Photoinduced Excited State Electron Transfer at Liquid/Liquid Interfaces

Cooper, Jason K.; Benjamin, Ilan

doi:10.1021/jp409541u

Cited by 9 publications

(8 citation statements)

References 131 publications

(308 reference statements)

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“…Molecular dynamics calculations of the reorganization free energy and solvation dynamics in the C314 at water/DMA system gave results in agreement with the experiments (114). The calculations suggest that the rate enhancement at the interface relative to the bulk is likely due to faster solvation dynamics at the interface.…”

Section: Photoinduced Et At Liquid/liquid Interfacessupporting

confidence: 80%

Reaction Dynamics at Liquid Interfaces

Benjamin

2015

Annu. Rev. Phys. Chem.

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The liquid interface is a narrow, highly anisotropic region, characterized by rapidly varying density, polarity, and molecular structure. I review several aspects of interfacial solvation and show how these affect reactivity at liquid/liquid interfaces. I specifically consider ion transfer, electron transfer, and SN2 reactions, showing that solvent effects on these reactions can be understood by examining the unique structure and dynamics of the liquid interface region.

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Section: Photoinduced Et At Liquid/liquid Interfacessupporting

confidence: 80%

Reaction Dynamics at Liquid Interfaces

Benjamin

2015

Annu. Rev. Phys. Chem.

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“…Electron transfer at interfaces has a long history that is justified by a broad applicability ranging from electrochemistry to biology and solar energy technologies (see ref for a recent review on these processes). Likewise, in bulk solution, Marcus theory − can account for the observed solvent effects on electron transfer at interfaces. , A study of photoinduced electron transfer at water/dimethylaniline interfaces , concluded that the interfacial processes are faster than the bulk processes, possibly due to faster solvation dynamics at the interface . The stability of solvated electrons at aqueous interfaces has also been studied, − and simulations have predicted that the water surface electron affinity is ∼0.6 eV higher than in the bulk, and that the conduction band edge is deeper in energy.…”

Section: Discussionmentioning

confidence: 99%

“…203,204 A study of photoinduced electron transfer at water/dimethylaniline interfaces 205,206 concluded that the interfacial processes are faster than the bulk processes, possibly due to faster solvation dynamics at the interface. 207 The stability of solvated electrons at aqueous interfaces has also been studied, [208][209][210] and simulations have predicted that the water surface electron affinity is ~0.6 eV higher than in the bulk, and that the conduction band edge is deeper in energy. Electron transfer is also relevant in pcet mechanisms and can be significantly affected by aqueous solvation, as shown for the 3 SO2 + H2O reaction 116 and the H2CO + HO2 reaction.…”

Section: Scheme 1 Factors Affecting Photo-induced Reactions At the Ai...mentioning

confidence: 99%

Photoinduced Oxidation Reactions at the Air–Water Interface

et al. 2020

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Chemistry on water is a fascinating area of research. The surface of water and the interfaces between water and air or hydrophobic media represent asymmetric environments with unique properties that lead to unexpected solvation effects on chemical and photochemical processes. Indeed, the features of interfacial reactions differ, often drastically, from those of bulk-phase reactions. In this Perspective, we focus on photoinduced oxidation reactions, which have attracted enormous interest in recent years because of their implications in many areas of chemistry, including atmospheric and environmental chemistry, biology, electrochemistry, and solar energy conversion. We have chosen a few representative examples of photoinduced oxidation reactions to focus on in this Perspective. Although most of these examples are taken from the field of atmospheric chemistry, they were selected because of their broad relevance to other areas. First, we outline a series of processes whose photochemistry generates hydroxyl radicals. These OH precursors include reactive oxygen species, reactive nitrogen species, and sulfur dioxide. Second, we discuss processes involving the photooxidation of organic species, either directly or via photosensitization. The photochemistry of pyruvic acid and fatty acid, two examples that demonstrate the complexity and versatility of this kind of chemistry, is described. Finally, we discuss the physicochemical factors that can be invoked to explain the kinetics and thermodynamics of photoinduced oxidation reactions at aqueous interfaces and analyze a number of challenges that need to be addressed in future studies.

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“…So far, X-ray reflectivity and molecular dynamics have not been applied to study electron transfer reactions, but these techniques would help to elucidate how the reactions actually happen. Recently, molecular dynamics simulations have been employed to study photoinduced electron transfer between coumarin 314 and N,N-dimethylaniline [32]. Spectroscopic techniques such as surface second harmonic generation [33], potential modulated fluorescence [29] etc.…”

Section: Graphical Abstract 1 Introductionmentioning

confidence: 99%

Heterogeneous versus homogeneous electron transfer reactions at liquid–liquid interfaces: The wrong question?

Peljo

Smirnov

Girault

2016

Journal of Electroanalytical Chemistry

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The exact mechanism of the electron transfer reactions at liquid-liquid interfaces still remains a source of interrogation. The purpose of this paper is to revisit this topic using a finite element simulation approach to analyze cyclic voltammograms for some previously published systems. Also, we compare the current obtained in the absence or presence of an adsorbed gold nanoparticle film. The current results indicate that the electron transfer between ferrocene in the organic phase and hexacyanoferrate(III) in the aqueous phase takes place by potential independent homogeneous reaction in the aqueous phase, while the observed potential dependence stems from that of the concomitant ion transfer reaction of ferrocenium. In the presence of the interfacial gold nanofilm the electron transfer takes place by a bipolar mechanism where the electrons are shuttled through the metallic nanofilm.

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Photoinduced Excited State Electron Transfer at Liquid/Liquid Interfaces

Cited by 9 publications

References 131 publications

Reaction Dynamics at Liquid Interfaces

Reaction Dynamics at Liquid Interfaces

Photoinduced Oxidation Reactions at the Air–Water Interface

Heterogeneous versus homogeneous electron transfer reactions at liquid–liquid interfaces: The wrong question?

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