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Paschal Ejims

Does MOPAC allows calculation of Standard Enthalpy of reaction in this way?

Dennis Ainsworth  Follow

The free energy change of a reaction occurring in solution can be computed using a thermodynamic cycle:$$\Delta G^\circ_{r,soln} = \Delta G^\circ_{r,gas} + \Delta\Delta G^\circ_{r,solv} $$$\Delta G^\circ_{r,soln}$ can also be written as$$\Delta G^\circ_{r,soln} = G^\circ_{soln}(B)- G^\circ_{soln}(A)$$where $$G^\circ_{soln}(X) = G^\circ_{gas}(X) + \Delta G^\circ_{solv} $$and $$G^\circ_{gas}(X) = E_{gas}(X) + G^\circ_{gas,RRHO}(X)$$The solvation energy is usually computed using a continuum as the difference in electronic energy with and without the continuum. $\Delta G^\circ_{solv}(X) = E^\prime_{soln}(X)-E^\prime_{gas}(X)$The parameters in the continuum model are usually optimized for a particular level of theory, which may not be appropriate for the computation of $\Delta G^\circ_{r,gas}$, so $E_{gas}(X)$ is not necessarily the same as $E^\prime_{gas}(X)$

However, if $E_{gas}(X) = E^\prime_{gas}(X)$ then $$G^\circ_{soln}(X) = E_{soln}(X) + G^\circ_{gas,RRHO}(X) $$

The parameters in the continuum model are usually determined using the gas phase geometry $(X)$. But if $E_{gas}(X) = E^\prime_{gas}(X)$ then many people often choose to use the geometry optimized in solution$G^\circ_{soln}(X_{soln}) = E_{soln}(X_{soln}) + G^\circ_{soln,RRHO}(X_{soln})$.

For semiempirical calculations, the electronic energy corresponds to the enthalpy of formation at 298K, so if one simply makes the substitution$$E(X) \rightarrow \Delta H^\circ_{f,298}(X)$$then (at 298K)$$G^\circ_{soln}(X) = \Delta H^\circ_{f,298}(X) -TS^\circ_{gas,RRHO}(X)$$ $G^\circ_{soln}(X)$ doesn't correspond to a measurable free energy because $S^\circ_{gas,RRHO} \ne S^\circ_{f}$ but it can still be used to compute $\Delta G^\circ_{r,soln}$ since the missing terms cancel.

For temperatures other than 298K$$G^\circ_{soln}(X) = \Delta H^\circ_{f,298}(X) + (H^\circ_{gas,RRHO}(X,T)-H^\circ_{gas,RRHO}(X,T=298K)) -TS^\circ_{gas,RRHO}(X)$$

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Ebhohon Victory  Follow
Yes. Yes, it is. Youre welcomeMore
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James Beamesderfer  Follow
the cycle is needed because the continuum model has parameters that need to be fitted to measured values. You cant measure $G^\circ_{soln}(X)$, but you can measure $\Delta G^\circ_{solv}(X)$. So you need the cycle to relate $\Delta G^\circ_{solv}(X)$. to $G^\circ_{soln}(X)$More
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James Conlon  Follow
I dont understand why the gas-solution cycle is needed, although I understand the procedure you wrote. But if mopac give us "$G_f$ "for each reactant in solution, why dont we direcly sum those values?(with corresponding index for reactant and products) –More
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Josep Cobos  Follow
damn..thats complicated. Thanks for the help..More
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