CCL: Activation Energy



Dear Vimal,

The rate constant and the activation energy or free energy of activation are related by the Arrhenius equation and the Eyring equation, respectively.  These are easily found in any physical chemistry textbook / Wikipedia.

From there, it is much less trivial.  To know how fast a reaction really is, one must know the rate law and concentrations of the species in the rate law.  Computational chemists rarely have the ability to apply true experimental conditions to our simulations.  Furthermore, a computed activation barrier may easily have an error of ±0.05 eV or more.  This will lead to an error in the absolute rate constant approaching a full order of magnitude.  For this reason, the ratio of rate constants (the relative rates) are more typically discussed, since it is hoped the errors cancel in the division.  

However, it is certainly possible to put numbers into context.  Consider the simplest case of a unimolecular rate law and k determined from the Eyring equation at 298 K.  A barrier of ~0.4 eV gives a rate constant on the order of 1E5 1/sec.  That’s fast.  Very fast.  A barrier of ~1 eV gives a rate constant on the order of 1E-5 1/sec.  That’s not nearly as slow as it might seem.  A barrier of ~1.5 eV gives a rate constant on the order of 1E-14 1/sec.  That’s very slow.

Now consider the half-lives of those three examples, which provides the same information > from a different perspective:  ~1E-6 sec, ~1E4 sec, ~1E13 sec.  The first is still obviously very, very fast.  This is similar to the barrier to the chair flip in cyclohexane, which requires cryogenic temperatures to inhibit.  It is now a bit more clear that the 1 eV barrier has a half life that is still perfectly reasonable if one is willing to wait a few days for the reaction to complete.  The 1.5 eV barrier, though…  A half life of about 1 million years is no one’s idea of “fast” except on a geologic or cosmic timescale (all things are relative!).

In summary, it is trivial to compute a unimolecular rate constant from an activation barrier.  After that, use the specifics of your system to decide what is “fast” and what isn’t.

Cheers,
Eric


----------------------------------------------------
Eric V. Patterson, PhD
Director of Undergraduate Laboratories
Senior Lecturer

Stony Brook University
Department of Chemistry
3400 SUNY
Stony  Brook, NY 11794-3400

465 Chemistry
eric.patterson*o*stonybrook.edu

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On Mar 8, 2019, at 2:35 PM, Jeya Vimalan jeyavimalan2k#gmail.com <owner-chemistry*o*ccl.net> wrote:

Dear All,

I have the following question.

What is the range of activation energy that can happen at room temperature.
For example, in one paper i see 0.4 eV and in some cases 1+ eV.
Sometimes more than 1.5 eV  when plane wave basis sets are used.
Are there any papers that correlates activation energy to temperature. 
If anyone has a script/methodology, can you please share it with me.

Thanks in advance.
Vimal