activation: key role of superoxide radicals |
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