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); Tao Y(陶冶)
刊名JOURNAL OF PHYSICAL CHEMISTRY LETTERS
2016
卷号7期号:24页码:5253-5258
DOI10.1021/acs.jpclett.6b02479
通讯作者陶冶
文章类型期刊论文
英文摘要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.
类目[WOS]Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical
关键词[WOS]AQUEOUS-SOLUTION ; COBALT COMPLEX ; POLYPYRIDYL CATALYSTS ; WATER ; REDUCTION ; PATHWAYS ; COBALOXIME ; MECHANISM ; DYNAMICS ; SYSTEM
语种英语
WOS记录号WOS:000390087000046
引用统计
被引频次:2[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.ihep.ac.cn/handle/311005/260359
专题中国科学院高能物理研究所_多学科研究中心_期刊论文
中国科学院高能物理研究所_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
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
20161190.pdf(2424KB)期刊论文作者接受稿开放获取CC BY-NC-SA浏览 请求全文
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
文件名: 20161190.pdf
格式: Adobe PDF
所有评论 (0)
暂无评论
 

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。