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
文献类型：期刊论文
| 作者 | Shi, Wenbo; Deng, Liezheng; Du, Shuyan; Cui, Rongrong; Yang, Heping; Sha, Guohe; Zhang, Cunhao |
| 刊名 | journal of physical chemistry c
 |
| 出版日期 | 2008-06-26 |
| 卷号 | 112期号:25页码:9412-9417 |
| 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. |
| 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 |
| 关键词[WOS] | oxygen-iodine lasers ; singlet oxygen ; generator ; water ; h2o2 ; accommodation ; solvation ; molecules ; dynamics |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000256920000044 |
| 公开日期 | 2015-11-17 |
| 源URL | [http://159.226.238.44/handle/321008/140764]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 作者单位 | Dalian Inst Chem Phys, Chinese Acad Sci, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China |
| 推荐引用方式 GB/T 7714 | 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. |
| APA | Shi, Wenbo.,Deng, Liezheng.,Du, Shuyan.,Cui, Rongrong.,Yang, Heping.,...&Zhang, Cunhao.(2008).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.journal of physical chemistry c,112(25),9412-9417. |
| MLA | Shi, Wenbo,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".journal of physical chemistry c 112.25(2008):9412-9417. |
入库方式： OAI收割
来源：大连化学物理研究所
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