Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering
文献类型：期刊论文
| 作者 | Xiao, ML; Chen, YT; Zhu, JB; Zhang, H; Zhao, X; Gao, LQ; Wang, X; Zhao, J; Ge, JJ; Jiang, Z |
| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
 |
| 出版日期 | 2019 |
| 卷号 | 141期号:44页码:17763-17770 |
| 关键词 | OXYGEN REDUCTION REACTION DOPED CARBON NANOTUBES IRON-BASED CATALYSTS ELECTROCATALYTIC ACTIVITY ACTIVE-SITES EFFICIENT ELECTROCATALYST TRANSITION-METALS FE-N/C IDENTIFICATION COORDINATION |
| ISSN号 | 0002-7863 |
| DOI | 10.1021/jacs.9b08362 |
| 文献子类 | 期刊论文 |
| 英文摘要 | Great enthusiasm in single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) has been aroused by the discovery of M-N-x as a promising ORR catalysis center. However, the performance of SACs lags far behind that of state-of-the-art Pt due to the unsatisfactory adsorption-desorption behaviors of the reported catalytic centers. To address this issue, rational manipulation of the active site configuration toward a well-managed energy level and geometric structure is urgently desired, yet still remains a challenge. Herein, we report a novel strategy to accomplish this task through the construction of an Fe-Co dual-atom centered site. A spontaneously absorbed electron-withdrawing OH ligand was proposed to act proactively as an energy level modifier to empower easy intermediate desorption, while the triangular Fe-Co-OH coordination facilitates O-O bond scission. Benefiting from these attributes, the as-constructed FeCoN5-OH site enables an ORR onset potential and half-wave potential of up to 1.02 and 0.86 V (vs RHE), respectively, with an intrinsic activity over 20 times higher than the single-atom FeN4 site. Our finding not only opens up a novel strategy to tailor the electronic structure of an atomic site toward boosted activity but also provides new insights into the fundamental understanding of diatomic sites for ORR electrocatalysis. |
| 语种 | 英语 |
| 源URL | [http://ir.sinap.ac.cn/handle/331007/31998]  |
| 专题 | 上海应用物理研究所_中科院上海应用物理研究所2011-2017年 |
| 作者单位 | 1.Chinese Acad Sci, Changchun Inst Appl Chem, Jilin Prov Key Lab Low Carbon Chem Power, State Key Lab Electroanalyt Chem, Changchun 130022, Jilin, Peoples R China; 2.Wuhan Univ, Coll Chem & Mol Sci, Hubei Electrochem Power Sources Key Lab, Wuhan 430072, Hubei, Peoples R China; 3.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China; 4.Univ Electrocommun, Innovat Res Ctr Fuel Cells, Chofu, Tokyo 1828585, Japan; 5.Chinese Acad Sci, Shanghai Adv Res Inst, Zhangjiang Natl Lab, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China |
| 推荐引用方式 GB/T 7714 | Xiao, ML,Chen, YT,Zhu, JB,et al. Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2019,141(44):17763-17770. |
| APA | Xiao, ML.,Chen, YT.,Zhu, JB.,Zhang, H.,Zhao, X.,...&Xing, W.(2019).Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(44),17763-17770. |
| MLA | Xiao, ML,et al."Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.44(2019):17763-17770. |
入库方式： OAI收割
来源：上海应用物理研究所
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