Acetic Acid Adsorption and Reactions on Ni(110)

Hofman, Michelle S.; Scoullos, Emanuel V.; Robbins, Jason P.; Ezeonu, Lotanna; Potapenko, Denis V.; Yang, Xiaofang; Podkolzin, Simon G.; Koel, Bruce E.

doi:10.1021/acs.langmuir.0c00713

Acetic Acid Adsorption and Reactions on Ni(110)

Journal Article · Mon Jun 15 00:00:00 EDT 2020 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.0c00713· OSTI ID:1985488

Hofman, Michelle S. ^[1]; Scoullos, Emanuel V. ^[2]; Robbins, Jason P. ^[3]; Ezeonu, Lotanna ^[3]; Potapenko, Denis V. ^[2]; Yang, Xiaofang ^[2]; ^[3]; ^[2]

Princeton University, NJ (United States); Princeton University
Princeton University, NJ (United States)
Stevens Institute of Technology, Hoboken, NJ (United States)

Acetic acid adsorption and reactions at multiple surface coverage values on Ni(110) were studied with temperature-programmed desorption (TPD) and infrared reflection absorption spectroscopy (IRAS) at 90–500 K. The experimental measurements were interpreted with density functional theory (DFT) calculations that provided information on adsorbate geometries, energies, and vibrational modes. Below the monolayer saturation coverage of 0.36 ML at 90 K, acetic acid adsorbs mostly molecularly. Above this coverage, a physisorbed layer is formed with dimers and catemers, without detectable monomers. Dimers and catemers desorb as molecular acetic acid at 157 and 172 K, respectively. Between 90 and 200 K, the O–H bond in acetic acid breaks to form bridge-bonded bidentate acetate that becomes the dominant surface species. Desorption-limited hydrogen evolution is observed at 265 K. However, even after the acetate formation, acetic acid desorbs molecularly at 200–300 K due to recombination. Minor surface species observed at 200 K, acetyls or acetates with a carbonyl group, decompose below 350 K and generate adsorbed carbon monoxide. At 350 K, the surface likely undergoes restructuring, the extent of which increases with acetic acid coverage. The initial dominant bridge-bonded bidentate acetate species formed below 200 K remain on the surface, but they now mostly adsorb on the restructured sites. Here, the acetates and all other remaining hydrocarbon species decompose simultaneously at 425 K in a narrow temperature range with concurrent evolution of hydrogen, carbon monoxide, and carbon dioxide. Above 425 K, only carbon remains on the surface.

View Accepted Manuscript (DOE)

Research Organization:: Princeton University, NJ (United States)

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

Grant/Contract Number:: SC0019052

OSTI ID:: 1985488

Alternate ID(s):: OSTI ID: 1803533

Report Number(s):: DOE-PU-0019052-2

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 30 Vol. 36; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (38)

Geometric Requirements for Hydrocarbon Catalytic Sites on Platinum Surfaces Gao, Jie; Zhao, Haibo; Yang, Xiaofang Angewandte Chemie International Edition, Vol. 53, Issue 14 https://doi.org/10.1002/anie.201309043	journal	February 2014
Observation and Identification of an Atomic Oxygen Structure on Catalytic Gold Nanoparticles Liu, Kai; Chen, Tao; He, Shuyue Angewandte Chemie International Edition, Vol. 56, Issue 42 https://doi.org/10.1002/anie.201706647	journal	September 2017
Catalytic Platinum Nanoparticles Decorated with Subnanometer Molybdenum Clusters for Biomass Processing Zheng, Yiteng; Tang, Ziyu; Podkolzin, Simon G. Chemistry – A European Journal, Vol. 26, Issue 23 https://doi.org/10.1002/chem.202000139	journal	March 2020
Acetic Acid on Rh(110): The Stabilization and Autocatalytic Decomposition of Acetate Li, Y. X.; Bowker, M. Journal of Catalysis, Vol. 142, Issue 2 https://doi.org/10.1006/jcat.1993.1236	journal	August 1993
From surface science to catalysis: Surface ?explosions? observed on Rh crystals and supported catalysts Cassidy, T. J.; Allen, M. D.; Li, Y. Catalysis Letters, Vol. 21, Issue 3-4 https://doi.org/10.1007/BF00769484	journal	January 1993
Acetate formation and explosive decomposition during ethanol oxidation on Rh Bowker, Michael; Li, Yongxue Catalysis Letters, Vol. 10, Issue 3-4 https://doi.org/10.1007/BF00772078	journal	January 1991
The autocatalytic decomposition of acetic acid on Ni(110) Madix, R. J.; Falconer, J. L.; Suszko, A. M. Surface Science, Vol. 54, Issue 1 https://doi.org/10.1016/0039-6028(76)90083-2	journal	January 1976
Decomposition of acetic acid monomer, acetic acid dimer, and acetic anhydride on Ni(111) Schoofs, Gregory R.; Benziger, Jay B. Surface Science, Vol. 143, Issue 2-3 https://doi.org/10.1016/0039-6028(84)90547-8	journal	August 1984
Surface reconstruction and surface explosion phenomena in the nickel (110)/hydrogen system Christmann, K.; Chehab, F.; Penka, V. Surface Science, Vol. 152-153 https://doi.org/10.1016/0039-6028(85)90165-7	journal	April 1985
Surface phases of Ni(110) induced by adsorption of deuterium Jackman, T. E.; Griffiths, K.; Unertl, W. N. Surface Science, Vol. 179, Issue 2-3 https://doi.org/10.1016/0039-6028(87)90060-4	journal	January 1987
Self-acceleration in the decomposition of acetic acid on Rh{111}: a combined TPD and laser induced desorption study Hoogers, G.; Papageorgopoulos, D. C.; Ge, Q. Surface Science, Vol. 340, Issue 1-2 https://doi.org/10.1016/0039-6028(95)00673-7	journal	October 1995
Spectres de vibration des molecules CH3COOH, CH3COOD, CD3COOH et CD3COOD—III. Spectres infrarouges des cristaux Haurie, Michel; Novak, Alexander Spectrochimica Acta, Vol. 21, Issue 7 https://doi.org/10.1016/0371-1951(65)80205-3	journal	July 1965
Adsorption and reaction of acetaldehyde on Pt( 111 ) and Sn/Pt( 111 ) surface alloys Zhao, Haibo; Kim, Jooho; Koel, Bruce E. Surface Science, Vol. 538, Issue 3 https://doi.org/10.1016/S0039-6028(03)00602-2	journal	July 2003
Core-shell nickel catalysts for the steam reforming of acetic acid Pu, Jianglong; Nishikado, Katsuki; Wang, Ningning Applied Catalysis B: Environmental, Vol. 224 https://doi.org/10.1016/j.apcatb.2017.09.058	journal	May 2018
Steam reforming of acetic acid over nickel-based catalysts: The intrinsic effects of nickel precursors on behaviors of nickel catalysts Yu, Zhenjie; Hu, Xun; Jia, Peng Applied Catalysis B: Environmental, Vol. 237 https://doi.org/10.1016/j.apcatb.2018.06.020	journal	December 2018
Effects of hydrogen and propylene presence on decomposition of hydrogen peroxide over palladium catalysts Chen, Tao; Kertalli, Emila; Nijhuis, T. Alexander Journal of Catalysis, Vol. 341 https://doi.org/10.1016/j.jcat.2016.06.012	journal	September 2016
Copper ferrite supported gold nanoparticles as efficient and recyclable catalyst for liquid-phase ethanol oxidation Hu, Wenjia; Li, Deping; Yang, Yang Journal of Catalysis, Vol. 357 https://doi.org/10.1016/j.jcat.2017.11.011	journal	January 2018
Acetic acid adsorption and decomposition on Pd(110) Bowker, Michael; Morgan, Chris; Couves, John Surface Science, Vol. 555, Issue 1-3 https://doi.org/10.1016/j.susc.2003.12.040	journal	April 2004
Identification of Vertical and Horizontal Configurations for BPE Adsorption on Silver Surfaces Chen, Tao; Pal, Amrita; Gao, Jie The Journal of Physical Chemistry C, Vol. 119, Issue 43 https://doi.org/10.1021/acs.jpcc.5b07831	journal	October 2015
Guaiacol Adsorption and Decomposition on Platinum Scoullos, Emanuel V.; Hofman, Michelle S.; Zheng, Yiteng The Journal of Physical Chemistry C, Vol. 122, Issue 51 https://doi.org/10.1021/acs.jpcc.8b06555	journal	October 2018
Synthesis of Transportation Fuels from Biomass: Chemistry, Catalysts, and Engineering Huber, George W.; Iborra, Sara; Corma, Avelino Chemical Reviews, Vol. 106, Issue 9, p. 4044-4098 https://doi.org/10.1021/cr068360d	journal	September 2006
Recent Advances in Hydrotreating of Pyrolysis Bio-Oil and Its Oxygen-Containing Model Compounds Wang, Huamin; Male, Jonathan; Wang, Yong ACS Catalysis, Vol. 3, Issue 5 https://doi.org/10.1021/cs400069z	journal	April 2013
Controlling Acetylene Adsorption and Reactions on Pt–Sn Catalytic Surfaces Gao, Jie; Zhao, Haibo; Yang, Xiaofang ACS Catalysis, Vol. 3, Issue 6 https://doi.org/10.1021/cs400198f	journal	April 2013
Ethylene adsorption and decomposition on platinum (210): chemistry of .pi.-bound ethylene Backman, A. L.; Masel, R. I. The Journal of Physical Chemistry, Vol. 94, Issue 13 https://doi.org/10.1021/j100376a026	journal	June 1990
The Vibrational Spectrum, Associative and Thermodynamic Properties of Acetic Acid Vapor Weltner, William Journal of the American Chemical Society, Vol. 77, Issue 15 https://doi.org/10.1021/ja01620a003	journal	August 1955
Rotational Isomerism in Acetic Acid: The First Experimental Observation of the High-Energy Conformer Maçôas, Ermelinda M. S.; Khriachtchev, Leonid; Pettersson, Mika Journal of the American Chemical Society, Vol. 125, Issue 52 https://doi.org/10.1021/ja038341a	journal	December 2003
Carbon Dioxide Hydrogenation on Ni(110) Vesselli, Erik; De Rogatis, Loredana; Ding, Xunlei Journal of the American Chemical Society, Vol. 130, Issue 34 https://doi.org/10.1021/ja802554g	journal	July 2008
Low Temperature Oxidation of Ethane to Oxygenates by Oxygen over Iridium-Cluster Catalysts Jin, Renxi; Peng, Mi; Li, Ang Journal of the American Chemical Society, Vol. 141, Issue 48 https://doi.org/10.1021/jacs.9b06986	journal	October 2019
High-Pressure Carbon Monoxide Adsorption on Pt(111) Revisited: A Sum Frequency Generation Study ^† Rupprechter, G.; Dellwig, T.; Unterhalt, H. The Journal of Physical Chemistry B, Vol. 105, Issue 18 https://doi.org/10.1021/jp003585s	journal	May 2001
The Role of Surface Deconstruction in the Autocatalytic Decomposition of Formate and Acetate on Ni(110) ^† Alemozafar, Ali R.; Madix, Robert J. The Journal of Physical Chemistry B, Vol. 108, Issue 38 https://doi.org/10.1021/jp0400061	journal	September 2004
Adsorption and Reaction of Aldehydes on Pd Surfaces Shekhar, Ratna; Barteau, Mark A.; Plank, Russell V. The Journal of Physical Chemistry B, Vol. 101, Issue 40 https://doi.org/10.1021/jp971077l	journal	October 1997
Acetic Anhydride in the Gas Phase, Studied by Electron Diffraction and Infrared Spectroscopy, Supplemented With ab Initio Calculations of Geometries and Force Fields Wu, Guang; Van Alsenoy, C.; Geise, H. J. The Journal of Physical Chemistry A, Vol. 104, Issue 7 https://doi.org/10.1021/jp993131z	journal	January 2000
Hydrogen bonding in carboxylic acid adlayers on Pd(111): evidence for catemer formation Davis, J. L.; Barteau, M. A. Langmuir, Vol. 5, Issue 6 https://doi.org/10.1021/la00090a004	journal	November 1989
Kinetic explosion and bistability in adsorption and reaction of acetic acid on Pd(110) Bowker, Michael; Morgan, Chris; Zhdanov, Vladimir P. Physical Chemistry Chemical Physics, Vol. 9, Issue 42 https://doi.org/10.1039/b709384e	journal	January 2007
Adsorption and autocatalytic decomposition of acetic acid on Pd(110) Aas, Nina; Bowker, Michael Journal of the Chemical Society, Faraday Transactions, Vol. 89, Issue 8 https://doi.org/10.1039/ft9938901249	journal	January 1993
From molecules to solids with the DMol3 approach Delley, B. The Journal of Chemical Physics, Vol. 113, Issue 18 https://doi.org/10.1063/1.1316015	journal	November 2000
An all‐electron numerical method for solving the local density functional for polyatomic molecules Delley, B. The Journal of Chemical Physics, Vol. 92, Issue 1 https://doi.org/10.1063/1.458452	journal	January 1990
The formation of acetic anhydride by decomposition of acetic acid adsorbed on Ni(111) Erley, W.; Chen, J. G.; Sander, D. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 8, Issue 2 https://doi.org/10.1116/1.576906	journal	March 1990

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