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Enthalpy and entropy of formation of the hydrated electron. [pulse radiolysis]

Journal Article · · Journal of Physical Chemistry; (United States)
DOI:https://doi.org/10.1021/j100170a058· OSTI ID:7017111
 [1]
  1. Brookhaven National Lab., Upton, NY (United States)

Pulse radiolysis was used to study the equilibrium of the reaction e{sub aq}{sup {minus}} + NH{sub 4}{sup +} {r equilibrium} H{sm bullet} + NH{sub 3} in aqueous solution between 4 and 87 C. The rate of equilibrium was much larger than the subsequent radical decay. The equilibrium constant (corrected to zero ionic strength) is 2.2 at 25 C, {Delta}H{degree} is {minus}2.0 kcal/mol, and {Delta}S{degree} is {minus}5.1 cal/(deg mol). When combined with thermodynamic data for NH{sub 4}{sup +}{sub aq}, NH{sub 3,aq}, and H{sm bullet}{sub aq}, these values give {Delta}G{degree}{sub f}(e{sub aq}{sup {minus}}) = 66.2 kcal/mol, {Delta}H{degree}{sub f}(e{sub aq}{sup {minus}}) = 66.3 kcal/mol, and S{degree}(e{sub aq}{sup {minus}}) = 16 cal/(deg mol). The enthalpy is 1-3.7 kcal/mol than recently published values based on kinetic studies. The forward and reverse rate constants of the reaction with ammonium ion are 1.0 {times} 10{sup 6} and 0.67 {times} 10{sup 6} M{sup {minus}1} s{sup {minus}1} at 0.05 M ionic strength and 25 C. The activation energy of the forward reaction is 7.2 kcal/mol.

DOE Contract Number:
AC02-76CH00016
OSTI ID:
7017111
Journal Information:
Journal of Physical Chemistry; (United States), Journal Name: Journal of Physical Chemistry; (United States) Vol. 95:17; ISSN 0022-3654; ISSN JPCHA
Country of Publication:
United States
Language:
English

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