Enhanced degradation of sulfamethoxazole by non-radical-dominated peroxymonosulfate activation with Co/Zn co-doped carbonaceous catalyst: Synergy between Co and Zn
Bimetallic catalysts are often used for peroxymonosulfate (PMS) activation in recent years due to the synergistic effects between two different metal species. However, the synergy between Zn and other transition metal in PMS activation are rarely studied because of the ease of evaporation of Zn spec...
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| Published in | The Science of the total environment Vol. 850; p. 158055 |
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| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Elsevier B.V
01.12.2022
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| Online Access | Get full text |
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| Abstract | Bimetallic catalysts are often used for peroxymonosulfate (PMS) activation in recent years due to the synergistic effects between two different metal species. However, the synergy between Zn and other transition metal in PMS activation are rarely studied because of the ease of evaporation of Zn species at high temperature. In this work, a Co/Zn co-doped carbonaceous catalyst derived from ZIF-67@ZIF-8 (Z67@8D) was prepared successfully by the core-shell replacement strategy, and used to activate PMS for sulfamethoxazole (SMX) degradation. Due to the co-existence of Co/Zn species (e.g., Co/Zn-N site), Z67@8D showed a much higher catalytic activity than that of Z8D, Z67D, and several commercial oxides. Importantly, the CoZn synergy was deeply revealed by combining experiments and density functional theory (DFT) calculations, in which Zn could adjust the electron distribution of Co, reducing the PMS adsorption energy and thus enhancing PMS decomposition and singlet oxygen (1O2) formation. Moreover, formed ZnO and graphitic structure of Z67@8D could also promote the catalytic activity. In addition, the good stability and reusability, universal applicability, and high environmental robustness of Z67@8D were demonstrated. Our findings may provide a new insight into the Zn-based bimetallic catalysts for PMS activation and pollutant degradation.
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•Co/Zn co-doped carbonaceous catalyst was prepared successfully by the core-shell replacement strategy.•Co/Zn-N synergistic sites could accelerate PMS decomposition to form 1O2 by adjusting Zn on the electron distribution of Co.•Formed ZnO and graphitic structure of Z67@8D could also promote catalytic activity.•The good stability and reusability, universal applicability, and high environmental robustness of Z67@8D were demonstrated. |
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| AbstractList | Bimetallic catalysts are often used for peroxymonosulfate (PMS) activation in recent years due to the synergistic effects between two different metal species. However, the synergy between Zn and other transition metal in PMS activation are rarely studied because of the ease of evaporation of Zn species at high temperature. In this work, a Co/Zn co-doped carbonaceous catalyst derived from ZIF-67@ZIF-8 (Z67@8D) was prepared successfully by the core-shell replacement strategy, and used to activate PMS for sulfamethoxazole (SMX) degradation. Due to the co-existence of Co/Zn species (e.g., Co/Zn-N site), Z67@8D showed a much higher catalytic activity than that of Z8D, Z67D, and several commercial oxides. Importantly, the CoZn synergy was deeply revealed by combining experiments and density functional theory (DFT) calculations, in which Zn could adjust the electron distribution of Co, reducing the PMS adsorption energy and thus enhancing PMS decomposition and singlet oxygen (1O2) formation. Moreover, formed ZnO and graphitic structure of Z67@8D could also promote the catalytic activity. In addition, the good stability and reusability, universal applicability, and high environmental robustness of Z67@8D were demonstrated. Our findings may provide a new insight into the Zn-based bimetallic catalysts for PMS activation and pollutant degradation.
[Display omitted]
•Co/Zn co-doped carbonaceous catalyst was prepared successfully by the core-shell replacement strategy.•Co/Zn-N synergistic sites could accelerate PMS decomposition to form 1O2 by adjusting Zn on the electron distribution of Co.•Formed ZnO and graphitic structure of Z67@8D could also promote catalytic activity.•The good stability and reusability, universal applicability, and high environmental robustness of Z67@8D were demonstrated. Bimetallic catalysts are often used for peroxymonosulfate (PMS) activation in recent years due to the synergistic effects between two different metal species. However, the synergy between Zn and other transition metal in PMS activation are rarely studied because of the ease of evaporation of Zn species at high temperature. In this work, a Co/Zn co-doped carbonaceous catalyst derived from ZIF-67@ZIF-8 (Z67@8D) was prepared successfully by the core-shell replacement strategy, and used to activate PMS for sulfamethoxazole (SMX) degradation. Due to the co-existence of Co/Zn species (e.g., Co/Zn-N site), Z67@8D showed a much higher catalytic activity than that of Z8D, Z67D, and several commercial oxides. Importantly, the CoZn synergy was deeply revealed by combining experiments and density functional theory (DFT) calculations, in which Zn could adjust the electron distribution of Co, reducing the PMS adsorption energy and thus enhancing PMS decomposition and singlet oxygen (1O2) formation. Moreover, formed ZnO and graphitic structure of Z67@8D could also promote the catalytic activity. In addition, the good stability and reusability, universal applicability, and high environmental robustness of Z67@8D were demonstrated. Our findings may provide a new insight into the Zn-based bimetallic catalysts for PMS activation and pollutant degradation.Bimetallic catalysts are often used for peroxymonosulfate (PMS) activation in recent years due to the synergistic effects between two different metal species. However, the synergy between Zn and other transition metal in PMS activation are rarely studied because of the ease of evaporation of Zn species at high temperature. In this work, a Co/Zn co-doped carbonaceous catalyst derived from ZIF-67@ZIF-8 (Z67@8D) was prepared successfully by the core-shell replacement strategy, and used to activate PMS for sulfamethoxazole (SMX) degradation. Due to the co-existence of Co/Zn species (e.g., Co/Zn-N site), Z67@8D showed a much higher catalytic activity than that of Z8D, Z67D, and several commercial oxides. Importantly, the CoZn synergy was deeply revealed by combining experiments and density functional theory (DFT) calculations, in which Zn could adjust the electron distribution of Co, reducing the PMS adsorption energy and thus enhancing PMS decomposition and singlet oxygen (1O2) formation. Moreover, formed ZnO and graphitic structure of Z67@8D could also promote the catalytic activity. In addition, the good stability and reusability, universal applicability, and high environmental robustness of Z67@8D were demonstrated. Our findings may provide a new insight into the Zn-based bimetallic catalysts for PMS activation and pollutant degradation. Bimetallic catalysts are often used for peroxymonosulfate (PMS) activation in recent years due to the synergistic effects between two different metal species. However, the synergy between Zn and other transition metal in PMS activation are rarely studied because of the ease of evaporation of Zn species at high temperature. In this work, a Co/Zn co-doped carbonaceous catalyst derived from ZIF-67@ZIF-8 (Z67@8D) was prepared successfully by the core-shell replacement strategy, and used to activate PMS for sulfamethoxazole (SMX) degradation. Due to the co-existence of Co/Zn species (e.g., Co/Zn-N site), Z67@8D showed a much higher catalytic activity than that of Z8D, Z67D, and several commercial oxides. Importantly, the CoZn synergy was deeply revealed by combining experiments and density functional theory (DFT) calculations, in which Zn could adjust the electron distribution of Co, reducing the PMS adsorption energy and thus enhancing PMS decomposition and singlet oxygen (¹O₂) formation. Moreover, formed ZnO and graphitic structure of Z67@8D could also promote the catalytic activity. In addition, the good stability and reusability, universal applicability, and high environmental robustness of Z67@8D were demonstrated. Our findings may provide a new insight into the Zn-based bimetallic catalysts for PMS activation and pollutant degradation. |
| ArticleNumber | 158055 |
| Author | Cui, Minshu Ding, Yan Cui, Kangping Chen, Yawen Liu, Tong Chen, Yihan Li, Wen-Wei Chen, Xing Li, Chen-Xuan |
| Author_xml | – sequence: 1 givenname: Yawen surname: Chen fullname: Chen, Yawen organization: School of Resources and Environmental Engineering, Hefei University of Technology, Hefei 230009, People's Republic of China – sequence: 2 givenname: Kangping surname: Cui fullname: Cui, Kangping organization: School of Resources and Environmental Engineering, Hefei University of Technology, Hefei 230009, People's Republic of China – sequence: 3 givenname: Tong surname: Liu fullname: Liu, Tong organization: School of Resources and Environmental Engineering, Hefei University of Technology, Hefei 230009, People's Republic of China – sequence: 4 givenname: Minshu surname: Cui fullname: Cui, Minshu organization: School of Resources and Environmental Engineering, Hefei University of Technology, Hefei 230009, People's Republic of China – sequence: 5 givenname: Yan surname: Ding fullname: Ding, Yan organization: School of Resources and Environmental Engineering, Hefei University of Technology, Hefei 230009, People's Republic of China – sequence: 6 givenname: Yihan surname: Chen fullname: Chen, Yihan organization: School of Resources and Environmental Engineering, Hefei University of Technology, Hefei 230009, People's Republic of China – sequence: 7 givenname: Xing surname: Chen fullname: Chen, Xing organization: School of Resources and Environmental Engineering, Hefei University of Technology, Hefei 230009, People's Republic of China – sequence: 8 givenname: Wen-Wei surname: Li fullname: Li, Wen-Wei organization: CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science & Technology of China, Hefei 230026, People's Republic of China – sequence: 9 givenname: Chen-Xuan surname: Li fullname: Li, Chen-Xuan email: cxli@hfut.edu.cn organization: School of Resources and Environmental Engineering, Hefei University of Technology, Hefei 230009, People's Republic of China |
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| Keywords | Singlet oxygen Peroxymonosulfate Synergistic effect of Co-Zn DFT calculations Co/Zn co-doped carbonaceous catalyst |
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| SubjectTerms | adsorption catalysts catalytic activity Co/Zn co-doped carbonaceous catalyst density functional theory DFT calculations energy environment evaporation Peroxymonosulfate pollutants Singlet oxygen species sulfamethoxazole Synergistic effect of Co-Zn temperature |
| Title | Enhanced degradation of sulfamethoxazole by non-radical-dominated peroxymonosulfate activation with Co/Zn co-doped carbonaceous catalyst: Synergy between Co and Zn |
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