Tracking Co(I) Intermediate in Operando in Photocatalytic Hydrogen Evolution by X-ray Transient Absorption Spectroscopy and DFT Calculation | |
Li, ZJ; Zhan F(展飞); Zhan, F; Xiao, HY; Zhang, XY; Kong, QY; Fan, XB; Liu, WQ; Huang, MY; Huang, C; Gao, YJ; Li, XB; Meng, QY; Feng, K; Chen, B; Tung, CH; Zhao, HF; Tao, Y; Wu, LZ; Zhao HF(赵海峰)![]() | |
2016 | |
发表期刊 | JOURNAL OF PHYSICAL CHEMISTRY LETTERS (IF:9.353[JCR-2016],8.334[5-Year]) |
ISSN | 1948-7185 |
卷号 | 7期号:24页码:5253-5258 |
通讯作者 | 陶冶 |
文章类型 | Article |
摘要 | X-ray transient absorption spectroscopy (XTA) and optical transient spectroscopy (OTA) were used to probe the Co(I) intermediate generated in situ from an aqueous photocatalytic hydrogen evolution system, with [Ru-II(bpy)(3)]Cl-2 center dot 6H(2)O as the photosensitizer, ascorbic acid/ascorbate as the electron donor, and the Co-polypyridyl complex ([Co-II(DPA-Bpy)Cl]Cl) as the precatalyst. Upon exposure to light, the XTA measured at Co K-edge visualizes the grow and decay of the Co(I) intermediate, and reveals its Co-N bond contraction of 0.09 +/- 0.03 angstrom. Density functional theory (DFT) calculations support the bond contraction and illustrate that the metal-to-ligand pi back bonding greatly stabilizes the penta-coordinated Co(I) intermediate, which provides easy photon access. To the best of our knowledge, this is the first example of capturing the penta-coordinated Co(I) intermediate in operando with bond contraction by XTA, thereby providing new insights for fundamental understanding of structure-function relationship of cobalt-based molecular catalysts. |
DOI | 10.1021/acs.jpclett.6b02479 |
关键词[WOS] | AQUEOUS-SOLUTION ; COBALT COMPLEX ; POLYPYRIDYL CATALYSTS ; WATER ; REDUCTION ; PATHWAYS ; COBALOXIME ; MECHANISM ; DYNAMICS ; SYSTEM |
收录类别 | SCI |
语种 | 英语 |
WOS类目 | Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical |
WOS记录号 | WOS:000390087000046 |
引用统计 | 正在获取...
|
文献类型 | 期刊论文 |
条目标识符 | https://ir.ihep.ac.cn/handle/311005/260359 |
专题 | 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 | Li, ZJ,Zhan F,Zhan, F,et al. Tracking Co(I) Intermediate in Operando in Photocatalytic Hydrogen Evolution by X-ray Transient Absorption Spectroscopy and DFT Calculation[J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS,2016,7(24):5253-5258. |
APA | Li, ZJ.,展飞.,Zhan, F.,Xiao, HY.,Zhang, XY.,...&陶冶.(2016).Tracking Co(I) Intermediate in Operando in Photocatalytic Hydrogen Evolution by X-ray Transient Absorption Spectroscopy and DFT Calculation.JOURNAL OF PHYSICAL CHEMISTRY LETTERS,7(24),5253-5258. |
MLA | Li, ZJ,et al."Tracking Co(I) Intermediate in Operando in Photocatalytic Hydrogen Evolution by X-ray Transient Absorption Spectroscopy and DFT Calculation".JOURNAL OF PHYSICAL CHEMISTRY LETTERS 7.24(2016):5253-5258. |
条目包含的文件 | ||||||
文件名称/大小 | 文献类型 | 版本类型 | 开放类型 | 使用许可 |
个性服务 |
推荐该条目 |
保存到收藏夹 |
查看访问统计 |
导出为Endnote文件 |
谷歌学术 |
谷歌学术中相似的文章 |
[Li, ZJ]的文章 |
[展飞]的文章 |
[Zhan, F]的文章 |
百度学术 |
百度学术中相似的文章 |
[Li, ZJ]的文章 |
[展飞]的文章 |
[Zhan, F]的文章 |
必应学术 |
必应学术中相似的文章 |
[Li, ZJ]的文章 |
[展飞]的文章 |
[Zhan, F]的文章 |
相关权益政策 |
暂无数据 |
收藏/分享 |
除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。
修改评论