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题名: O-2((1)Delta) quenching mechanism in Cl-2/basic hydrogen peroxide(basic deuterium peroxide) gas/liquid reaction and the determination of O-2((1)Delta)/BHP(BDP) interface free energy
作者: Shi, Wenbo1;  Deng, Liezheng1;  Du, Shuyan1;  Cui, Rongrong1;  Yang, Heping1;  Sha, Guohe1;  Zhang, Cunhao1
刊名: JOURNAL OF PHYSICAL CHEMISTRY C
发表日期: 2008-06-26
DOI: 10.1021/jp8005348
卷: 112, 期:25, 页:9412-9417
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Nanoscience & Nanotechnology ;  Materials Science, Multidisciplinary
研究领域[WOS]: Chemistry ;  Science & Technology - Other Topics ;  Materials Science
英文摘要: In a jet-type singlet oxygen generator, we have studied the generation of O-2((1)Delta) via the reaction of chlorine gas with aqueous basic hydrogen peroxide (BHP) and with basic deuterium peroxide (BDP). The O-2((1)Delta) detachment yield with BDP is measured to be 72.5 +/- 1.5%, merely 2.5% higher than that with BHP, despite a 10 times longer O-2((1)Delta) lifetime in BDP than in BHP. By a careful kinetic analysis of the Cl-2 + BHP(BDP) reactions, we found that the main resistance that prevents the nascent O-2((1)Delta) from escaping off the solution into the bulk gas flow does not lie in the liquid or gas phase, but in the gas/liquid interface. Thus, the seemingly weird experimental result can be justified by postulating a higher energy barrier at the O-2((1)Delta)/BDP interface than that of the O-2((1)Delta)/BHP so as to detain the O-2((1)Delta) for a longer time in BDP. In fact, this postulation has been proved as follows: according to the physical model of Copeland and Zagidullin, the O-2((1)Delta) mass accommodation coefficient is calculated from our experimental solvation detachment yield to be similar to 4.0 x 10(-6) on the BHP surface and similar to 1.7 x 10(-6) on the BDP surface. Then, based on the thermodynamics of phase equilibrium in dilute solutions, the corresponding Gibbs energy of O-2((1)Delta) at the BHP surface is computed as similar to 2.65 x 10(4) J/mol, and the value of O-2((1)Delta) at the BDP surface is similar to 2.86 x 10(4) J/mol. This higher O-2((1)Delta)/ BDP interface energy barrier may result from both larger D2O molecular mass and stronger hydrogen bonding between D2O molecules in BDP solution. The present methodology can be further improved by using microwave-discharge production of O-2((1)Delta) so as to make direct measurements of its quenching probability. Hence, more key thermodynamic and kinetic information about the O-2/aqueous electrolyte solution interfaces will be made available. Work along this line is now under way.
关键词[WOS]: OXYGEN-IODINE LASERS ;  SINGLET OXYGEN ;  GENERATOR ;  WATER ;  H2O2 ;  ACCOMMODATION ;  SOLVATION ;  MOLECULES ;  DYNAMICS
语种: 英语
WOS记录号: WOS:000256920000044
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/140764
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Dalian Inst Chem Phys, Chinese Acad Sci, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China

Recommended Citation:
Shi, Wenbo,Deng, Liezheng,Du, Shuyan,et al. O-2((1)Delta) quenching mechanism in Cl-2/basic hydrogen peroxide(basic deuterium peroxide) gas/liquid reaction and the determination of O-2((1)Delta)/BHP(BDP) interface free energy[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2008,112(25):9412-9417.
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