Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes
文献类型：期刊论文
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| 作者 | Feng, QC; Zhao, S; Wang, Y; Dong, JC ; Chen, WX; He, DS; Wang, DS; Yang, J; Zhu, YM; Zhu, HL
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| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
 ; JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
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| 出版日期 | 2017 ; 2017 |
| 卷号 | 139期号:21页码:7294-7301 |
| ISSN号 | 0002-7863 ; 0002-7863 |
| DOI | 10.1021/jacs.7b01471 ; 10.1021/jacs.7b01471 |
| 文献子类 | Article ; Article |
| 英文摘要 | Improving the catalytic selectivity of Pd catalysts is of key importance for various industrial processes and remains a challenge so far. Given the unique properties of single-atom catalysts, isolating contiguous Pd atoms into a single-Pd site with another metal to form intermetallic structures is an effective way to endow Pd with high catalytic selectivity and to stabilize the single site with the intermetallic structures. Based on density functional theory modeling, we demonstrate that the (110) surface of Pm (3) over barm PdIn with single-atom Pd sites shows high selectivity for semihydrogenation of acetylene, whereas the (111) surface of P4/mmm Pd3In with Pd trimer sites shows low selectivity. This idea has been further validated by experimental results that intermetallic PdIn nanocrystals mainly exposing the (110) surface exhibit much higher selectivity for acetylene hydrogenation than Pd3In nanocrystals mainly exposing the (111) surface (92% vs 21% ethylene selectivity at 90 degrees C). This work provides insight for rational design of bimetallic metal catalysts with specific catalytic properties.; Improving the catalytic selectivity of Pd catalysts is of key importance for various industrial processes and remains a challenge so far. Given the unique properties of single-atom catalysts, isolating contiguous Pd atoms into a single-Pd site with another metal to form intermetallic structures is an effective way to endow Pd with high catalytic selectivity and to stabilize the single site with the intermetallic structures. Based on density functional theory modeling, we demonstrate that the (110) surface of Pm (3) over barm PdIn with single-atom Pd sites shows high selectivity for semihydrogenation of acetylene, whereas the (111) surface of P4/mmm Pd3In with Pd trimer sites shows low selectivity. This idea has been further validated by experimental results that intermetallic PdIn nanocrystals mainly exposing the (110) surface exhibit much higher selectivity for acetylene hydrogenation than Pd3In nanocrystals mainly exposing the (111) surface (92% vs 21% ethylene selectivity at 90 degrees C). This work provides insight for rational design of bimetallic metal catalysts with specific catalytic properties. |
| WOS关键词 | ABSORPTION FINE-STRUCTURE ; ABSORPTION FINE-STRUCTURE ; ATOMICALLY DISPERSED PALLADIUM ; LIQUID-PHASE HYDROGENATION ; TOTAL-ENERGY CALCULATIONS ; WAVE BASIS-SET ; STRUCTURE SPECTROSCOPY ; CO OXIDATION ; STRUCTURE STANDARDS ; SURFACE DYNAMICS ; PART II ; ATOMICALLY DISPERSED PALLADIUM ; LIQUID-PHASE HYDROGENATION ; TOTAL-ENERGY CALCULATIONS ; WAVE BASIS-SET ; STRUCTURE SPECTROSCOPY ; CO OXIDATION ; STRUCTURE STANDARDS ; SURFACE DYNAMICS ; PART II |
| WOS研究方向 | Chemistry ; Chemistry |
| 语种 | 英语 ; 英语 |
| WOS记录号 | WOS:000402691800027 ; WOS:000402691800027 |
| 源URL | [http://ir.ihep.ac.cn/handle/311005/285214]  |
| 专题 | 高能物理研究所_多学科研究中心 高能物理研究所_管理与技术支持 高能物理研究所_东莞分部 中国科学院高能物理研究所_中国散裂中子源 |
| 作者单位 | 中国科学院高能物理研究所 |
| 推荐引用方式 GB/T 7714 | Feng, QC,Zhao, S,Wang, Y,et al. Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes, Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2017, 2017,139, 139(21):7294-7301, 7294-7301. |
| APA | Feng, QC.,Zhao, S.,Wang, Y.,Dong, JC.,Chen, WX.,...&朱海亮.(2017).Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,139(21),7294-7301. |
| MLA | Feng, QC,et al."Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 139.21(2017):7294-7301. |
入库方式： OAI收割
来源：高能物理研究所
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