Reaction selectivity-regulation via interfacial reconstruction for preventing hazardous slime generation: driving mechanism of Pb-based anode with oxygen vacancy-rich MnO2
Limited selectivity in coexisted anodic reactions on lead-based anodes leads to severe lead-dissolution, anodic slime-generation and high energy-consumption. Herein, anodic reaction selectivity was regulated by phase-controlled MnO2 (MnO2-PC) on lead-based anodes which was prepared under a lower vol...
| Main Authors: | , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
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2024
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| Online Access: | https://hdl.handle.net/10356/174071 |
| _version_ | 1826121666093121536 |
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| author | Zhuang, Siwei Duan, Ning Jiang, Linhua Zhang, Feilong Hu, Jun Chen, Zhong Xu, Fuyuan |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Zhuang, Siwei Duan, Ning Jiang, Linhua Zhang, Feilong Hu, Jun Chen, Zhong Xu, Fuyuan |
| author_sort | Zhuang, Siwei |
| collection | NTU |
| description | Limited selectivity in coexisted anodic reactions on lead-based anodes leads to severe lead-dissolution, anodic slime-generation and high energy-consumption. Herein, anodic reaction selectivity was regulated by phase-controlled MnO2 (MnO2-PC) on lead-based anodes which was prepared under a lower voltage and a higher Mn2+ concentration. Compared with α-MnO2 formed under normal conditions, composite phase of γ-MnO2 and ε-MnO2 was obtained from MnO2-PC with specific crystal planes exposure and rich oxygen vacancy defects enabling higher oxygen evolution reaction selectivity (OER, overpotential reduced by ∼99 mV). Meanwhile, reaction of lead corrosion and manganese oxidation, as the main reasons for generation of hazardous lead-containing slime, were synergistically suppressed by 86.8% and 91.7%, respectively. Density functional theory (DFT) calculations further clarified that the change in coordinative environment of Mn and O brought lower energy barrier of rate-determining step of OER and stronger electron delocalization ability of MnO2, beneficial for promoting the catalysis of OER. MnO2-PC also displayed excellent inhibition effects on the generation and accumulation of Mn3+, an important precursor of MnO2 slime, and changed the selectivity in the oxidative path of Mn2+. The long-term electrolysis tests proved the stable performance of Pb–Ag/MnO2-PC. This study provides an efficient, low-cost, high economic benefits and environmental-friendly strategy for designing target functional materials towards reaction selectivity regulation via phase-control and microstructure reconstruction. |
| first_indexed | 2024-10-01T05:36:15Z |
| format | Journal Article |
| id | ntu-10356/174071 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T05:36:15Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1740712024-03-13T08:46:03Z Reaction selectivity-regulation via interfacial reconstruction for preventing hazardous slime generation: driving mechanism of Pb-based anode with oxygen vacancy-rich MnO2 Zhuang, Siwei Duan, Ning Jiang, Linhua Zhang, Feilong Hu, Jun Chen, Zhong Xu, Fuyuan School of Materials Science and Engineering Engineering Lead-based anode Hazardous lead-containing slime Limited selectivity in coexisted anodic reactions on lead-based anodes leads to severe lead-dissolution, anodic slime-generation and high energy-consumption. Herein, anodic reaction selectivity was regulated by phase-controlled MnO2 (MnO2-PC) on lead-based anodes which was prepared under a lower voltage and a higher Mn2+ concentration. Compared with α-MnO2 formed under normal conditions, composite phase of γ-MnO2 and ε-MnO2 was obtained from MnO2-PC with specific crystal planes exposure and rich oxygen vacancy defects enabling higher oxygen evolution reaction selectivity (OER, overpotential reduced by ∼99 mV). Meanwhile, reaction of lead corrosion and manganese oxidation, as the main reasons for generation of hazardous lead-containing slime, were synergistically suppressed by 86.8% and 91.7%, respectively. Density functional theory (DFT) calculations further clarified that the change in coordinative environment of Mn and O brought lower energy barrier of rate-determining step of OER and stronger electron delocalization ability of MnO2, beneficial for promoting the catalysis of OER. MnO2-PC also displayed excellent inhibition effects on the generation and accumulation of Mn3+, an important precursor of MnO2 slime, and changed the selectivity in the oxidative path of Mn2+. The long-term electrolysis tests proved the stable performance of Pb–Ag/MnO2-PC. This study provides an efficient, low-cost, high economic benefits and environmental-friendly strategy for designing target functional materials towards reaction selectivity regulation via phase-control and microstructure reconstruction. This research was supported by the National Natural Science Foundation of China (52174385; 41877392), and Fundamental Research Funds for the Central Universities, Tongji University (22120220166). 2024-03-13T08:45:17Z 2024-03-13T08:45:17Z 2023 Journal Article Zhuang, S., Duan, N., Jiang, L., Zhang, F., Hu, J., Chen, Z. & Xu, F. (2023). Reaction selectivity-regulation via interfacial reconstruction for preventing hazardous slime generation: driving mechanism of Pb-based anode with oxygen vacancy-rich MnO2. Journal of Cleaner Production, 404, 136961-. https://dx.doi.org/10.1016/j.jclepro.2023.136961 0959-6526 https://hdl.handle.net/10356/174071 10.1016/j.jclepro.2023.136961 2-s2.0-85151005953 404 136961 en Journal of Cleaner Production © 2023 Elsevier Ltd. All rights reserved. |
| spellingShingle | Engineering Lead-based anode Hazardous lead-containing slime Zhuang, Siwei Duan, Ning Jiang, Linhua Zhang, Feilong Hu, Jun Chen, Zhong Xu, Fuyuan Reaction selectivity-regulation via interfacial reconstruction for preventing hazardous slime generation: driving mechanism of Pb-based anode with oxygen vacancy-rich MnO2 |
| title | Reaction selectivity-regulation via interfacial reconstruction for preventing hazardous slime generation: driving mechanism of Pb-based anode with oxygen vacancy-rich MnO2 |
| title_full | Reaction selectivity-regulation via interfacial reconstruction for preventing hazardous slime generation: driving mechanism of Pb-based anode with oxygen vacancy-rich MnO2 |
| title_fullStr | Reaction selectivity-regulation via interfacial reconstruction for preventing hazardous slime generation: driving mechanism of Pb-based anode with oxygen vacancy-rich MnO2 |
| title_full_unstemmed | Reaction selectivity-regulation via interfacial reconstruction for preventing hazardous slime generation: driving mechanism of Pb-based anode with oxygen vacancy-rich MnO2 |
| title_short | Reaction selectivity-regulation via interfacial reconstruction for preventing hazardous slime generation: driving mechanism of Pb-based anode with oxygen vacancy-rich MnO2 |
| title_sort | reaction selectivity regulation via interfacial reconstruction for preventing hazardous slime generation driving mechanism of pb based anode with oxygen vacancy rich mno2 |
| topic | Engineering Lead-based anode Hazardous lead-containing slime |
| url | https://hdl.handle.net/10356/174071 |
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