期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 139, 期 33, 页码 11519-11526出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b05116
关键词
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资金
- National Institutes of Health (NIH) [GM57375]
- National Science Foundation (NSF) [CHE-1265679]
- Chevron Energy Technology Company
- Natural Sciences and Engineering Research Council of Canada
- Canadian Institutes of Health Research (CIHR)
- Saskatchewan Health Research Foundation
- University of Saskatchewan
- Canada Research Chairs
- CIHR
- CIHR/Heart and Stroke Foundation of Canada Synchrotron Medical Imaging Team Grant [CIF 99472]
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- DOE Office of Biological and Environmental Research
- NIH, National Institute of General Medical Sciences [P41GM103393]
- CIHR Training grant in Health Research using Synchrotron Techniques (CIHR-THRUST)
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1265679] Funding Source: National Science Foundation
- Grants-in-Aid for Scientific Research [26620025] Funding Source: KAKEN
Sulfur-based thiyl radicals are known to be involved in a wide range of chemical and biological processes, but they are often highly reactive, which makes them difficult to observe directly. We report herein X-ray absorption spectra and analysis that support the direct observation of two different thiyl species generated photochemically by X-ray irradiation. The thiyl radical sulfur K-edge X-ray absorption spectra of both species are characterized by a uniquely low energy transition at about 2465 eV, which occurs at a lower energy than any previously observed feature at the sulfur K-edge and corresponds to a 1s -> 3p transition to the singly occupied molecular orbital of the free radical. Our results constitute the first observation of substantial levels of thiyl radicals generated by X-ray irradiation and detected by sulfur Kedge X-ray absorption spectroscopy.
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