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Öğe "pop-On and Pop-Off" Surface Chemistry of Alanine on Ni{111} under Elevated Hydrogen Pressures(American Chemical Society, 2018) Nicklin R.E.J.; Shavorskiy A.; Aksoy Akgul F.; Liu Z.; Bennett R.A.; Sacchi M.; Held G.The coadsorption of hydrogen with a simple chiral modifier, alanine, on Ni{111} was studied using density functional theory in combination with ambient-pressure X-ray photoelectron spectroscopy and X-ray absorption spectroscopy at temperatures of 300 K and above, which are representative of chiral hydrogenation reactions. Depending on the hydrogen pressure, the surface enables protons to "pop-on and -off" the modifier molecules, thus significantly altering the adsorption geometry and chemical nature of alanine from anionic tridentate in ultrahigh vacuum to predominantly zwitterionic bidentate at hydrogen pressures above 0.1 Torr. This hydrogen-stabilized modifier geometry allows alternative mechanisms for proton transfer and the creation of enatioselective reaction environments. © 2018 American Chemical Society.
