Br?nsted basicity of the air-water interface

Mishra H.; Enami S.; Nielsen R.J.Stewart L.A.Hoffmann M.R.Goddard III W.A.Colussi A.J.

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Br?nsted basicity of the air-water interface

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Differences in the extent of protonation of functional groups lying on either side of water-hydrophobe interfaces are deemed essential to enzymatic catalysis, molecular recognition, bioenergetic transduction, and atmospheric aerosol-gas exchanges. The sign and range of such differences, however, remain conjectural. Herein we report experiments showing that gaseous carboxylic acids RCOOH(g) begin to deprotonate on the surface of water significantly more acidic than that supporting the dissociation of dissolved acids RCOOH(aq). Thermodynamic analysis indicates that > 6 H_2O molecules must participate in the deprotonation of RCOOH(g) on water, but quantum mechanical calculations on a model air-water interface predict that such event is hindered by a significant kinetic barrier unless OH~- ions are present therein. Thus, by detecting RCOO~- we demonstrate the presence of OH ~- on the aerial side of on pH > 2 water exposed to RCOOH(g). Furthermore, because in similar experiments the base (Me)_3N(g) is protonated only on pH 1 nm) deeper shear planes probed in electrophoresis, thereby implying the existence of OH~- gradients in the interfacial region. This fact could account for the weak OH~- signals detected by surface-specific spectroscopies.

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《Proceedings of the National Academy of Sciences of the United States of America》 |2012年第46期|18679-18683|共5页
作者
Mishra H.; Enami S.; Nielsen R.J.Stewart L.A.Hoffmann M.R.Goddard III W.A.Colussi A.J.;
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作者单位

Ronald and Maxine Linde Center for Global Environmental Science, California Institute of Technology, Pasadena, CA 91125, United States;

Hakubi Center for Advanced Research, Kyoto University, Kyoto 606-8302, Japan;

Materials and Process Simulation Center, California Institute of Technology, Pasadena, CA 91125, United StatesPhysics Department, University of California, Santa Barbara, Santa Barbara, CA 93106, United StatesMaterials Science Department, California Institute of Technology, Pasadena, CA 91125, United States;

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收录信息美国《科学引文索引》(SCI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
原文格式 PDF
正文语种英语
中图分类自然科学总论;
关键词
Gas-liquid reactions; Interfacial proton transfer; Surface potential; Water surface acidity;

Br?nsted basicity of the air-water interface

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