A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal-Organic Framework for Efficient H2O2 Electrosynthesis
文献类型：期刊论文
| 作者 | Li, Zhenxin1; Jia, Jingjing1; Sang, Zhiyuan1; Liu, Wei1; Nie, Jiahuan1; Yin, Lichang2; Hou, Feng1; Liu, Jiachen1; Liang, Ji1 |
| 刊名 | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
 |
| 出版日期 | 2024-10-08 |
| 页码 | 10 |
| 关键词 | conductive metal-organic frameworks multi-site catalysts two-electron oxygen reduction reaction hydrogen peroxide |
| ISSN号 | 1433-7851 |
| DOI | 10.1002/anie.202408500 |
| 通讯作者 | Sang, Zhiyuan(sangzhiyuan@tju.edu.cn) ; Liang, Ji(liangji@tju.edu.cn) |
| 英文摘要 | Electrochemical synthesis of hydrogen peroxide (H2O2) via the two-electron oxygen reduction reaction (2e(-)-ORR) provides an alternative method to the energy-intensive anthraquinone method. Metal macrocycles with precise coordination are widely used for 2e(-)-ORR electrocatalysis, but they have to be commonly loaded on conductive substrates, thus exposing a large number of 2e(-)-ORR-inactive sites that result in poor H2O2 production rate and efficiency. Herein, guided by first-principle predictions, a substrate-free and two-dimensional conductive metal-organic framework (Ni-TCPP(Co)), composed of CoN4 sites in porphine(Co) centers and Ni2O8 nodes, is designed as a multi-site catalyst for H2O2 electrosynthesis. The approperiate distance between the CoN4 and Ni2O8 sites in Ni-TCPP(Co) weakens the electron transfer between them, thus ensuring their inherent activities and creating high-density active sites. Meanwhile, the intrinsic electronic conductivity and porosity of Ni-TCPP(Co) further facilitate rapid reaction kinetics. Therefore, outstanding 2e(-)-ORR electrocatalytic performance has been achieved in both alkaline and neutral electrolytes (>90 %/85 % H2O2 selectivity within 0-0.8 V vs. RHE and >18.2/18.0 mol g(-1) h(-1) H2O2 yield under alkaline/neutral conditions), with confirmed feasibility for water purification and disinfection applications. This strategy thus provides a new avenue for designing catalysts with precise coordination and high-density active sites, promoting high-efficiency electrosynthesis of H2O2 and beyond. |
| 资助项目 | National Natural Science Foundation of China ; [22379111] ; [22179093] |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:001331233400001 |
| 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 | Li, Zhenxin,Jia, Jingjing,Sang, Zhiyuan,et al. A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal-Organic Framework for Efficient H2O2 Electrosynthesis[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2024:10. |
| APA | Li, Zhenxin.,Jia, Jingjing.,Sang, Zhiyuan.,Liu, Wei.,Nie, Jiahuan.,...&Liang, Ji.(2024).A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal-Organic Framework for Efficient H2O2 Electrosynthesis.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,10. |
| MLA | Li, Zhenxin,et al."A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal-Organic Framework for Efficient H2O2 Electrosynthesis".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2024):10. |
入库方式： OAI收割
来源：金属研究所
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