Mechanism of the Accelerated Water Formation Reaction under Interfacial Confinement

Wang, Mengen; Zhou, Chen; Akter, Nusnin; Tysoe, Wilfred T.; Boscoboinik, J. Anibal; Lu, Deyu

doi:10.1021/acscatal.9b05289

Title: Mechanism of the Accelerated Water Formation Reaction under Interfacial Confinement

Journal Article · Thu Apr 23 00:00:00 EDT 2020 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.9b05289· OSTI ID:1616436

^[1]; Zhou, Chen ^[1]; Akter, Nusnin ^[1];

^[2];

^[3];

^[3]

Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Stony Brook Univ., NY (United States)
Univ. of Wisconsin, Milwaukee, WI (United States). Lab. for Surface Studies
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Subnanoscale spaces at the interface between weakly coupled thin films and their metal supports offer exciting opportunities for studying chemical reactions under confinement. Here, we investigated the kinetics of water formation (from hydrogen and chemisorbed oxygen) in the confined space at the interface between bilayer (BL) silica and a Ru(0001) support, compared to the reaction on the bare Ru(0001) surface. Ambient pressure X-ray photoelectron spectroscopy (AP-XPS) experiments were carried out at different temperatures at elevated pressures of H₂ to follow the reaction kinetics. The apparent activation energy at the BL-silica/Ru(0001) interface was found to be 0.38 eV lower than that on bare Ru(0001), consistent with a recent report by Prieto et al. (Angew. Chem., Int. Ed.2018, 57(28), 8749–8753) carried out at lower H₂ pressures using low-energy electron microscopy. Density functional theory calculations revealed that the rate-limiting step in the direct hydrogenation pathway on the Ru(0001) surface is the first hydrogen addition step (*H + *O ↔ *OH). The confinement at the BL-silica/Ru(0001) interface only marginally affects the energy barrier of the first hydrogen addition. Instead, it activates an alternative disproportionation reaction pathway (*H₂O + *O ↔ 2*OH). On the bare Ru(0001) surface, the disproportionation pathway can only occur at cryogenic temperatures or under high water vapor pressures. However, the presence of the BL-silica increases the desorption barrier for water molecules at the interface. The increased residence time allows trapped water molecules to react with chemisorbed oxygen to produce two *OH per H₂O with an activation energy 0.25 eV lower than that of the first hydrogen addition step. Finally, this work reveals the origin of the observed accelerated water formation reaction at the BL-silica/Ru(0001) interface in the low-temperature regime (T < 350 K) and points to a route to engineer chemical reaction pathways by leveraging subnanoscale confined spaces at metal–oxide interfaces.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1616436

Alternate ID(s):: OSTI ID: 1618404

Report Number(s):: BNL-215883-2020-JAAM; BNL-215917-2020-JAAM

Journal Information:: ACS Catalysis, Vol. 10, Issue 11; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 18 works

Citation information provided by
Web of Science

References (67)

Fundamental Studies of Nanofluidics: Nanopores, Nanochannels, and Nanopipets Haywood, Daniel G.; Saha-Shah, Anumita; Baker, Lane A. Analytical Chemistry, Vol. 87, Issue 1 https://doi.org/10.1021/ac504180h	journal	December 2014
Nanoscopic Cellular Imaging: Confinement Broadens Understanding Lee, Stephen A.; Ponjavic, Aleks; Siv, Chanrith ACS Nano, Vol. 10, Issue 9 https://doi.org/10.1021/acsnano.6b02863	journal	September 2016
Effect of Nanoscale Confinement on the Crystallization of Potassium Ferrocyanide Anduix-Canto, Clara; Kim, Yi-Yeoun; Wang, Yun-Wei Crystal Growth & Design, Vol. 16, Issue 9 https://doi.org/10.1021/acs.cgd.6b00894	journal	August 2016
Alignment of Organic Crystals under Nanoscale Confinement Ha, Jeong-Myeong; Hamilton, Benjamin D.; Hillmyer, Marc A. Crystal Growth & Design, Vol. 12, Issue 9 https://doi.org/10.1021/cg3006635	journal	August 2012
Simulation of Intermediate Channeling by Nanoscale Confinement Chavan, Kanchan Suklal; Calabrese Barton, Scott The Journal of Physical Chemistry C, Vol. 122, Issue 26 https://doi.org/10.1021/acs.jpcc.8b01922	journal	May 2018
Effects of Zeolite Structural Confinement on Adsorption Thermodynamics and Reaction Kinetics for Monomolecular Cracking and Dehydrogenation of n -Butane Janda, Amber; Vlaisavljevich, Bess; Lin, Li-Chiang Journal of the American Chemical Society, Vol. 138, Issue 14 https://doi.org/10.1021/jacs.5b11355	journal	March 2016
The Effect of Nano Confinement on the C–H Activation and its Corresponding Structure-Activity Relationship Shao, Jing; Yuan, Linghua; Hu, Xingbang Scientific Reports, Vol. 4, Issue 1 https://doi.org/10.1038/srep07225	journal	November 2014
The Effects of Confinement inside Carbon Nanotubes on Catalysis Pan, Xiulian; Bao, Xinhe Accounts of Chemical Research, Vol. 44, Issue 8 https://doi.org/10.1021/ar100160t	journal	August 2011
The catalytic diversity of zeolites: confinement and solvation effects within voids of molecular dimensions Gounder, Rajamani; Iglesia, Enrique Chemical Communications, Vol. 49, Issue 34 https://doi.org/10.1039/c3cc40731d	journal	January 2013
The confined space inside carbon nanotubes can dictate the stereo- and regioselectivity of Diels–Alder reactions Smith, Nicole M.; Swaminathan Iyer, K.; Corry, Ben Physical Chemistry Chemical Physics, Vol. 16, Issue 15 https://doi.org/10.1039/c3cp54295e	journal	January 2014
Confined catalysis under two-dimensional materials Li, Haobo; Xiao, Jianping; Fu, Qiang Proceedings of the National Academy of Sciences, Vol. 114, Issue 23 https://doi.org/10.1073/pnas.1701280114	journal	May 2017
Surface chemistry and catalysis confined under two-dimensional materials Fu, Qiang; Bao, Xinhe Chemical Society Reviews, Vol. 46, Issue 7 https://doi.org/10.1039/C6CS00424E	journal	January 2017
Hexagonal Boron Nitride Cover on Pt(111): A New Route to Tune Molecule–Metal Interaction and Metal-Catalyzed Reactions Zhang, Yanhong; Weng, Xuefei; Li, Huan Nano Letters, Vol. 15, Issue 5 https://doi.org/10.1021/acs.nanolett.5b01205	journal	April 2015
Graphene cover-promoted metal-catalyzed reactions Yao, Yunxi; Fu, Qiang; Zhang, Y. Y. Proceedings of the National Academy of Sciences, Vol. 111, Issue 48 https://doi.org/10.1073/pnas.1416368111	journal	November 2014
Enhancing the Hydrogen Activation Reactivity of Nonprecious Metal Substrates via Confined Catalysis Underneath Graphene Zhou, Yinong; Chen, Wei; Cui, Ping Nano Letters, Vol. 16, Issue 10 https://doi.org/10.1021/acs.nanolett.6b02052	journal	September 2016
Permeation of a Single-Layer SiO ₂ Membrane and Chemistry in Confined Space Emmez, Emre; Yang, Bing; Shaikhutdinov, Shamil The Journal of Physical Chemistry C, Vol. 118, Issue 50 https://doi.org/10.1021/jp503253a	journal	June 2014
Gas Separation through Bilayer Silica, the Thinnest Possible Silica Membrane Yao, Bowen; Mandrà, Salvatore; Curry, John O. ACS Applied Materials & Interfaces, Vol. 9, Issue 49 https://doi.org/10.1021/acsami.7b13302	journal	December 2017
Growth and Characterization of Crystalline Silica Films on Pd(100) Altman, Eric I.; Götzen, Jan; Samudrala, Niveditha The Journal of Physical Chemistry C, Vol. 117, Issue 49 https://doi.org/10.1021/jp4101152	journal	November 2013
Support effects on the atomic structure of ultrathin silica films on metals Yu, Xin; Yang, Bing; Anibal Boscoboinik, Jorge Applied Physics Letters, Vol. 100, Issue 15 https://doi.org/10.1063/1.3703609	journal	April 2012
Modeling Zeolites with Metal-Supported Two-Dimensional Aluminosilicate Films Boscoboinik, Jorge Anibal; Yu, Xin; Yang, Bing Angewandte Chemie International Edition, Vol. 51, Issue 24 https://doi.org/10.1002/anie.201201319	journal	April 2012
A Large-Area Transferable Wide Band Gap 2D Silicon Dioxide Layer Büchner, Christin; Wang, Zhu-Jun; Burson, Kristen M. ACS Nano, Vol. 10, Issue 8 https://doi.org/10.1021/acsnano.6b03929	journal	July 2016
Preparation of an ordered ultra-thin aluminosilicate framework composed of hexagonal prisms forming a percolated network Boscoboinik, J. Anibal; Yu, Xin; Shaikhutdinov, Shamil Microporous and Mesoporous Materials, Vol. 189 https://doi.org/10.1016/j.micromeso.2013.10.023	journal	May 2014
Exploring Zeolite Chemistry with the Tools of Surface Science: Challenges, Opportunities, and Limitations Boscoboinik, J. Anibal; Shaikhutdinov, Shamil Catalysis Letters, Vol. 144, Issue 12 https://doi.org/10.1007/s10562-014-1369-3	journal	September 2014
The Atomic Structure of a Metal-Supported Vitreous Thin Silica Film Lichtenstein, Leonid; Büchner, Christin; Yang, Bing Angewandte Chemie International Edition, Vol. 51, Issue 2 https://doi.org/10.1002/anie.201107097	journal	November 2011
Ultrathin Silica Films: The Atomic Structure of Two-Dimensional Crystals and Glasses Büchner, Christin; Lichtenstein, Leonid; Yu, Xin Chemistry - A European Journal, Vol. 20, Issue 30 https://doi.org/10.1002/chem.201402452	journal	July 2014
Silica bilayer supported on Ru(0001): Following the crystalline to vitreous transformation in real time with spectro‐microscopy Klemm, Hagen W.; Prieto, Mauricio Javier; Xiong, Feng Angewandte Chemie International Edition https://doi.org/10.1002/anie.202002514	journal	March 2020
First-Principles Study of Interface Structures and Charge Rearrangement at the Aluminosilicate/Ru(0001) Heterojunction Wang, Mengen; Zhong, Jian-Qiang; Stacchiola, Dario J. The Journal of Physical Chemistry C, Vol. 123, Issue 13 https://doi.org/10.1021/acs.jpcc.8b05853	journal	September 2018
Energy Level Shifts at the Silica/Ru(0001) Heterojunction Driven by Surface and Interface Dipoles Wang, Mengen; Zhong, Jian-Qiang; Kestell, John Topics in Catalysis, Vol. 60, Issue 6-7 https://doi.org/10.1007/s11244-016-0704-x	journal	September 2016
CO adsorption on a silica bilayer supported on Ru(0001) Schlexer, Philomena; Pacchioni, Gianfranco; Włodarczyk, Radosław Surface Science, Vol. 648 https://doi.org/10.1016/j.susc.2015.10.027	journal	June 2016
Adsorption of Au and Pd on Ruthenium-Supported Bilayer Silica Büchner, Christin; Lichtenstein, Leonid; Stuckenholz, Stefanie The Journal of Physical Chemistry C, Vol. 118, Issue 36 https://doi.org/10.1021/jp5055342	journal	August 2014
Stabilization of Oxidized Copper Nanoclusters in Confined Spaces Akter, Nusnin; Wang, Mengen; Zhong, Jian-Qiang Topics in Catalysis, Vol. 61, Issue 5-6 https://doi.org/10.1007/s11244-017-0879-9	journal	January 2018
Immobilization of single argon atoms in nano-cages of two-dimensional zeolite model systems Zhong, Jian-Qiang; Wang, Mengen; Akter, Nusnin Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms16118	journal	July 2017
Ionization‐Facilitated Formation of 2D (Alumino)Silicate–Noble Gas Clathrate Compounds Zhong, Jian‐Qiang; Wang, Mengen; Akter, Nusnin Advanced Functional Materials, Vol. 29, Issue 20 https://doi.org/10.1002/adfm.201806583	journal	March 2019
Size Specifically High Activity of Ru Nanoparticles for Hydrogen Oxidation Reaction in Alkaline Electrolyte Ohyama, Junya; Sato, Takuma; Yamamoto, Yuta Journal of the American Chemical Society, Vol. 135, Issue 21 https://doi.org/10.1021/ja4021638	journal	May 2013
Platinum-Coated Copper Nanowires with High Activity for Hydrogen Oxidation Reaction in Base Alia, Shaun M.; Pivovar, Bryan S.; Yan, Yushan Journal of the American Chemical Society, Vol. 135, Issue 36 https://doi.org/10.1021/ja405598a	journal	August 2013
The spectroscopic observation of water formation Fisher, G. B.; Gland, J. L.; Schmieg, S. J. Journal of Vacuum Science and Technology, Vol. 20, Issue 3 https://doi.org/10.1116/1.571421	journal	March 1982
Direct characterization of the hydroxyl intermediate during reduction of oxygen on Pt(111) by time-resolved electron energy loss spectroscopy Germer, Thomas A.; Ho, W. Chemical Physics Letters, Vol. 163, Issue 4-5 https://doi.org/10.1016/0009-2614(89)85166-8	journal	November 1989
The low temperature water formation reaction on Pt(111): A static SIMS and TDS study Ogle, K. M.; White, J. M. Surface Science, Vol. 139, Issue 1 https://doi.org/10.1016/0039-6028(84)90007-4	journal	April 1984
The hydrogen-oxygen reaction over the Pt(111) surface: Transient titration of adsorbed oxygen with hydrogen Gland, J. Journal of Catalysis, Vol. 77, Issue 1 https://doi.org/10.1016/0021-9517(82)90167-1	journal	September 1982
Kinetics of the hydrogen-oxygen reaction on platinum Hellsing, B. Journal of Catalysis, Vol. 132, Issue 1 https://doi.org/10.1016/0021-9517(91)90258-6	journal	November 1991
Autocatalytic behavior and role of oxygen diffusion in the hydrogen-oxygen reaction on Pt(111) Verheij, Laurens K.; Freitag, Martin; Hugenschmidt, Markus B. Surface Science, Vol. 272, Issue 1-3 https://doi.org/10.1016/0039-6028(92)91450-P	journal	January 1992
Dual-Path Mechanism for Catalytic Oxidation of Hydrogen on Platinum Surfaces Völkening, S.; Bedürftig, K.; Jacobi, K. Physical Review Letters, Vol. 83, Issue 13 https://doi.org/10.1103/PhysRevLett.83.2672	journal	September 1999
Catalytic Water Formation on Platinum: A First-Principles Study Michaelides, A.; Hu, P. Journal of the American Chemical Society, Vol. 123, Issue 18 https://doi.org/10.1021/ja003576x	journal	May 2001
The influence of steps on the water-formation reaction on Ru(001) Koch, M. H.; Jakob, P.; Menzel, D. Surface Science, Vol. 367, Issue 3 https://doi.org/10.1016/S0039-6028(96)00811-4	journal	December 1996
Interaction of gas‐phase atomic deuterium with the Ru(001)– p (1×2)–O surface: Kinetics of hydroxyl and water formation Schick, M.; Xie, J.; Mitchell, W. J. The Journal of Chemical Physics, Vol. 104, Issue 19 https://doi.org/10.1063/1.471452	journal	May 1996
Oxidation and Reduction under Cover: Chemistry at the Confined Space between Ultrathin Nanoporous Silicates and Ru(0001) Zhong, Jian-Qiang; Kestell, John; Waluyo, Iradwikanari The Journal of Physical Chemistry C, Vol. 120, Issue 15 https://doi.org/10.1021/acs.jpcc.6b02851	journal	April 2016
Oxidation of the Ru(0001) surface covered by weakly bound, ultrathin silicate films Emmez, Emre; Anibal Boscoboinik, J.; Tenney, Samuel Surface Science, Vol. 646 https://doi.org/10.1016/j.susc.2015.06.019	journal	April 2016
Water Formation under Silica Thin Films: Real-Time Observation of a Chemical Reaction in a Physically Confined Space Prieto, Mauricio J.; Klemm, Hagen W.; Xiong, Feng Angewandte Chemie International Edition, Vol. 57, Issue 28 https://doi.org/10.1002/anie.201802000	journal	June 2018
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Chemical accuracy for the van der Waals density functional Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos Journal of Physics: Condensed Matter, Vol. 22, Issue 2 https://doi.org/10.1088/0953-8984/22/2/022201	journal	December 2009
Van der Waals density functionals applied to solids Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos Physical Review B, Vol. 83, Issue 19 https://doi.org/10.1103/PhysRevB.83.195131	journal	May 2011
Higher-accuracy van der Waals density functional Lee, Kyuho; Murray, Éamonn D.; Kong, Lingzhu Physical Review B, Vol. 82, Issue 8 https://doi.org/10.1103/PhysRevB.82.081101	journal	August 2010
A climbing image nudged elastic band method for finding saddle points and minimum energy paths Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904 https://doi.org/10.1063/1.1329672	journal	December 2000
Theoretical study of O adlayers on Ru(0001) Stampfl, C.; Scheffler, M. Physical Review B, Vol. 54, Issue 4 https://doi.org/10.1103/PhysRevB.54.2868	journal	July 1996
Adsorbate induced reconstruction by strong chemisorption: Ru(001)p(2×2)-O Lindroos, M.; Pfnür, H.; Held, G. Surface Science, Vol. 222, Issue 2-3 https://doi.org/10.1016/0039-6028(89)90371-3	journal	November 1989
Oxygen induced reconstruction of a close-packed surface: A LEED IV study on Ru(001)-p(2 × 1)O Pfnür, H.; Held, G.; Lindroos, M. Surface Science, Vol. 220, Issue 1 https://doi.org/10.1016/0039-6028(89)90462-7	journal	October 1989
Formation and Geometry of a High-Coverage Oxygen Adlayer on Ru(001), the p(2 × 2)-3O Phase Gsell, Marianne; Stichler, Markus; Jakob, Peter Israel Journal of Chemistry, Vol. 38, Issue 4 https://doi.org/10.1002/ijch.199800039	journal	January 1998
The geometries of coadsorbate layers of O and H on Ru(001): How well can quantitative LEED see hydrogen atoms? Gsell, Marianne; Menzel, Dietrich Surface Science, Vol. 603, Issue 10-12 https://doi.org/10.1016/j.susc.2008.07.045	journal	June 2009
O- and H-induced surface core level shifts on Ru(0001): prevalence of the additivity rule Lizzit, S.; Zhang, Y.; Kostov, K. L. Journal of Physics: Condensed Matter, Vol. 21, Issue 13 https://doi.org/10.1088/0953-8984/21/13/134009	journal	March 2009
High coverage adsorption and co-adsorption of CO and H ₂ on Ru(0001) from DFT and thermodynamics Zhao, Peng; He, Yurong; Cao, Dong-Bo Physical Chemistry Chemical Physics, Vol. 17, Issue 29 https://doi.org/10.1039/C5CP02486B	journal	January 2015
Trends in the Exchange Current for Hydrogen Evolution Nørskov, J. K.; Bligaard, T.; Logadottir, A. Journal of The Electrochemical Society, Vol. 152, Issue 3 https://doi.org/10.1149/1.1856988	journal	January 2005
Water-induced surface reconstruction of oxygen $(2 \times 1)$ covered Ru(0001) Maier, Sabine; Cabrera-Sanfelix, Pepa; Stass, Ingeborg Physical Review B, Vol. 82, Issue 7 https://doi.org/10.1103/PhysRevB.82.075421	journal	August 2010
Stability of water monolayers on Ru(0001): Thermal and electronically induced dissociation Faradzhev, N. S.; Kostov, K. L.; Feulner, P. Chemical Physics Letters, Vol. 415, Issue 1-3 https://doi.org/10.1016/j.cplett.2005.08.119	journal	October 2005
Catalytic test reactions for the evaluation of hierarchical zeolites Hartmann, Martin; Machoke, Albert Gonche; Schwieger, Wilhelm Chemical Society Reviews, Vol. 45, Issue 12 https://doi.org/10.1039/C5CS00935A	journal	January 2016
Modifying the adsorption characteristics of water on Ru{0001} with preadsorbed oxygen Gladys, M. J.; El-Zein, A. A.; Mikkelsen, A. Physical Review B, Vol. 78, Issue 3 https://doi.org/10.1103/PhysRevB.78.035409	journal	July 2008
Ambient pressure x-ray photoelectron spectroscopy study of water formation and adsorption under two-dimensional silica and aluminosilicate layers on Pd(111) Jhang, Jin-Hao; Boscoboinik, J. Anibal; Altman, Eric I. The Journal of Chemical Physics, Vol. 152, Issue 8 https://doi.org/10.1063/1.5142621	journal	February 2020

Similar Records

Water Formation Reaction under Interfacial Confinement: Al0.25Si0.75O2 on O-Ru(0001)

Journal Article · Thu Jan 06 00:00:00 EST 2022 · Nanomaterials · OSTI ID:1616436

Cored, Jorge; Wang, Mengen; Akter, Nusnin; +10 more

Mechanistic Insights on C-O and C-C Bond Activation and Hydrogen Insertion during Acetic Acid Hydrogenation Catalyzed by Ruthenium Clusters in Aqueous Medium

Journal Article · Tue Jun 07 00:00:00 EDT 2016 · Journal of Catalysis · OSTI ID:1616436

Shangguan, Junnan; Olarte, Mariefel V.; Chin, Ya-Huei

Initial Steps in Forming the Electrode–Electrolyte Interface: H₂O Adsorption and Complex Formation on the Ag(111) Surface from Combining Quantum Mechanics Calculations and Ambient Pressure X-ray Photoelectron Spectroscopy

Journal Article · Thu Apr 04 00:00:00 EDT 2019 · Journal of the American Chemical Society · OSTI ID:1616436

Qian, Jin; Ye, Yifan; Yang, Hao; +3 more

Related Subjects

36 MATERIALS SCIENCE
Water formation reaction
Reaction pathway
Interfacial confinement
Silica bilayer film
Ambient pressure X-ray photoelectron spectroscopy
Density Functional Theory
Nanoreactor.

Title: Mechanism of the Accelerated Water Formation Reaction under Interfacial Confinement

Citation Formats

References (67)

Similar Records

Related Subjects