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High Electric Fields on Water Microdroplets Catalyze Spontaneous and Fast Reactions in Halogen-Bond Complexes.
Zhu, Chenghui; Pham, Le Nhan; Yuan, Xu; Ouyang, Haoran; Coote, Michelle L; Zhang, Xinxing.
Afiliação
  • Zhu C; College of Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Renewable Energy Conversion and Storage Centre, Tianjin Key Laboratory of Biosensing and Molecular Recognition, Frontiers Science Centre for New Organic Matter, Nankai University, Tianjin, 300071, Ch
  • Pham LN; Beijing National Laboratory for Molecular Sciences, Beijing, 100190, China.
  • Yuan X; Institute for Nanoscale Science & Technology, Flinders University, Adelaide, South Australia 5042, Australia.
  • Ouyang H; College of Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Renewable Energy Conversion and Storage Centre, Tianjin Key Laboratory of Biosensing and Molecular Recognition, Frontiers Science Centre for New Organic Matter, Nankai University, Tianjin, 300071, Ch
  • Coote ML; Beijing National Laboratory for Molecular Sciences, Beijing, 100190, China.
  • Zhang X; College of Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Renewable Energy Conversion and Storage Centre, Tianjin Key Laboratory of Biosensing and Molecular Recognition, Frontiers Science Centre for New Organic Matter, Nankai University, Tianjin, 300071, Ch
J Am Chem Soc ; 145(39): 21207-21212, 2023 Oct 04.
Article em En | MEDLINE | ID: mdl-37724917
The use of external electric fields as green and efficient catalysts in synthetic chemistry has recently received significant attention for their ability to deliver remarkable control of reaction selectivity and acceleration of reaction rates. Technically, methods of generating high electric fields in the range of 1-10 V/nm are limited, as in-vacuo techniques have obvious scalability issues. The spontaneous high fields at various interfaces promise to solve this problem. In this study, we take advantage of the spontaneous high electric field at the air-water interface of sprayed water microdroplets in the reactions of several halogen bond systems: Nu:--X-X, where Nu: is pyridine or quinuclidine and X is bromine or iodine. The field facilitates ultrafast electron transfer from Nu:, yielding a Nu-X covalent bond and causing the X-X bond to cleave. This reaction occurs in microseconds in microdroplets but takes days to weeks in bulk solution. Density functional theory calculations predict that the reaction becomes barrier-free in the presence of oriented external electric fields, supporting the notion that the electric fields in the water droplets are responsible for the catalysis. We anticipate that microdroplet chemistry will be an avenue rich in opportunities in the reactions facilitated by high electric fields and provides an alternative way to tackle the scalability problem.

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: J Am Chem Soc Ano de publicação: 2023 Tipo de documento: Article

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: J Am Chem Soc Ano de publicação: 2023 Tipo de documento: Article