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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)
2016
发表期刊JOURNAL OF PHYSICAL CHEMISTRY LETTERS (IF:9.353[JCR-2016],8.334[5-Year])
ISSN1948-7185
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.
DOI10.1021/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
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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
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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.
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