期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 13, 期 38, 页码 8921-8927出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.2c02335
关键词
-
类别
资金
- U.S. Department of Energy Office of Science, Division of Chemical Sciences, Geosciences and Biosciences [DE-AC02-06CH11357]
The photolysis reaction pathways of [Au(III)Cl4]- in aqueous solution were studied, showing that UV excitation breaks the Au-Cl bond to form [Au(II)Cl3]-, which then becomes highly reactive. On the other hand, intense near-infrared lasers can generate hydrated electrons from water to reduce [Au(III)Cl4]- to [Au(II)Cl3]-, leading to the formation of Au nanoparticles.
Photolysis reaction pathways of [Au(III)Cl4]- in aqueous solution have been investigated by time-resolved X-ray absorption spectroscopy. Ultraviolet excitation directly breaks the Au-Cl bond in [Au(III)Cl4]- to form [Au(II)Cl3]- that becomes highly reactive within 79 ps. Disproportionation of [Au(II)Cl3]- generates [Au(I)Cl2]-, which is stable for <= 10 mu s. In contrast, intense near-infrared lasers photolyze water to generate hydrated electrons, which then reduce [Au(III)Cl4]- to [Au(II)Cl3]- at 5 ns. Hydrated electrons further induce a chain reaction from [Au(II)Cl3]- to [Au(0)Cl]- by successively removing one Cl-. The zero-valency Au anions quickly polymerize and condense to form Au nanoparticles, which become the dominating product after 400 s. Our results reveal that the condensation of zero-valency Au starts with dimerization of gold clusters coordinated with chloride ions rather than direct condensation of pristine Au atoms.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据