4f-2p-3d Orbital Coupling in Ce-Ni3S2 Enhancing the Urea Oxidation Reaction
文献类型：期刊论文
| 作者 | Zheng, Wei1; Duan, Naiyuan1; Yang, Yang1; Wang, Peichen2; Qu, Yafei2; Zong, Cichang3; Chen, Qianwang1,2,3
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| 刊名 | INORGANIC CHEMISTRY
 |
| 出版日期 | 2024-07-22 |
| 卷号 | 63 |
| ISSN号 | 0020-1669 |
| DOI | 10.1021/acs.inorgchem.4c02111 |
| 通讯作者 | Chen, Qianwang(cqw@ustc.edu.cn) |
| 英文摘要 | The electrocatalytic urea oxidation reaction (UOR) provides a promising alternative to the oxygen evolution reaction (OER) for various renewable energy-related systems owing to its lower thermodynamic barriers. However, its optimization and commercial utilization were hampered due to a lack of mechanistic understanding. Here, we demonstrate a Ce-doped Ni3S2 catalyst supported on Ni foam (Ce-Ni3S2/NF) with superior activity toward UOR. The resultant Ce-Ni3S2/NF catalyst exhibits a lower Tafel slope of 20.3 mV dec(-1), a higher current density of 100 mA cm(-2) at 1.39 V versus RHE, and better durability than those for Ni3S2/NF. Based on in situ synchrotron radiation X-ray absorption spectroscopy, in situ Fourier transform infrared (FTIR), and in situ Raman spectroscopy, we observe the structural reconstruction of sulfide and identify the adsorbed intermediates during UOR. Density functional theory (DFT) calculations reveal that Ce can regulate the electronic structure of Ni through Ce(4f)-O(2p)-Ni(3d) orbital electronic coupling. The modulated Ni sites have weaker adsorption of carbonaceous intermediates, thus accelerating the UOR. This work provides a promising route for the design of high-activity UOR catalysts. |
| WOS关键词 | CATALYST ; OXIDES |
| 资助项目 | National Key R&D Program of China[2021YFA1600202] ; National Natural Science Foundation[22102155] ; National Natural Science Foundation[22072140] |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:001274503100001 |
| 出版者 | AMER CHEMICAL SOC |
| 资助机构 | National Key R&D Program of China ; National Natural Science Foundation |
| 源URL | [http://ir.hfcas.ac.cn:8080/handle/334002/137244]  |
| 专题 | 中国科学院合肥物质科学研究院 |
| 通讯作者 | Chen, Qianwang |
| 作者单位 | 1.Univ Sci & Technol China, Dept Mat Sci & Engn, Hefei 230026, Peoples R China 2.Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Hefei 230026, Peoples R China 3.Chinese Acad Sci, Hefei Inst Phys Sci, High Magnet Field Lab, Hefei 230031, Peoples R China |
| 推荐引用方式 GB/T 7714 | Zheng, Wei,Duan, Naiyuan,Yang, Yang,et al. 4f-2p-3d Orbital Coupling in Ce-Ni3S2 Enhancing the Urea Oxidation Reaction[J]. INORGANIC CHEMISTRY,2024,63. |
| APA | Zheng, Wei.,Duan, Naiyuan.,Yang, Yang.,Wang, Peichen.,Qu, Yafei.,...&Chen, Qianwang.(2024).4f-2p-3d Orbital Coupling in Ce-Ni3S2 Enhancing the Urea Oxidation Reaction.INORGANIC CHEMISTRY,63. |
| MLA | Zheng, Wei,et al."4f-2p-3d Orbital Coupling in Ce-Ni3S2 Enhancing the Urea Oxidation Reaction".INORGANIC CHEMISTRY 63(2024). |
入库方式： OAI收割
来源：合肥物质科学研究院
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