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Generating singlet oxygen bubbles: a new mechanism for gas-liquid oxidations in water.

ABSTRACT: Laser-coupled microphotoreactors were developed to bubble singlet oxygen [(1)O(2) ((1)?(g))] into an aqueous solution containing an oxidizable compound. The reactors consisted of custom-modified SMA fiberoptic receptacles loaded with 150 ?m silicon phthalocyanine glass sensitizer particles, where the particles were isolated from direct contact with water by a membrane adhesively bonded to the bottom of each device. A tube fed O(2) gas to the reactor chambers. In the presence of O(2), singlet oxygen was generated by illuminating the sensitizer particles with 669 nm light from an optical fiber coupled to the top of the reactor. The generated (1)O(2) was transported through the membrane by the O(2) stream and formed bubbles in solution. In solution, singlet oxygen reacted with probe compounds (9,10-anthracene dipropionate dianion, trans-2-methyl-2-pentanoate anion, N-benzoyl-D,L-methionine, or N-acetyl-D,L-methionine) to give oxidized products in two stages. The early stage was rapid and showed that (1)O(2) transfer occurred via bubbles mainly in the bulk water solution. The later stage was slow; it arose only from (1)O(2)-probe molecule contact at the gas/liquid interface. A mechanism is proposed that involves (1)O(2) mass transfer and solvation, where smaller bubbles provide better penetration of (1)O(2) into the flowing stream due to higher surface-to-volume contact between the probe molecules and (1)O(2).

SUBMITTER: Bartusik D

PROVIDER: S-EPMC3329934 | biostudies-literature | 2012 Feb

REPOSITORIES: biostudies-literature

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Generating singlet oxygen bubbles: a new mechanism for gas-liquid oxidations in water.

Bartusik Dorota D Aebisher David D Ghafari BiBi B Lyons Alan M AM Greer Alexander A

Langmuir : the ACS journal of surfaces and colloids 20120120 5

Laser-coupled microphotoreactors were developed to bubble singlet oxygen [(1)O(2) ((1)Δ(g))] into an aqueous solution containing an oxidizable compound. The reactors consisted of custom-modified SMA fiberoptic receptacles loaded with 150 μm silicon phthalocyanine glass sensitizer particles, where the particles were isolated from direct contact with water by a membrane adhesively bonded to the bottom of each device. A tube fed O(2) gas to the reactor chambers. In the presence of O(2), singlet oxy ...[more]

PMID: 22260325

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Project description:In electrochemical processes, gas bubbles on the electrode can cause an increase in both overpotential and ohmic voltage drop which leads to higher energy consumption. Applying power ultrasound during water electrolysis can help to reduce the overpotential, enhance mass transfer, and save energy. In this study, we investigated the effect of ultrasound (20 kHz) on the hydrogen evolution reaction (HER) on a stainless steel plate with varying concentrations of NaOH solutions at 298 K, using linear sweep voltammetry (LSV). We especially focused on understanding the bubble behavior on the stainless steel plate during HER using high-speed imaging in ultrasonic field. When ultrasound was applied to solutions with NaOH concentrations of 0.1, 0.5, 1 M, the current density increased by about 9.0, 5.9, 2.8 %, respectively. As the ultrasound irradiation began, the bubbles tended to hover around on the electrode surface, coalescing with other bubbles, rather than rising. When the size of the coalesced bubbles became too large to stay on the surface of the electrode, they were expelled from the ultrasonic field. The repeated collapse and coalescence of these bubbles was observed while they were rising. The velocity increased about 2 times when ultrasound irradiation began, and increased by more than 6 times in the ultrasonic field. More nucleation of bubbles was observed on the electrode in the ultrasonic field. Using ultrasound reduced the critical diameter of bubbles which detached from the electrode, from 58.0 to 15.9 μm, and the residence time of the bubbles, from 533 to 118 ms. Further, when the ultrasound was applied, the mean diameter of bubbles decreased from 71.8 to 17 μm. Hence, bubble coverage on the electrode surface decreased from 8.3 to 1 % despite an increase in the total number of bubbles. As a result, ultrasound was found to be effective for hydrogen production during water electrolysis, increasing current by the faster removal of gas from the stainless steel plate.

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Generating singlet oxygen bubbles: a new mechanism for gas-liquid oxidations in water.

Publications

Generating singlet oxygen bubbles: a new mechanism for gas-liquid oxidations in water.

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