This remark has a bearing on current efforts to develop theoretical-only methods that
can yield predictions with the accuracy required for direct use in synthetic chemistry:
even if the kinetic parameters of Fig. 11 were calculated with, let us say, 0.1 kcal/mol
accuracy, it would still be necessary to figure out and calculate also all the possible
interaction mechanisms down to that interaction energy level. Since those accurate
and complex calculations are not yet available, more accessible alternatives are
being sought in the meantime, like the combined DFT-microkinetic methodology
that we have discussed here.
References
1. Besora M, Maseras F (2018) WIREs Comput Mol Sci 8:e1372
2. Mhadeshwar AB, Vlachos DG (2005) J Catal 234:48
3. Prieto C, González Delgado JA, Arteaga JF, Jaraíz M, López-Pérez JL, Barrero AF (2015) Org
Biomol Chem 13:3462
4. Gokhale AA, Dumesic JA, Mavrikakis M (2008) J Am Chem Soc 130:1402
5. Rush LA, Pringle PG, Harvey JN (2014) Angew Chem Int Ed 53:8672
6. Szlapa EN, Harvey JN (2018) Chem A Eur J 24:17096
7. Pérez-Soto R, Besora M, Maseras F (2020) Org Lett. https://doi.org/10.1021/acs.orglett.
0c00367
8. Darù A, Hu X, Harvey JN (2020) ACS Omega 5:1586
9. Brezny AC, Landis CR (2019) ACS Catal 9:2501
10. Robertson C, Habershon S (2019) Catal Sci Tech 9:6357
11. Blackmond DG (2005) Angew Chem Int Ed 44:4302
12. Blackmond DG (2015) J Am Chem Soc 137:10852
13. Cramer CJ (2004) Essentials of computational chemistry. Wiley, Chichester
14. Jaraíz M, Enríquez L, Pinacho R, Rubio JE, Lesarri A, López-Perez JL (2017) J Org Chem
82:3760
15. COPASI v 4.24 available free of charge from http://copasi.org
16. Weires NA, Caspi DD, Garg NK (2017) ACS Catal 7:4381
17. Crabtree RH (2015) Chem Rev 115:127
18. Zhang L, Yang H, Jiao L (2016) J Am Chem Soc 138:7151
19. Yu Y, Zhu Y, Bhagat MN, Raghuraman A, Hirsekorn KF, Notestein JM, Nguyen ST, Broadbelt
LJ (2018) ACS Catal 8:11119
20. Jaraíz M, Rubio JE, Enríquez L, Pinacho R, López-Perez JL, Lesarri A (2019) ACS Catal
9:4804
DFT-Based Microkinetic Simulations: A Bridge Between Experiment and Theory in. . .
105
can yield predictions with the accuracy required for direct use in synthetic chemistry:
even if the kinetic parameters of Fig. 11 were calculated with, let us say, 0.1 kcal/mol
accuracy, it would still be necessary to figure out and calculate also all the possible
interaction mechanisms down to that interaction energy level. Since those accurate
and complex calculations are not yet available, more accessible alternatives are
being sought in the meantime, like the combined DFT-microkinetic methodology
that we have discussed here.
References
1. Besora M, Maseras F (2018) WIREs Comput Mol Sci 8:e1372
2. Mhadeshwar AB, Vlachos DG (2005) J Catal 234:48
3. Prieto C, González Delgado JA, Arteaga JF, Jaraíz M, López-Pérez JL, Barrero AF (2015) Org
Biomol Chem 13:3462
4. Gokhale AA, Dumesic JA, Mavrikakis M (2008) J Am Chem Soc 130:1402
5. Rush LA, Pringle PG, Harvey JN (2014) Angew Chem Int Ed 53:8672
6. Szlapa EN, Harvey JN (2018) Chem A Eur J 24:17096
7. Pérez-Soto R, Besora M, Maseras F (2020) Org Lett. https://doi.org/10.1021/acs.orglett.
0c00367
8. Darù A, Hu X, Harvey JN (2020) ACS Omega 5:1586
9. Brezny AC, Landis CR (2019) ACS Catal 9:2501
10. Robertson C, Habershon S (2019) Catal Sci Tech 9:6357
11. Blackmond DG (2005) Angew Chem Int Ed 44:4302
12. Blackmond DG (2015) J Am Chem Soc 137:10852
13. Cramer CJ (2004) Essentials of computational chemistry. Wiley, Chichester
14. Jaraíz M, Enríquez L, Pinacho R, Rubio JE, Lesarri A, López-Perez JL (2017) J Org Chem
82:3760
15. COPASI v 4.24 available free of charge from http://copasi.org
16. Weires NA, Caspi DD, Garg NK (2017) ACS Catal 7:4381
17. Crabtree RH (2015) Chem Rev 115:127
18. Zhang L, Yang H, Jiao L (2016) J Am Chem Soc 138:7151
19. Yu Y, Zhu Y, Bhagat MN, Raghuraman A, Hirsekorn KF, Notestein JM, Nguyen ST, Broadbelt
LJ (2018) ACS Catal 8:11119
20. Jaraíz M, Rubio JE, Enríquez L, Pinacho R, López-Perez JL, Lesarri A (2019) ACS Catal
9:4804
DFT-Based Microkinetic Simulations: A Bridge Between Experiment and Theory in. . .
105