A Generalized Coordination Engineering Strategy for Single-Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis
文献类型：期刊论文
| 作者 | Liu, Wei1; Chen, Rui1; Sang, Zhiyuan1; Li, Zhenxin1; Nie, Jiahuan1; Yin, Lichang2; Hou, Feng1; Liang, Ji1 |
| 刊名 | ADVANCED MATERIALS
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| 出版日期 | 2024-07-22 |
| 页码 | 10 |
| 关键词 | 2e-ORR metal-organic frameworks single-atom catalysts |
| ISSN号 | 0935-9648 |
| DOI | 10.1002/adma.202406403 |
| 通讯作者 | Sang, Zhiyuan(sangzhiyuan@tju.edu.cn) ; Liang, Ji(liangji@tju.edu.cn) |
| 英文摘要 | Designing non-noble metal single-atom catalysts (M-SACs) for two-electron oxygen reduction reaction (2e-ORR) is attractive for the hydrogen peroxide (H2O2) electrosynthesis, in which the coordination configuration of the M-SACs essentially affects the reaction activity and product selectivity. Though extensively investigated, a generalized coordination engineering strategy has not yet been proposed, which fundamentally hinders the rational design of M-SACs with optimized catalytic capabilities. Herein, a generalized coordination engineering strategy is proposed for M-SACs toward H2O2 electrosynthesis via introducing heteroatoms (e.g., oxygen or sulfur atoms) with higher or lower electronegativity than nitrogen atoms into the first sphere of metal-N4 system to tailor their electronic structure and adjust the adsorption strength for *OOH intermediates, respectively, thus optimizing their electrocatalytic capability for 2e-ORR. Specifically, the (O, N)-coordinated Co SAC (Co-N3O) and (S, N)-coordinated Ni SAC (Ni-N3S) are precisely synthesized, and both present superior 2e-ORR activity (Eonset: approximate to 0.80 V versus RHE) and selectivity (approximate to 90%) in alkaline conditions compared with conventional Co-N4 and Ni-N4 sites. The high H2O2 yield rates of 14.2 and 17.5 moL g-1 h-1 and long-term stability over 12 h are respectively achieved for Co-N3O and Ni-N3S. Such favorable 2e-ORR pathway of the catalysts is also theoretically confirmed by the kinetics simulations. During the generalized coordination engineering strategy, the representative samples Co-N3O and Ni-N3S are precisely synthesized, and both of them present excellent activity and H2O2 selectivity (approximate to 90%) compared with conventional Metal-N4 configurations. Moreover, they enable a high H2O2 production of 14.2 and 17.5 moL g-1 h-1 in the three-phrase flow cell and maintain a satisfying stability over 12 h. image |
| 资助项目 | National Natural Science Foundation of China[22379111] ; National Natural Science Foundation of China[22179093] |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
| 语种 | 英语 |
| WOS记录号 | WOS:001273242900001 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| 资助机构 | National Natural Science Foundation of China |
| 源URL |  |
| 专题 | 金属研究所_中国科学院金属研究所 |
| 通讯作者 | Sang, Zhiyuan; Liang, Ji |
| 作者单位 | 1.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin 300072, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China |
| 推荐引用方式 GB/T 7714 | Liu, Wei,Chen, Rui,Sang, Zhiyuan,et al. A Generalized Coordination Engineering Strategy for Single-Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis[J]. ADVANCED MATERIALS,2024:10. |
| APA | Liu, Wei.,Chen, Rui.,Sang, Zhiyuan.,Li, Zhenxin.,Nie, Jiahuan.,...&Liang, Ji.(2024).A Generalized Coordination Engineering Strategy for Single-Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis.ADVANCED MATERIALS,10. |
| MLA | Liu, Wei,et al."A Generalized Coordination Engineering Strategy for Single-Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis".ADVANCED MATERIALS (2024):10. |
入库方式： OAI收割
来源：金属研究所
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