OXYGEN-ATOM EXCHANGE IN AQUEOUS-SOLUTION BY O-+H2O-]OH-+OH AND OH+H2O-]H2O+OH - A STUDY OF HYDROGEN-ATOM TRANSFER

被引：10
|
作者：
KLANING, UK [1 ]
LARSEN, E [1 ]
SEHESTED, K [1 ]
机构：
[1] RISO NATL LAB,DK-4000 ROSKILDE,DENMARK
来源：
JOURNAL OF PHYSICAL CHEMISTRY | 1994年 / 98卷 / 36期
关键词：
D O I：
10.1021/j100087a022
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
The title reactions were studied by measuring the oxygen isotope composition of H2O2 and O-2 produced by electron pulse irradiation and gamma-irradiation of solutions of N2O and BrO4- in water enriched with (H2O)-O-18. The fraction, xi, of the reaction O- + H2O --> OH- + OH that takes place by hydrogen atom transfer is found to be 0.22 +/- 0.02 at 22 degrees C and increases with temperature. The difference between the enthalpies of activation for hydrogen atom transfer and proton transfer is estimated to be 16 +/- 2 kJ mol(-1) and the corresponding entropy of activation at 22 degrees C to be 44 +/- 8 J K-1 mol(-1). A molecular model is sketched according to which 10-100 reversible proton transfers take place for each hydrogen atom transferred. Assuming no interference from impurities, the rate constant for the exchange reaction *OH + H2O --> H-2*O + OH is found to be 57 +/- 6 s(-1) at 30 degrees C.
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收藏
页码：8946 / 8951
页数：6
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