Photo-Excited High-Spin State Ni (III) Species in Mo-Doped Ni3S2 for Efficient Urea Oxidation Reaction
文献类型：期刊论文
| 作者 | Wang, Peichen1,2; Zheng, Wei1,2; Qu, Yafei1,2; Duan, Naiyuan1,2; Yang, Yang1,2; Wang, Dongdong1,2; Wang, Hui3; Chen, Qianwang1,2,3
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| 刊名 | SMALL
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| 出版日期 | 2024-07-19 |
| 关键词 | high spin state illumination assisted strategy urea electrolysis urea oxidation reaction |
| ISSN号 | 1613-6810 |
| DOI | 10.1002/smll.202403107 |
| 通讯作者 | Chen, Qianwang(cqw@ustc.edu.cn) |
| 英文摘要 | Designing robust catalysts for increasing the sluggish kinetics of the urea oxidation reaction (UOR) is challenging. Herein, the regulation of spin states for metal active sites by photoexcitation to facilitate the adsorption of urea and intermediates is demonstrated. Mo-doped nickel sulfide nanoribbon arrays (Mo-Ni3S2@NMF) with excellent light-trapping capacity are successfully prepared. Under AM 1.5G illumination, the activity of the Mo-Ni3S2@NMF exhibits a 50% improvement in the UOR current. Compared with those under dark conditions, Mo-Ni3S2@NMF achieve 10 mA cm(-2 )at 1.315 VRHE for UOR and 1.32 Vcell for urea electrolysis, which are decreases of 15 and 80 mV, respectively. The electron spin resonance, in situ Fourier transform infrared spectroscopy analysis and density functional theory calculations reveal that illumination led to the formation of Ni3+ active sites in a high-spin state, which strengthens the d-p orbital hybridization of Ni-N, hence facilitating the adsorption of urea. C & horbar;N cleavage of the *CONN intermediate is further inhibited, which promotes the oxidation of urea molecules via the active N2 pathway, thereby accelerating the UOR rate. |
| WOS关键词 | FE ; SPECTROSCOPY ; CO |
| 资助项目 | National Key R&D Program of China[22072140] ; National Key R&D Program of China[22272155] ; National Key R&D Program of China[22102169] ; National Natural Science Foundation of China[2021YFA1600202] |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
| 语种 | 英语 |
| WOS记录号 | WOS:001272677800001 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| 资助机构 | National Key R&D Program of China ; National Natural Science Foundation of China |
| 源URL | [http://ir.hfcas.ac.cn:8080/handle/334002/137317]  |
| 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 | Wang, Peichen,Zheng, Wei,Qu, Yafei,et al. Photo-Excited High-Spin State Ni (III) Species in Mo-Doped Ni3S2 for Efficient Urea Oxidation Reaction[J]. SMALL,2024. |
| APA | Wang, Peichen.,Zheng, Wei.,Qu, Yafei.,Duan, Naiyuan.,Yang, Yang.,...&Chen, Qianwang.(2024).Photo-Excited High-Spin State Ni (III) Species in Mo-Doped Ni3S2 for Efficient Urea Oxidation Reaction.SMALL. |
| MLA | Wang, Peichen,et al."Photo-Excited High-Spin State Ni (III) Species in Mo-Doped Ni3S2 for Efficient Urea Oxidation Reaction".SMALL (2024). |
入库方式： OAI收割
来源：合肥物质科学研究院
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