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Kinetics and mechanisms of reactions for hydrated electron with chlorinated benzenes in aqueous solution

Frontiers of Environmental Science & Engineering 2015年第4期9卷 583-590页

作者： Haixia YUAN Huxiang PAN Jin SHI Hongjing LI Wenbo DONG Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention Department of Environmental Science & Engineering Fudan University Shanghai 200433 China Institutes of Naval Medicine Shanghai 200433 China

The reactions between chlorinated benzenes （CBzs） and hydrated electron （eaq^-） were investigated by the electron beam （EB） and laser flash photolysis （LFP） experiments. Under the EB irradiation, the effects of irradiation dose, initial concentration and the number of Cl atoms on the removal efficiencies were further examined. At 10 kGy, the removal efficiencies of mono-CB, 1,3-diCB, 1,2-diCB and 1,4-diCB were 41.2%, 87.2%, 84.0%, and 84.1%, respectively. While irradiation dose was 50 kGy, the removal efficiencies increased to 47.4%, 95.8%, 95.0%, and 95.2%, respectively. Irradiation of CBzs solutions has shown that the higher the initial concentration, the lower the percentage of CBzs removal. In addition to this, the dechlorination efficiencies of 1,2-dichlorobenzene （1,2-diCB）, 1,3-dichlorobenzene （1,3-diCB） and 1,4-dichlorobenzene （1,4-diCB） were much higher than that of chlorobenzene （mono-CB）. The kinetics of the reactions was achieved with nanosecond LFP. The rate constants of second-order reaction between eaq^- with mono-CB, 1,2-diCB, 1,3-diCB and 1,4-diCB were （5.3±0.4） × 10^8, （4.76±0.1） × 10^9, （1.01±0.1） × 1010 and （3.29±0.2） × 10^9 L·mol^-1·s^-1, respectively. Density functional theory （DFT） calculations were performed to determine the optical properties of unstable CBzs anion radicals, and the main absorption peaks lied in the range of 300–550 nm. The primary reaction pathway of CBzs with eaq^- was gradual dechlorination, and the major products were Cl^- and benzene （CBzs（-Cl^-））. Furthermore, biphenyl （or chlorobiphenyl） was observed during the LFP, which was probably formed by recombination of benzene radicals.

关键词： chlorinated benzenes hydrated electron electron beam laser flash photolysis

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Ultrafast Liquid-jet Photoelectron Spectroscopy of hydrated electron:A New Method for Directly Tracking electrons in Aqueous Solutions

Ultrafast Liquid-jet Photoelectron Spectroscopy of Hydrated ...

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第十五届全国化学动力学会议

作者：龙金友邱梓恒刘凯张冰 State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics Wuhan Institute of Physics and MathematicsChinese Academy of Sciences

Water is important for life,however,it is surprising that the seemingly simplest electronic structure quantity,that is,the binding energy(BE) of electrons in the highest occupied molecular orbital(HOMO),from given aqueous solutions is relatively unknown for a long *** is because photoelectron spectroscopy(PES) of liquids is technically difficult due to the incompatibility of using volatile liquids with the high vacuum required for ***,ultrafast photoelectron spectroscopy from highly volatile liquids,especially from water and aqueous solutions,has become possible due to the development of the vacuum liquid microjet technique(shown in the inset of Fig.1)and has succeeded in the direct mearsurement of the BE of hydrated electron(e(aq)),suggesting that it could be applied to study ultrafast dynamics of excited molecules in solutions[1].Currently,we have also succeeded in building this kind of new experimental setup and extended our research field from the gas phase to the liquid ***,we describe a detailed spectrometer characterization based on the spectroscopy of nitric oxide in the gas phase,and then present the direct measurement of the vertical binding energy(VBE) of a hydrated electron in bulk water by using the time-resolved photoelectron spectroscopy(TRPES)of the charge-transfer-to-solvent(CTTS) reaction in aqueous NaI *** importantly,the observed time-dependent PKED also reveals a wealth of information on the ultrafast CTTS dynamics,i.e.,the evolution of the solvated electrons(e(aq))(as shown in Fig.1).Applications of liquid-jet PES go well beyond the example given here,including such as solvation of biological relevant molecules by water,aqueous electron attachment,charge-transfer and light-energy conversion *** thus we are looking forward to gaining new insights into the in situ photoreactions that are closely related to real life science within aqueous environment.

关键词： water hydrated electron aqueous solution photoelectron spectroscopy

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Visualization of gold nanoparticles formation in DC plasma-liquid systems

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Plasma Science and Technology 2021年第7期23卷 144-152页

作者： Zhaoyuan LIU Qiang CHEN Qinghuo LIU Kostya(Ken)OSTRIKOV Shenzhen Research Institute of Xiamen University Institute of Electromagnetics and AcousticsFujian Provincial Key Laboratory of Plasma and Magnetic ResonanceKey Laboratory of Electromagnetic Wave Science and Detection TechnologyXiamen UniversityXiamen 361005People’s Republic of China Department of Electrical and Computer Engineering Duke UniversityDurhamNC 27708United States of America School of Chemistry and Physics Queensland University of TechnologyBrisbaneQueensland 4000Australia

Dual argon plasmas ignited by one direct current power source are used to treat an aqueous solution of hydrogen tetrachloroaurate-(Ⅲ)trihydrate(HAuCl_(4)·3H_(2)O)which is contained in an H-type electrochemical *** solution contained in one cell acts as a cathode,and in the other as an *** are carried out to directly visualize the formation process of gold nanoparticles(Au NPs)in separated cells of the H-type electrochemical *** results and analyzes suggest that hydrogen peroxide and hydrated electrons generated from the plasma-liquid interactions play the roles of reductants in the solutions,*** peroxide can be generated in the case of the liquid being a cathode or an anode,while most of hydrated electrons are formed in the case of the liquid being an ***,the reduction of the AuCl_(4)−ions is mostly attributed to the hydrogen peroxide as the liquid acts as a cathode,while to the hydrogen peroxide and hydrated electrons as the liquid acts as an ***,the p H value of the solution can be used to tune the formation processes and final form of the Au NPs due to its mediation of reductants.

关键词： dual plasma gold nanoparticles hydrogen peroxide hydrated electron H-type electrochemical cell

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