When the Surface Matters: Prebiotic Peptide-Bond Formation on the TiO2 (101) Anatase Surface through Periodic DFT-D2 Simulations

Chemistry : a European Journal
Stefano PantaleoneAlbert Rimola

Abstract

The mechanism of the peptide-bond formation between two glycine (Gly) molecules has been investigated by means of PBE-D2* and PBE0-D2* periodic simulations on the TiO2 (101) anatase surface. This is a process of great relevance both in fundamental prebiotic chemistry, as the reaction univocally belongs to one of the different organizational events that ultimately led to the emergence of life on Earth, as well as from an industrial perspective, since formation of amides is a key reaction for pharmaceutical companies. The efficiency of the surface catalytic sites is demonstrated by comparing the reactions in the gas phase and on the surface. At variance with the uncatalyzed gas-phase reaction, which involves a concerted nucleophilic attack and dehydration step, on the surface these two steps occur along a stepwise mechanism. The presence of surface Lewis and Brönsted sites exerts some catalytic effect by lowering the free energy barrier for the peptide-bond formation by about 6 kcal mol-1 compared to the gas-phase reaction. Moreover, the co-presence of molecules acting as proton-transfer assistants (i.e., H2 O and Gly) provide a more significant kinetic energy barrier decrease. The reaction on the surface is also favorable from a...Continue Reading

References

May 2, 1996·Nature·J P FerrisL E Orgel
Apr 16, 1998·Proceedings of the National Academy of Sciences of the United States of America·J V Smith
Jun 5, 1998·Origins of Life and Evolution of the Biosphere : the Journal of the International Society for the Study of the Origin of Life·L E Orgel
Oct 15, 1996·Physical Review. B, Condensed Matter·G Kresse, J Furthmüller
Jan 1, 1993·Physical Review. B, Condensed Matter·G Kresse, J Hafner
Oct 28, 1996·Physical Review Letters·J P PerdewM Ernzerhof
Nov 26, 1999·Origins of Life and Evolution of the Biosphere : the Journal of the International Society for the Study of the Origin of Life·J Bujdák, B M Rode
Nov 1, 2000·Proceedings of the National Academy of Sciences of the United States of America·L E Orgel
Jan 1, 1990·Annual Review of Earth and Planetary Sciences·J OróA Lazcano
Oct 16, 2001·Origins of Life and Evolution of the Biosphere : the Journal of the International Society for the Study of the Origin of Life·J W Delano
Mar 29, 2002·Nature·Max P BernsteinLouis J Allamandola
Mar 29, 2002·Nature·G M Muñoz CaroJ M Greenberg
May 16, 2002·Journal of Inorganic Biochemistry·J Bujdák, B M Rode
Jun 10, 2003·Chembiochem : a European Journal of Chemical Biology·Raffaele SaladinoErnesto Di Mauro
Dec 14, 2005·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Albert RimolaPiero Ugliengo
Jan 21, 2006·Proceedings of the National Academy of Sciences of the United States of America·S D Senanayake, H Idriss
Sep 7, 2006·Journal of Computational Chemistry·Stefan Grimme
Sep 30, 2006·Philosophical Transactions of the Royal Society of London. Series B, Biological Sciences·Charles S Cockell
Jan 24, 2007·Journal of Computational Chemistry·Edward SanvilleGraeme Henkelman
Jun 8, 2007·Journal of the American Chemical Society·Albert RimolaPiero Ugliengo
Jan 5, 2008·Origins of Life and Evolution of the Biosphere : the Journal of the International Society for the Study of the Origin of Life·Michel NuevoLouis d'Hendecourt
Jan 15, 2008·The Journal of Chemical Physics·Johannes Kästner, Paul Sherwood
Feb 8, 2008·Journal of the American Chemical Society·Eduard SchreinerDominik Marx
Mar 18, 2008·Origins of Life and Evolution of the Biosphere : the Journal of the International Society for the Study of the Origin of Life·Jean-François Lambert
Apr 10, 2008·The Journal of Chemical Physics·Daniel SheppardGraeme Henkelman
Sep 30, 2008·Nature Reviews. Microbiology·William MartinMichael J Russell
Apr 27, 2010·Physical Chemistry Chemical Physics : PCCP·Bartolomeo CivalleriClaudio M Zicovich-Wilson
Feb 18, 2011·Journal of Computational Chemistry·Daniel Sheppard, Graeme Henkelman
Mar 3, 2011·The Journal of Chemical Physics·C RomanzinH Linnartz
Jun 24, 2011·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Oranit PhuakkongJumras Limtrakul
Jul 6, 2011·Physical Chemistry Chemical Physics : PCCP·Yasuhiro ObaValerio Pirronello
Feb 25, 2009·Journal of Physics. Condensed Matter : an Institute of Physics Journal·W TangG Henkelman
Dec 24, 2011·Nature·Vijaya R Pattabiraman, Jeffrey W Bode
Dec 27, 2011·Proceedings of the National Academy of Sciences of the United States of America·Dorian S N ParkerA G G M Tielens
Mar 1, 2012·The Journal of Chemical Physics·Daniel SheppardGraeme Henkelman
Jun 30, 2012·Chemical Society Reviews·H James CleavesRobert Hazen

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Citations

Feb 23, 2019·Physical Chemistry Chemical Physics : PCCP·Giovanni BarcaroSusanna Monti
Apr 9, 2020·Physical Chemistry Chemical Physics : PCCP·Stefano PantaleonePiero Ugliengo
May 7, 2020·Pharmaceutics·Anna Helena MazurekDariusz Maciej Pisklak
Mar 27, 2021·Angewandte Chemie·Tomislav StolarJosé G Hernández

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