Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 119, Issue 12, Pages -Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.2200991119
Keywords
microdroplet; pyridine; negative ion; air-water interface; hydroxyl
Categories
Funding
- National Natural Science Foundation of China (NSF) [22003027, 22174073]
- National Key Research and Development (R&D) Program of China [2018YFE0115000]
- NSF of Tianjin City [21JCJQJC00010]
- Beijing National Laboratory for Molecular Sciences [BNLMS202106]
- Frontiers Science Center for New Organic Matter at Nankai University [63181206]
- Air Force Office of Scientific Research through the Basic Research Initiative [AFOSR FA9550-16-1-0113]
- Air Force Office of Scientific Research through Multidisciplinary University Research Initiative (MURI) program [AFOSR FA9550-21-1-0170]
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This study reveals that the formation of the anion of pyridine in water microdroplets provides a green chemistry approach for synthesizing value-added chemicals.
The anion of pyridine, C5H5N-, has been thought to be short lived in the gas phase and was only previously observed indirectly. In the condensed phase, C5H5N- is high electric field at the air-water interface of a microdroplet helps OH- to transfer an electron to pyridine to form C5H5N- and the hydroxyl radical center dot OH. Oxidation products of the Py reacting with center dot OH are also observed in the mass spectrum recorded in positive mode, which further supports this mechanism. The present study pushes the limits of the reducing and oxidizing power of water microdroplets to a new level, emphasizing how different the behavior of microdroplets can be from bulk water. We also note that the easy formation of C5H5N- in water microdroplets presents a green chemistry way to synthesize value-added chemicals.
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