Ce-induced NiS bifunctional catalyst transformation: enhancing urea oxidation coupled with hydrogen electrolysis
The treatment of urea-containing wastewater is crucial for sustainable environmental development, given its low theoretical thermodynamic barrier (0.37 V), which can effectively replace the OER process in water electrolysis and enhance hydrogen production efficiency. Nevertheless, designing dual-fun...
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sg-ntu-dr.10356-1817842024-12-20T15:32:15Z Ce-induced NiS bifunctional catalyst transformation: enhancing urea oxidation coupled with hydrogen electrolysis Zhang, Yingzhen Zhang, Wei Huang, Jianying Cai, Weilong Lai, Yuekun School of Chemistry, Chemical Engineering and Biotechnology Engineering Urea oxidation Hydrogen electrolysis The treatment of urea-containing wastewater is crucial for sustainable environmental development, given its low theoretical thermodynamic barrier (0.37 V), which can effectively replace the OER process in water electrolysis and enhance hydrogen production efficiency. Nevertheless, designing dual-functional catalysts capable of effectively performing catalytic tasks remains a challenge. Herein, in this work a cerium-doped nickel sulfide (Ce-NiS) catalyst is synthesized by an electrodeposition method, which is used as a bifunctional catalyst for electrolytic hydrogen production from urea-containing wastewater. Ce-NiS exhibits a higher Faradaic efficiency (FE, 91.39%) compared to NiS (67.52%) for hydrogen production from simulated urea-containing wastewater. In situ Raman spectroscopy reveals that Ce doping induces the reconstruction of NiS into high-valence nickel species (NiOOH), which is considered the actual active center for the electrochemical UOR process. Notably, the apparent electrochemical activation energy for the UOR decreased from 8.72 kJ mol−1 (NiS) to 5.68 kJ mol−1 (Ce-NiS), indicating that doping with Ce significantly reduces the energy barrier for the UOR and enhances the catalytic urea oxidation capability. This study employs a strategy of rare-earth metal (Ce) doping to enhance the efficiency of urea-coupled electrolytic hydrogen production, providing promising insights for energy recovery from urea-containing wastewater and the development of high-performance dual-functional catalysts. Published version The authors thank the financial support from the International Cooperation and Exchanges NSFC (22361162607), National Key Research and Development Program of China (No. 2022YFB 3804905), National Natural Science Foundation of China (22075046, 22378071, 22375047, 22378068), and Orientation Lab Project and Major Project of Qingyuan Innovation Laboratory (No. 00621005 and 00122006). 2024-12-17T07:45:37Z 2024-12-17T07:45:37Z 2024 Journal Article Zhang, Y., Zhang, W., Huang, J., Cai, W. & Lai, Y. (2024). Ce-induced NiS bifunctional catalyst transformation: enhancing urea oxidation coupled with hydrogen electrolysis. EES Catalysis, 2(6), 1306-1313. https://dx.doi.org/10.1039/d4ey00119b 2753-801X https://hdl.handle.net/10356/181784 10.1039/d4ey00119b 2-s2.0-85201920362 6 2 1306 1313 en EES Catalysis © 2024 The Author(s). Published by the Royal Society of Chemistry. This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. application/pdf |
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Engineering Urea oxidation Hydrogen electrolysis |
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Engineering Urea oxidation Hydrogen electrolysis Zhang, Yingzhen Zhang, Wei Huang, Jianying Cai, Weilong Lai, Yuekun Ce-induced NiS bifunctional catalyst transformation: enhancing urea oxidation coupled with hydrogen electrolysis |
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The treatment of urea-containing wastewater is crucial for sustainable environmental development, given its low theoretical thermodynamic barrier (0.37 V), which can effectively replace the OER process in water electrolysis and enhance hydrogen production efficiency. Nevertheless, designing dual-functional catalysts capable of effectively performing catalytic tasks remains a challenge. Herein, in this work a cerium-doped nickel sulfide (Ce-NiS) catalyst is synthesized by an electrodeposition method, which is used as a bifunctional catalyst for electrolytic hydrogen production from urea-containing wastewater. Ce-NiS exhibits a higher Faradaic efficiency (FE, 91.39%) compared to NiS (67.52%) for hydrogen production from simulated urea-containing wastewater. In situ Raman spectroscopy reveals that Ce doping induces the reconstruction of NiS into high-valence nickel species (NiOOH), which is considered the actual active center for the electrochemical UOR process. Notably, the apparent electrochemical activation energy for the UOR decreased from 8.72 kJ mol−1 (NiS) to 5.68 kJ mol−1 (Ce-NiS), indicating that doping with Ce significantly reduces the energy barrier for the UOR and enhances the catalytic urea oxidation capability. This study employs a strategy of rare-earth metal (Ce) doping to enhance the efficiency of urea-coupled electrolytic hydrogen production, providing promising insights for energy recovery from urea-containing wastewater and the development of high-performance dual-functional catalysts. |
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School of Chemistry, Chemical Engineering and Biotechnology |
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School of Chemistry, Chemical Engineering and Biotechnology Zhang, Yingzhen Zhang, Wei Huang, Jianying Cai, Weilong Lai, Yuekun |
format |
Article |
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Zhang, Yingzhen Zhang, Wei Huang, Jianying Cai, Weilong Lai, Yuekun |
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Zhang, Yingzhen |
title |
Ce-induced NiS bifunctional catalyst transformation: enhancing urea oxidation coupled with hydrogen electrolysis |
title_short |
Ce-induced NiS bifunctional catalyst transformation: enhancing urea oxidation coupled with hydrogen electrolysis |
title_full |
Ce-induced NiS bifunctional catalyst transformation: enhancing urea oxidation coupled with hydrogen electrolysis |
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Ce-induced NiS bifunctional catalyst transformation: enhancing urea oxidation coupled with hydrogen electrolysis |
title_full_unstemmed |
Ce-induced NiS bifunctional catalyst transformation: enhancing urea oxidation coupled with hydrogen electrolysis |
title_sort |
ce-induced nis bifunctional catalyst transformation: enhancing urea oxidation coupled with hydrogen electrolysis |
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2024 |
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https://hdl.handle.net/10356/181784 |
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1819113051451817984 |