Size Sensitivity of Supported Palladium Species on Layered Double Hydroxides for the Electro-oxidation Dehydrogenation of Hydrazine: From Nanoparticles to Nanoclusters and Single Atoms
文献类型：期刊论文
| 作者 | Liu, Guihao; Nie, Tianqi; Wang, Huijuan; Shen, Tianyang; Sun, Xiaoliang; Bai, Sha ; Zheng, Lirong; Song, Yu-Fei
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| 刊名 | ACS CATALYSIS
 |
| 出版日期 | 2022 |
| 卷号 | 12期号:17页码:10711-10717 |
| DOI | 10.1021/acscatal.2c02628 |
| 文献子类 | Article |
| 英文摘要 | The hydrazine oxidation reaction (HzOR) is structure-sensitive, and a slight modification of the catalyst structure can generate a significant change in activity. To date, no study on the size effect of the catalyst at a subnanometer scale on HzOR has been reported yet. Herein, we report the fabrication of Pd species with sizes ranging from nanoparticles (NPs) and nanoclusters (NCs) to single atoms (SAs) onto a NiFe-layered double hydroxide by fine-tuning precursors and reduction methods. When applied for the electro-oxidation dehydrogenation of hydrazine, the as-prepared Pd NCs/NiFe exhibit a current density of 4.3 A mgPd-1 at 0.35 V versus RHE. It should be noted that the mass activity of Pd NCs/NiFe was 36 times that of Pd SAs/NiFe and 7 times that of Pd NPs/NiFe, respectively. The in situ electrochemical impedance spectroscopy and density functional theory calculation demonstrate that different from previous studies, both the Pd SAs/NiFe and Pd NPs/NiFe are suboptimal in HzOR due to the isolated active sites of the Pd SAs/NiFe and large steric hindrance of Pd NPs/NiFe, respectively. Instead, the strong intracluster interactions of Pd NCs/NiFe lift the d-band center closer to the Fermi level, leading to stronger hybridization of Pd d-orbitals and the σ orbitals of N2H4 molecules. Consequently, the excellent performance of Pd NCs/NiFe can be attributed to its multiple neighboring metal sites, high d-band center, and small steric hindrance. © 2022 American Chemical Society. |
| 电子版国际标准刊号 | 2155-5435 |
| 语种 | 英语 |
| WOS记录号 | WOS:000863485700001 |
| 源URL | [http://ir.ihep.ac.cn/handle/311005/299081]  |
| 专题 | 高能物理研究所_加速器中心 高能物理研究所_多学科研究中心 |
| 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 | Liu, Guihao,Nie, Tianqi,Wang, Huijuan,et al. Size Sensitivity of Supported Palladium Species on Layered Double Hydroxides for the Electro-oxidation Dehydrogenation of Hydrazine: From Nanoparticles to Nanoclusters and Single Atoms[J]. ACS CATALYSIS,2022,12(17):10711-10717. |
| APA | Liu, Guihao.,Nie, Tianqi.,Wang, Huijuan.,Shen, Tianyang.,Sun, Xiaoliang.,...&Song, Yu-Fei.(2022).Size Sensitivity of Supported Palladium Species on Layered Double Hydroxides for the Electro-oxidation Dehydrogenation of Hydrazine: From Nanoparticles to Nanoclusters and Single Atoms.ACS CATALYSIS,12(17),10711-10717. |
| MLA | Liu, Guihao,et al."Size Sensitivity of Supported Palladium Species on Layered Double Hydroxides for the Electro-oxidation Dehydrogenation of Hydrazine: From Nanoparticles to Nanoclusters and Single Atoms".ACS CATALYSIS 12.17(2022):10711-10717. |
入库方式： OAI收割
来源：高能物理研究所
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