Ireneo L. de la Cruz, Jr., Cheng-I. Lee, Kun-Mo Lin
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The [<sup>•</sup>OH<sub>(aq)</sub>]<sub>M</sub> in the solutions is determined from the fluorescence measurements by exciting 2-hydroxyterephthalic acid at 310 nm and detecting the fluorescence emitted at 425 nm for cases with different plasma treatment times. The developed numerical model considers both the diffusion and convection for the domain covering 1 mm above the interface with the dominant generation and consumption mechanisms considered in the discharge plume to evaluate the incoming flux of <sup>•</sup>OH<sub>(g)</sub> through the interface, which is calibrated with [<sup>•</sup>OH<sub>(aq)</sub>]<sub>M</sub> in the solution treated. The simulated results show that the transport behavior (i.e., diffusion and convection) plays only a minor role in the contribution of [<sup>•</sup>OH<sub>(aq)</sub>]<sub>S</sub>, while the electron-impact dissociation reactions play significant roles in the generation of <sup>•</sup>OH<sub>(g)</sub> in the discharge plume, leading to the high local [<sup>•</sup>OH<sub>(g)</sub>] and incoming flux of <sup>•</sup>OH<sub>(g)</sub> to the interface. The self-association reactions of <sup>•</sup>OH<sub>(g)</sub> contribute to the remarkable consumption of <sup>•</sup>OH<sub>(g)</sub>. The simulated [<sup>•</sup>OH<sub>(g)</sub>] distribution increases from the [<sup>•</sup>OH<sub>(g)</sub>]<sub>M</sub> determined at the upstream boundary to its maximum near the central region as the density reaches 9.5 × 10<sup>19</sup> m<sup>–3</sup> and decreases rapidly above the interface.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"82 1","pages":""},"PeriodicalIF":6.7000,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Investigation of OH Species in a Helium Atmospheric Pressure Plasma Jet: from Gas Phase to Liquid Phase through the Plasma–Liquid Interface\",\"authors\":\"Ireneo L. de la Cruz, Jr., Cheng-I. 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引用次数: 0
摘要
本研究建立了一种半经验一维数值模型,以平均测量的[•OH(g)](记为[•OH(g)]M)作为边界条件,以测量的[•OH(aq)](记为[•OH(aq)]M)来校准等离子体射流处理的溶液中累积的[•OH(aq)]模型(记为[•OH(aq)]S)。等离子体羽流中得到的[•OH(g)]M是根据在界面上方1mm处径向探测到的[•OH(g)]分布进行积分的。溶液中的[•OH(aq)]M通过在310 nm处激发2-羟基对苯二甲酸和在425 nm处检测不同等离子体处理时间的荧光测量来确定。所建立的数值模型考虑了界面上方1mm区域的扩散和对流,并考虑了放电羽流中主要的产生和消耗机制,以评估通过界面进入的•OH(g)通量,并用处理溶液中的[•OH(aq)]M进行校准。模拟结果表明,传输行为(即扩散和对流)对[•OH(aq)]S的贡献作用较小,而电子碰撞解离反应对放电羽流中•OH(g)的产生起着重要作用,导致了高的局部[•OH(g)]和进入界面的•OH(g)通量。•OH(g)的自缔合反应有助于•OH(g)的显著消耗。模拟的[•OH(g)]分布从上游边界处的[•OH(g)]M增大到靠近中心区域的最大值,密度达到9.5 × 1019 M - 3,在界面以上迅速减小。
Investigation of OH Species in a Helium Atmospheric Pressure Plasma Jet: from Gas Phase to Liquid Phase through the Plasma–Liquid Interface
This work develops a semiempirical 1D numerical model with average measured [•OH(g)] (denoted as [•OH(g)]M) as the boundary condition and measured [•OH(aq)] (denoted as [•OH(aq)]M) to calibrate the accumulated [•OH(aq)] modeled (denoted as [•OH(aq)]S) in the solution treated by a plasma jet. The [•OH(g)]M obtained in the plasma plume is integrated from the [•OH(g)] distribution detected in the radial direction at position 1 mm above the interface. The [•OH(aq)]M in the solutions is determined from the fluorescence measurements by exciting 2-hydroxyterephthalic acid at 310 nm and detecting the fluorescence emitted at 425 nm for cases with different plasma treatment times. The developed numerical model considers both the diffusion and convection for the domain covering 1 mm above the interface with the dominant generation and consumption mechanisms considered in the discharge plume to evaluate the incoming flux of •OH(g) through the interface, which is calibrated with [•OH(aq)]M in the solution treated. The simulated results show that the transport behavior (i.e., diffusion and convection) plays only a minor role in the contribution of [•OH(aq)]S, while the electron-impact dissociation reactions play significant roles in the generation of •OH(g) in the discharge plume, leading to the high local [•OH(g)] and incoming flux of •OH(g) to the interface. The self-association reactions of •OH(g) contribute to the remarkable consumption of •OH(g). The simulated [•OH(g)] distribution increases from the [•OH(g)]M determined at the upstream boundary to its maximum near the central region as the density reaches 9.5 × 1019 m–3 and decreases rapidly above the interface.
期刊介绍:
Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.