Water Dissociative Adsorption on α-Al2O3(112̅0) Is Controlled by Surface Site Undercoordination, Density, and Topology
- Sophia HeidenSophia HeidenUniversity of Potsdam, Institute of Chemistry, Karl-Liebknecht-Strasse 24-25, Potsdam 14476, GermanyMore by Sophia Heiden
- ,
- Yanhua YueYanhua YueFritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, GermanyMore by Yanhua Yue
- ,
- Harald KirschHarald KirschFritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, GermanyMore by Harald Kirsch
- ,
- Jonas WirthJonas WirthUniversity of Potsdam, Institute of Chemistry, Karl-Liebknecht-Strasse 24-25, Potsdam 14476, GermanyMore by Jonas Wirth
- ,
- Peter SaalfrankPeter SaalfrankUniversity of Potsdam, Institute of Chemistry, Karl-Liebknecht-Strasse 24-25, Potsdam 14476, GermanyMore by Peter Saalfrank
- , and
- R. Kramer Campen*R. Kramer Campen*Phone: [+4930] 8413-5230. Fax: [+4930] 8413-5106. E-mail: [email protected]Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, GermanyMore by R. Kramer Campen
Abstract
α-Al2O3 surfaces are common in a wide variety of applications and useful models of more complicated, environmentally abundant, alumino-silicate surfaces. While decades of work have clarified that all properties of these surfaces depend sensitively on the crystal face and the presence of even small amounts of water, quantitative insight into this dependence has proven challenging. Overcoming this challenge requires systematic study of the mechanism by which water interacts with various α-Al2O3 surfaces. Such insight is most easily gained for the interaction of small amounts of water with surfaces in ultra high vacuum. In this study, we continue our combined theoretical and experimental approach to this problem, previously applied to water interaction with the α-Al2O3 (0001) and (11̅02) surfaces, now to water interaction with the third most stable surface, that is, the (112̅0). Because we characterize all three surfaces using similar tools, it is straightforward to conclude that the (112̅0) is most reactive with water. The most important factor explaining its increased reactivity is that the high density of undercoordinated surface Al atoms on the (112̅0) surface allows the bidentate adsorption of OH fragments originating from dissociatively adsorbed water, while only monodentate adsorption is possible on the (0001) and (11̅02) surfaces: the reactivity of α-Al2O3 surfaces with water depends strongly, and nonlinearly, on the density of undercoordinated surface Al atoms.
Cited By
This article is cited by 16 publications.
- Yanhua Yue, Giacomo Melani, Harald Kirsch, Alexander Paarmann, Peter Saalfrank, R. Kramer Campen, Yujin Tong. Structure and Reactivity of α-Al2O3(0001) Surfaces: How Do Al–I and Gibbsite-like Terminations Interconvert?. The Journal of Physical Chemistry C 2022, 126 (31) , 13467-13476. https://doi.org/10.1021/acs.jpcc.2c03743
- Niko Prasetyo, Ahya Aulia Oktarini, Mokhammad Fajar Pradipta. Fate of Water Molecules on (11-20) and (1-102) α-Alumina Surfaces: 2D Periodic Self-Consistent Charge-Density Functional Tight-Binding/Molecular Mechanics Molecular Dynamics Study. The Journal of Physical Chemistry C 2022, 126 (27) , 11148-11157. https://doi.org/10.1021/acs.jpcc.2c01415
- Shalini Halan Joghee, Kamachi Mudali Uthandi, Nimmi Singh, Sanjeev Katti, Peeyush Kumar, Ravi Kottan Renganayagalu, Biji Pullithadathil. Evolution of Temperature-Driven Interfacial Wettability and Surface Energy Properties on Hierarchically Structured Porous Superhydrophobic Pseudoboehmite Thin Films. Langmuir 2020, 36 (23) , 6352-6364. https://doi.org/10.1021/acs.langmuir.0c00368
- Sophia Heiden, Denis Usvyat, Peter Saalfrank. Theoretical Surface Science Beyond Gradient-Corrected Density Functional Theory: Water at α-Al2O3(0001) as a Case Study. The Journal of Physical Chemistry C 2019, 123 (11) , 6675-6684. https://doi.org/10.1021/acs.jpcc.9b00407
- Sophia Heiden, Jonas Wirth, R. Kramer Campen, Peter Saalfrank. Water Molecular Beam Scattering at α-Al2O3(0001): An Ab Initio Molecular Dynamics Study. The Journal of Physical Chemistry C 2018, 122 (27) , 15494-15504. https://doi.org/10.1021/acs.jpcc.8b04179
- Arvin Kakekhani, Luke T. Roling, Ambarish Kulkarni, Allegra A. Latimer, Hadi Abroshan, Julia Schumann, Hassan AlJama, Samira Siahrostami, Sohrab Ismail-Beigi, Frank Abild-Pedersen, Jens K. Nørskov. Nature of Lone-Pair–Surface Bonds and Their Scaling Relations. Inorganic Chemistry 2018, 57 (12) , 7222-7238. https://doi.org/10.1021/acs.inorgchem.8b00902
- Giacomo Melani. Vibrational dynamics and energy transfer at aqueous oxide interfaces: Insights from theory and simulations. 2024, 18-29. https://doi.org/10.1016/B978-0-323-85669-0.00026-X
- Verena Pramhaas, Günther Rupprechter. Sum Frequency Generation (SFG) Spectroscopy. 2023, 213-233. https://doi.org/10.1007/978-3-031-07125-6_10
- Jiachen Chen, Dmitry Sharapa, Philipp N. Plessow. Stability and formation of hydroxylated α − Al 2 O 3 ( 0001 ) surfaces at high temperatures. Physical Review Research 2022, 4 (1) https://doi.org/10.1103/PhysRevResearch.4.013232
- . Hydration-driven stabilization and volume collapse of grain boundaries in Mg2SiO4 forsterite predicted by first-principles simulations. American Mineralogist 2021https://doi.org/10.2138/am-2021-7732
- Walber Gonçalves Guimarães, Guilherme Ferreira de Lima, Hélio Anderson Duarte. Comparative DFT study of the oxy(hydr)oxides of iron and aluminum – structural, electronic and surface properties.. Surface Science 2021, 708 , 121821. https://doi.org/10.1016/j.susc.2021.121821
- Giacomo Melani, Yuki Nagata, Peter Saalfrank. Vibrational energy relaxation of interfacial OH on a water-covered α-Al 2 O 3 (0001) surface: a non-equilibrium ab initio molecular dynamics study. Physical Chemistry Chemical Physics 2021, 23 (13) , 7714-7723. https://doi.org/10.1039/D0CP03777J
- Chengyu He, Tie Liu, Lei Tian, Yubao Xiao, Shang Yuan, Qiang Wang. Effect of crystal orientation on droplet wetting behavior on single-crystal Al2O3 substrates: An experimental study. Physics of Fluids 2020, 32 (12) https://doi.org/10.1063/5.0030285
- Giacomo Melani, Yuki Nagata, R. Kramer Campen, Peter Saalfrank. Vibrational spectra of dissociatively adsorbed D2O on Al-terminated α-Al2O3(0001) surfaces from ab initio molecular dynamics. The Journal of Chemical Physics 2019, 150 (24) https://doi.org/10.1063/1.5099895
- Hui Zhao, Na Qi, Ying Li. Interaction between polysaccharide monomer and SiO2/Al2O3/CaCO3 surfaces: A DFT theoretical study. Applied Surface Science 2019, 466 , 607-614. https://doi.org/10.1016/j.apsusc.2018.10.085
- Giacomo Melani, Yuki Nagata, Jonas Wirth, Peter Saalfrank. Vibrational spectroscopy of hydroxylated α-Al2O3(0001) surfaces with and without water: An ab initio molecular dynamics study. The Journal of Chemical Physics 2018, 149 (1) https://doi.org/10.1063/1.5023347