Atomic Layer Deposition for Preparing Isolated Co Sites on SiO2 for Ethane Dehydrogenation Catalysis

Huang, Renjing; Cheng, Yuan; Ji, Yichen; Gorte, Raymond J.

doi:10.3390/nano10020244

Title: Atomic Layer Deposition for Preparing Isolated Co Sites on SiO₂ for Ethane Dehydrogenation Catalysis

Journal Article · 29 January 2020 · Nanomaterials

DOI: https://doi.org/10.3390/nano10020244 · OSTI ID:1595934

Huang, Renjing ^[1]; Cheng, Yuan ^[2]; Ji, Yichen ^[2]; Gorte, Raymond J. ^[3]

University of Pennsylvania, Philadelphia, PA (United States); University of Pennsylvania
University of Pennsylvania, Philadelphia, PA (United States)
University of Pennsylvania, Philadelphia, PA (United States); Catalysis Center for Energy Innovation, Newark, DE (United States)

Unlike Co clusters, isolated Co atoms have been shown to be selective for catalytic dehydrogenation of ethane to ethylene; however, preparation of isolated Co sites requires special preparation procedures. Here, we demonstrate that Atomic Layer Deposition (ALD) of tris(2,2,6,6-tetramethyl-3,5-heptanedionato)cobalt(III) (Co(TMHD)₃) on silica and other supports is effective in producing these isolated species. Silica-supported catalysts prepared with one ALD cycle showed ethylene selectivities greater than 96% at 923 K and were stable when CO₂ was co-fed with the ethane. Co catalysts prepared by impregnation formed clusters that were significantly less active, selective, and stable. Rates and selectivities also decreased for catalysts with multiple ALD cycles. Isolated Co catalysts prepared on Al₂O₃ and MgAl₂O₄ showed reasonable selectivity for ethane dehydrogenation but were not as effective as their silica counterpart.

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Research Organization:: University of Pennsylvania, Philadelphia, PA (United States)

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

Grant/Contract Number:: SC0001004

OSTI ID:: 1595934

Journal Information:: Nanomaterials, Journal Name: Nanomaterials Journal Issue: 2 Vol. 10; ISSN 2079-4991; ISSN NANOKO

Publisher:: MDPICopyright Statement

Country of Publication:: United States

Language:: English

References (64)

Oxidative Dehydrogenation of Ethane: Common Principles and Mechanistic Aspects Gärtner, Christian A.; van Veen, André C.; Lercher, Johannes A. ChemCatChem, Vol. 5, Issue 11 https://doi.org/10.1002/cctc.201200966	journal	March 2013
Growth Per Cycle in Atomic Layer Deposition: Real Application Examplesof a Theoretical Model Puurunen, R. L. Chemical Vapor Deposition, Vol. 9, Issue 6 https://doi.org/10.1002/cvde.200306266	journal	December 2003
Mechanistic Insight in the Ethane Dehydrogenation Reaction over Cr/Al2O3 Catalysts Olsbye, Unni; Virnovskaia, Anastasia; Prytz, Øystein Catalysis Letters, Vol. 103, Issue 1-2 https://doi.org/10.1007/s10562-005-6521-7	journal	September 2005
Oxidative Dehydrogenation of Ethane to Ethylene with Carbon dioxide over Cr–Ce/SBA-15 Catalysts Shi, Xuejun; Ji, Shengfu; Wang, Kai Catalysis Letters, Vol. 125, Issue 3-4 https://doi.org/10.1007/s10562-008-9569-3	journal	July 2008
A Study of Support Effects for CH4 and CO Oxidation over Pd Catalysts on ALD-Modified Al2O3 Mao, Xinyu; Foucher, Alexandre; Stach, Eric A. Catalysis Letters, Vol. 149, Issue 4 https://doi.org/10.1007/s10562-019-02699-6	journal	February 2019
Formation of filamentous carbon from iron, cobalt and chromium catalyzed decomposition of acetylene Baker, R. Journal of Catalysis, Vol. 30, Issue 1 https://doi.org/10.1016/0021-9517(73)90055-9	journal	July 1973
The influence of oxonium ion and carbenium ion stabilities on the Alcohol/H-ZSM-5 interaction*1 Aronson, M. Journal of Catalysis, Vol. 98, Issue 2 https://doi.org/10.1016/0021-9517(86)90331-3	journal	April 1986
A thermodynamic study of the redox properties of supported Co particles Bakhmutsky, Kevin; Wieder, Noah L.; Baldassare, Thomas Applied Catalysis A: General, Vol. 397, Issue 1-2 https://doi.org/10.1016/j.apcata.2011.03.013	journal	April 2011
Cr/ZSM-5 for ethane dehydrogenation: Enhanced catalytic activity through surface silanol Cheng, Yanhu; Miao, Changxi; Hua, Weiming Applied Catalysis A: General, Vol. 532 https://doi.org/10.1016/j.apcata.2016.12.025	journal	February 2017
Olefins from conventional and heavy feedstocks: Energy use in steam cracking and alternative processes Ren, T.; Patel, M.; Blok, K. Energy, Vol. 31, Issue 4 https://doi.org/10.1016/j.energy.2005.04.001	journal	March 2006
Silica-doped TiO2 as support of gallium oxide for dehydrogenation of ethane with CO2 Lei, Tian-qi; Cheng, Yan-hu; Miao, Chang-xi Fuel Processing Technology, Vol. 177 https://doi.org/10.1016/j.fuproc.2018.04.037	journal	August 2018
Selective propane dehydrogenation with single-site CoII on SiO2 by a non-redox mechanism Hu, Bo; “Bean” Getsoian, Andrew; Schweitzer, Neil M. Journal of Catalysis, Vol. 322 https://doi.org/10.1016/j.jcat.2014.10.018	journal	February 2015
Single-site zinc on silica catalysts for propylene hydrogenation and propane dehydrogenation: Synthesis and reactivity evaluation using an integrated atomic layer deposition-catalysis instrument Camacho-Bunquin, Jeffrey; Aich, Payoli; Ferrandon, Magali Journal of Catalysis, Vol. 345 https://doi.org/10.1016/j.jcat.2016.10.017	journal	January 2017
Zirconium Modification Promotes Catalytic Activity of a Single-Site Cobalt Heterogeneous Catalyst for Propane Dehydrogenation Zhao, Yiqing; Sohn, Hyuntae; Hu, Bo ACS Omega, Vol. 3, Issue 9 https://doi.org/10.1021/acsomega.8b00862	journal	September 2018
Catalytic Dehydrogenation of Light Alkanes on Metals and Metal Oxides Sattler, Jesper J. H. B.; Ruiz-Martinez, Javier; Santillan-Jimenez, Eduardo Chemical Reviews, Vol. 114, Issue 20 https://doi.org/10.1021/cr5002436	journal	August 2014
Fluid Catalytic Cracking Study of Coker Gas Oil: Effects of Processing Parameters on Sulfur and Nitrogen Distributions Zhang, Jinhong; Shan, Honghong; Chen, Xiaobo Energy & Fuels, Vol. 28, Issue 2 https://doi.org/10.1021/ef401990s	journal	December 2013
Preparation and characterization of highly dispersed cobalt oxide and sulfide catalysts supported on silica Okamoto, Yasuaki; Nagata, Kozo; Adachi, Toshinori The Journal of Physical Chemistry, Vol. 95, Issue 1 https://doi.org/10.1021/j100154a057	journal	January 1991
Smart Pd Catalyst with Improved Thermal Stability Supported on High-Surface-Area LaFeO ₃ Prepared by Atomic Layer Deposition Onn, Tzia Ming; Monai, Matteo; Dai, Sheng Journal of the American Chemical Society, Vol. 140, Issue 14 https://doi.org/10.1021/jacs.7b12900	journal	January 2018
Carbon dioxide reduction in tandem with light-alkane dehydrogenation Gomez, Elaine; Yan, Binhang; Kattel, Shyam Nature Reviews Chemistry, Vol. 3, Issue 11 https://doi.org/10.1038/s41570-019-0128-9	journal	September 2019
Control of metal-support interactions in heterogeneous catalysts to enhance activity and selectivity van Deelen, Tom W.; Hernández Mejía, Carlos; de Jong, Krijn P. Nature Catalysis, Vol. 2, Issue 11 https://doi.org/10.1038/s41929-019-0364-x	journal	November 2019
Dehydrogenation of ethane over gallium oxide in the presence of carbon dioxide Nakagawa, Kiyoharu; Okamura, Masato; Ikenaga, Naoki Chemical Communications, Issue 9 https://doi.org/10.1039/a800184g	journal	January 1998
A Characterization Study of Reactive Sites in ALD-Synthesized WOx/ZrO2 Catalysts Wang, Cong; Mao, Xinyu; Lee, Jennifer Catalysts, Vol. 8, Issue 7 https://doi.org/10.3390/catal8070292	journal	July 2018
Stabilization of ZrO2 Powders via ALD of CeO2 and ZrO2 Lin, Chao; Mao, Xinyu; Onn, Tzia Inorganics, Vol. 5, Issue 4 https://doi.org/10.3390/inorganics5040065	journal	October 2017
Atomic Layer Deposition on Porous Materials: Problems with Conventional Approaches to Catalyst and Fuel Cell Electrode Preparation Onn, Tzia; Küngas, Rainer; Fornasiero, Paolo Inorganics, Vol. 6, Issue 1 https://doi.org/10.3390/inorganics6010034	journal	March 2018
“Intelligent” Pt Catalysts Based on Thin LaCoO3 Films Prepared by Atomic Layer Deposition Mao, Xinyu; Foucher, Alexandre C.; Stach, Eric A. Inorganics, Vol. 7, Issue 9 https://doi.org/10.3390/inorganics7090113	journal	September 2019
Oxidative Dehydrogenation of Ethane: Common Principles and Mechanistic Aspects Gärtner, Christian A.; van Veen, André C.; Lercher, Johannes A. ChemCatChem, Vol. 5, Issue 11 https://doi.org/10.1002/cctc.201200966	journal	March 2013
Growth Per Cycle in Atomic Layer Deposition: Real Application Examplesof a Theoretical Model Puurunen, R. L. Chemical Vapor Deposition, Vol. 9, Issue 6 https://doi.org/10.1002/cvde.200306266	journal	December 2003
Mechanistic Insight in the Ethane Dehydrogenation Reaction over Cr/Al2O3 Catalysts Olsbye, Unni; Virnovskaia, Anastasia; Prytz, Øystein Catalysis Letters, Vol. 103, Issue 1-2 https://doi.org/10.1007/s10562-005-6521-7	journal	September 2005
Oxidative dehydrogenation of ethane over Co–BaCO3 catalysts using CO2 as oxidant: effects of Co promoter Zhang, Xin; Ye, Qing; Xu, Boqing Catalysis Letters, Vol. 117, Issue 3-4 https://doi.org/10.1007/s10562-007-9122-9	journal	May 2007
Oxidative Dehydrogenation of Ethane to Ethylene with Carbon dioxide over Cr–Ce/SBA-15 Catalysts Shi, Xuejun; Ji, Shengfu; Wang, Kai Catalysis Letters, Vol. 125, Issue 3-4 https://doi.org/10.1007/s10562-008-9569-3	journal	July 2008
A Study of Support Effects for CH4 and CO Oxidation over Pd Catalysts on ALD-Modified Al2O3 Mao, Xinyu; Foucher, Alexandre; Stach, Eric A. Catalysis Letters, Vol. 149, Issue 4 https://doi.org/10.1007/s10562-019-02699-6	journal	February 2019
Catalytic growth of carbon filaments Baker, R. T. K. Carbon, Vol. 27, Issue 3 https://doi.org/10.1016/0008-6223(89)90062-6	journal	January 1989
Formation of filamentous carbon from iron, cobalt and chromium catalyzed decomposition of acetylene Baker, R. Journal of Catalysis, Vol. 30, Issue 1 https://doi.org/10.1016/0021-9517(73)90055-9	journal	July 1973
The influence of oxonium ion and carbenium ion stabilities on the Alcohol/H-ZSM-5 interaction*1 Aronson, M. Journal of Catalysis, Vol. 98, Issue 2 https://doi.org/10.1016/0021-9517(86)90331-3	journal	April 1986
Dehydrogenation and oxydehydrogenation of paraffins to olefins Bhasin, M. M.; McCain, J. H.; Vora, B. V. Applied Catalysis A: General, Vol. 221, Issue 1-2, p. 397-419 https://doi.org/10.1016/S0926-860X(01)00816-X	journal	November 2001
A thermodynamic study of the redox properties of supported Co particles Bakhmutsky, Kevin; Wieder, Noah L.; Baldassare, Thomas Applied Catalysis A: General, Vol. 397, Issue 1-2 https://doi.org/10.1016/j.apcata.2011.03.013	journal	April 2011
Silica is preferred over various single and mixed oxides as support for CO 2 -assisted cobalt-catalyzed oxidative dehydrogenation of ethane Koirala, Rajesh; Buechel, Robert; Pratsinis, Sotiris E. Applied Catalysis A: General, Vol. 527 https://doi.org/10.1016/j.apcata.2016.08.032	journal	October 2016
Cr/ZSM-5 for ethane dehydrogenation: Enhanced catalytic activity through surface silanol Cheng, Yanhu; Miao, Changxi; Hua, Weiming Applied Catalysis A: General, Vol. 532 https://doi.org/10.1016/j.apcata.2016.12.025	journal	February 2017
Effect of cobalt loading on structure and catalytic behavior of CoO x /SiO 2 in CO 2 -assisted dehydrogenation of ethane Koirala, Rajesh; Safonova, Olga V.; Pratsinis, Sotiris E. Applied Catalysis A: General, Vol. 552 https://doi.org/10.1016/j.apcata.2017.12.025	journal	February 2018
Olefins from conventional and heavy feedstocks: Energy use in steam cracking and alternative processes Ren, T.; Patel, M.; Blok, K. Energy, Vol. 31, Issue 4 https://doi.org/10.1016/j.energy.2005.04.001	journal	March 2006
Silica-doped TiO2 as support of gallium oxide for dehydrogenation of ethane with CO2 Lei, Tian-qi; Cheng, Yan-hu; Miao, Chang-xi Fuel Processing Technology, Vol. 177 https://doi.org/10.1016/j.fuproc.2018.04.037	journal	August 2018
Selective propane dehydrogenation with single-site CoII on SiO2 by a non-redox mechanism Hu, Bo; “Bean” Getsoian, Andrew; Schweitzer, Neil M. Journal of Catalysis, Vol. 322 https://doi.org/10.1016/j.jcat.2014.10.018	journal	February 2015
Single-site zinc on silica catalysts for propylene hydrogenation and propane dehydrogenation: Synthesis and reactivity evaluation using an integrated atomic layer deposition-catalysis instrument Camacho-Bunquin, Jeffrey; Aich, Payoli; Ferrandon, Magali Journal of Catalysis, Vol. 345 https://doi.org/10.1016/j.jcat.2016.10.017	journal	January 2017
Endothermic Reforming of n -Hexane on Metal (Pt, Ga) Containing H-ZSM-5 at High Pressures Yeh, Yu-Hao; Yu, Jingye; Luo, Jing Industrial & Engineering Chemistry Research, Vol. 54, Issue 43 https://doi.org/10.1021/acs.iecr.5b03121	journal	October 2015
CO Oxidation on Metal Oxide Supported Single Pt atoms: The Role of the Support Lou, Yang; Liu, Jingyue Industrial & Engineering Chemistry Research, Vol. 56, Issue 24 https://doi.org/10.1021/acs.iecr.7b01477	journal	June 2017
Atomically Dispersed Co and Cu on N-Doped Carbon for Reactions Involving C–H Activation Xie, Jiahan; Kammert, James D.; Kaylor, Nicholas ACS Catalysis, Vol. 8, Issue 5 https://doi.org/10.1021/acscatal.8b00141	journal	March 2018
Influence of Tight Confinement on Selective Oxidative Dehydrogenation of Ethane on MoVTeNb Mixed Oxides Annamalai, Leelavathi; Liu, Yilang; Ezenwa, Sopuruchukwu ACS Catalysis, Vol. 8, Issue 8 https://doi.org/10.1021/acscatal.8b01586	journal	July 2018
Interface Tailoring of Heterogeneous Catalysts by Atomic Layer Deposition Zhang, Bin; Qin, Yong ACS Catalysis, Vol. 8, Issue 11 https://doi.org/10.1021/acscatal.8b02659	journal	September 2018
“Intelligent” Pt Catalysts Studied on High-Surface-Area CaTiO ₃ Films Lin, Chao; Foucher, Alexandre C.; Ji, Yichen ACS Catalysis, Vol. 9, Issue 8 https://doi.org/10.1021/acscatal.9b01278	journal	June 2019
Zirconium Modification Promotes Catalytic Activity of a Single-Site Cobalt Heterogeneous Catalyst for Propane Dehydrogenation Zhao, Yiqing; Sohn, Hyuntae; Hu, Bo ACS Omega, Vol. 3, Issue 9 https://doi.org/10.1021/acsomega.8b00862	journal	September 2018
Catalytic Dehydrogenation of Light Alkanes on Metals and Metal Oxides Sattler, Jesper J. H. B.; Ruiz-Martinez, Javier; Santillan-Jimenez, Eduardo Chemical Reviews, Vol. 114, Issue 20 https://doi.org/10.1021/cr5002436	journal	August 2014
Fluid Catalytic Cracking Study of Coker Gas Oil: Effects of Processing Parameters on Sulfur and Nitrogen Distributions Zhang, Jinhong; Shan, Honghong; Chen, Xiaobo Energy & Fuels, Vol. 28, Issue 2 https://doi.org/10.1021/ef401990s	journal	December 2013
Preparation and characterization of highly dispersed cobalt oxide and sulfide catalysts supported on silica Okamoto, Yasuaki; Nagata, Kozo; Adachi, Toshinori The Journal of Physical Chemistry, Vol. 95, Issue 1 https://doi.org/10.1021/j100154a057	journal	January 1991
Smart Pd Catalyst with Improved Thermal Stability Supported on High-Surface-Area LaFeO ₃ Prepared by Atomic Layer Deposition Onn, Tzia Ming; Monai, Matteo; Dai, Sheng Journal of the American Chemical Society, Vol. 140, Issue 14 https://doi.org/10.1021/jacs.7b12900	journal	January 2018
Is True Ethane Oxydehydrogenation Feasible? Bhasin, Madan M. Topics in Catalysis, Vol. 23, Issue 1/4, p. 145-149 https://doi.org/10.1023/A:1024884623238	journal	January 2003
Carbon dioxide reduction in tandem with light-alkane dehydrogenation Gomez, Elaine; Yan, Binhang; Kattel, Shyam Nature Reviews Chemistry, Vol. 3, Issue 11 https://doi.org/10.1038/s41570-019-0128-9	journal	September 2019
Control of metal-support interactions in heterogeneous catalysts to enhance activity and selectivity van Deelen, Tom W.; Hernández Mejía, Carlos; de Jong, Krijn P. Nature Catalysis, Vol. 2, Issue 11 https://doi.org/10.1038/s41929-019-0364-x	journal	November 2019
Dehydrogenation of ethane over gallium oxide in the presence of carbon dioxide Nakagawa, Kiyoharu; Okamura, Masato; Ikenaga, Naoki Chemical Communications, Issue 9 https://doi.org/10.1039/a800184g	journal	January 1998
Conformality in atomic layer deposition: Current status overview of analysis and modelling Cremers, Véronique; Puurunen, Riikka L.; Dendooven, Jolien Applied Physics Reviews, Vol. 6, Issue 2 https://doi.org/10.1063/1.5060967	journal	June 2019
Controllable ALD synthesis of platinum nanoparticles by tuning different synthesis parameters Wang, Chuandao; Hu, Linhua; Lin, Yuyuan Journal of Physics D: Applied Physics, Vol. 50, Issue 41 https://doi.org/10.1088/1361-6463/aa8709	journal	September 2017
A Characterization Study of Reactive Sites in ALD-Synthesized WOx/ZrO2 Catalysts Wang, Cong; Mao, Xinyu; Lee, Jennifer Catalysts, Vol. 8, Issue 7 https://doi.org/10.3390/catal8070292	journal	July 2018
Stabilization of ZrO2 Powders via ALD of CeO2 and ZrO2 Lin, Chao; Mao, Xinyu; Onn, Tzia Inorganics, Vol. 5, Issue 4 https://doi.org/10.3390/inorganics5040065	journal	October 2017
Atomic Layer Deposition on Porous Materials: Problems with Conventional Approaches to Catalyst and Fuel Cell Electrode Preparation Onn, Tzia; Küngas, Rainer; Fornasiero, Paolo Inorganics, Vol. 6, Issue 1 https://doi.org/10.3390/inorganics6010034	journal	March 2018
“Intelligent” Pt Catalysts Based on Thin LaCoO3 Films Prepared by Atomic Layer Deposition Mao, Xinyu; Foucher, Alexandre C.; Stach, Eric A. Inorganics, Vol. 7, Issue 9 https://doi.org/10.3390/inorganics7090113	journal	September 2019

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36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Co/SiO2
Ethane dehydrogenation
atomic layer deposition (ALD)
cobalt
oxidative dehydrogenation
silica
single-site catalysts

Title: Atomic Layer Deposition for Preparing Isolated Co Sites on SiO2 for Ethane Dehydrogenation Catalysis

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References (64)

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Title: Atomic Layer Deposition for Preparing Isolated Co Sites on SiO₂ for Ethane Dehydrogenation Catalysis