Operando Structure Determination of Cu and Zn on Supported MgO/SiO2 Catalysts during Ethanol Conversion to 1,3-Butadiene

Taifan, William E.; Li, Yuanyuan; Baltrus, John P.; Zhang, Lihua; Frenkel, Anatoly I.; Baltrusaitis, Jonas

doi:10.1021/acscatal.8b03515

Title: Operando Structure Determination of Cu and Zn on Supported MgO/SiO₂ Catalysts during Ethanol Conversion to 1,3-Butadiene

Journal Article · 25 November 2018 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.8b03515 · OSTI ID:1492773

Taifan, William E. ^[1]; Li, Yuanyuan ^[2]; Baltrus, John P. ^[3]; Zhang, Lihua ^[4];

^[5];

^[1]

Lehigh Univ., Bethlehem, PA (United States)
Stony Brook Univ., NY (United States)
National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)

Electronic structure and reactivity of Cu- and Zn-promoted wet kneaded MgO/SiO₂ catalysts was interrogated during ethanol reaction to 1,3-BD. A multimodal nature of characterization, including in situ or operando X-ray, electron, light spectroscopies and steady state reactivity measurements demonstrated critical new information on the temporal evolution of the catalyst active sites including key measurements performed operando using synchrotron source (EXAFS and XANES). In situ DRIFT spectroscopy allowed to decouple the aldol condensation and dehydrogenation reactive steps due to the promotion with enhanced ability to carry out aldol condensation, as correlated with the steady state reactivity experiments . In situ UV-Vis spectroscopy presented a complex picture of the adsorbates with π- π* electronic transitions due to the allylic cations, cyclic or aromatic species while also suggesting oligomeric CuO species were formed. Operando X-ray measurements combined with ab initio multiple scattering modelling performed as a function of temperature identified a new transient intermediate assigned to a 4-fold coordinate Cu species that was key leading to increase in Cu-Cu pair number. For the first time, two types of Zn pairs, namely Zn-O and Zn-Mg, were identified during X-ray analysis under operating conditions. With Zn nearly 6-coordinated when in the vicinity of Mg while Zn-O species coordinated to nearly 4 nearest neighbors. The data suggest that such supported catalyst deactivation might proceed not only via carbon coking mechanism but also through the dispersed Cu site diffusion and growth due to the nearest neighbor oxygen atoms loss. The results presented suggest intermediates for segregation/deactivation mechanisms for a broader set of supported Cu and Zn catalysts used for alcohol upgrading catalytic reactions.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States); National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1492773

Report Number(s):: BNL--210922-2019-JAAM; NETL-PUB--21841

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 1 Vol. 9; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (83)

Spontaneous polymerization of acetaldehyde to polyacetaldehyde at close to dry-ice temperature Georgieff, K. K. Journal of Applied Polymer Science, Vol. 10, Issue 9 https://doi.org/10.1002/app.1966.070100908	journal	September 1966
Mechanistic Studies on Chabazite-Type Methanol-to-Olefin Catalysts: Insights from Time-Resolved UV/Vis Microspectroscopy Combined with Theoretical Simulations Van Speybroeck, Veronique; Hemelsoet, Karen; De Wispelaere, Kristof ChemCatChem, Vol. 5, Issue 1 https://doi.org/10.1002/cctc.201200580	journal	November 2012
Mechanistic Study of Ethanol Dehydrogenation over Silica-Supported Silver Sushkevich, Vitaly L.; Ivanova, Irina I.; Taarning, Esben ChemCatChem, Vol. 5, Issue 8 https://doi.org/10.1002/cctc.201300033	journal	May 2013
Combined Operando UV/Vis/IR Spectroscopy Reveals the Role of Methoxy and Aromatic Species during the Methanol-to-Olefins Reaction over H-SAPO-34 Qian, Qingyun; Vogt, Charlotte; Mokhtar, Mohamed ChemCatChem, Vol. 6, Issue 12 https://doi.org/10.1002/cctc.201402714	journal	October 2014
Ethanol to 1,3-Butadiene Conversion by using ZrZn-Containing MgO/SiO ₂ Systems Prepared by Co-precipitation and Effect of Catalyst Acidity Modification Da Ros, Simoní; Jones, Matthew D.; Mattia, Davide ChemCatChem, Vol. 8, Issue 14 https://doi.org/10.1002/cctc.201600331	journal	June 2016
Space- and Time-Resolved In-situ Spectroscopy on the Coke Formation in Molecular Sieves: Methanol-to-Olefin Conversion over H-ZSM-5 and H-SAPO-34 Mores, Davide; Stavitski, Eli; Kox, Marianne H. F. Chemistry - A European Journal, Vol. 14, Issue 36 https://doi.org/10.1002/chem.200801293	journal	November 2008
Coke Formation during the Methanol-to-Olefin Conversion: In Situ Microspectroscopy on Individual H-ZSM-5 Crystals with Different Brønsted Acidity Mores, Davide; Kornatowski , Jan; Olsbye, Unni Chemistry - A European Journal, Vol. 17, Issue 10 https://doi.org/10.1002/chem.201002624	journal	February 2011
Effects of Coke Deposits on the Catalytic Performance of Large Zeolite H-ZSM-5 Crystals during Alcohol-to-Hydrocarbon Reactions as Investigated by a Combination of Optical Spectroscopy and Microscopy Nordvang, Emily C.; Borodina, Elena; Ruiz-Martínez, Javier Chemistry - A European Journal, Vol. 21, Issue 48 https://doi.org/10.1002/chem.201503136	journal	October 2015
Design of a Metal-Promoted Oxide Catalyst for the Selective Synthesis of Butadiene from Ethanol Sushkevich, Vitaly L.; Ivanova, Irina I.; Ordomsky, Vitaly V. ChemSusChem, Vol. 7, Issue 9 https://doi.org/10.1002/cssc.201402346	journal	August 2014
Effect of Preparation Method and CuO Promotion in the Conversion of Ethanol into 1,3-Butadiene over SiO ₂ -MgO Catalysts Angelici, Carlo; Velthoen, Marjolein E. Z.; Weckhuysen, Bert M. ChemSusChem, Vol. 7, Issue 9 https://doi.org/10.1002/cssc.201402361	journal	July 2014
On the Chemistry of Ethanol on Basic Oxides: Revising Mechanisms and Intermediates in the Lebedev and Guerbet reactions Chieregato, Alessandro; Velasquez Ochoa, Juliana; Bandinelli, Claudia ChemSusChem, Vol. 8, Issue 2 https://doi.org/10.1002/cssc.201402632	journal	December 2014
Ternary Ag/MgO-SiO ₂ Catalysts for the Conversion of Ethanol into Butadiene Janssens, Wout; Makshina, Ekaterina V.; Vanelderen, Pieter ChemSusChem, Vol. 8, Issue 6 https://doi.org/10.1002/cssc.201402894	journal	November 2014
From Sugars to Wheels: The Conversion of Ethanol to 1,3-Butadiene over Metal-Promoted Magnesia-Silicate Catalysts Shylesh, Sankaranarayanapillai; Gokhale, Amit A.; Scown, Corinne D. ChemSusChem, Vol. 9, Issue 12 https://doi.org/10.1002/cssc.201600195	journal	May 2016
Ag-Promoted ZrBEA Zeolites Obtained by Post-Synthetic Modification for Conversion of Ethanol to Butadiene Sushkevich, Vitaly L.; Ivanova, Irina I. ChemSusChem, Vol. 9, Issue 16 https://doi.org/10.1002/cssc.201600572	journal	July 2016
CuO–SiO2 Sol–Gel Catalysts: Characterization and Catalytic Properties for NO Reduction Díaz, G.; Pérez-Hernández, R.; Gómez-Cortés, A. Journal of Catalysis, Vol. 187, Issue 1 https://doi.org/10.1006/jcat.1999.2578	journal	October 1999
ZnO/MgO containing ZnO nanoparticles as a highly effective heterogeneous base catalyst for the synthesis of 4H-pyrans and coumarins in [bmim]BF4 Valizadeh, H.; Azimi, A. A. Journal of the Iranian Chemical Society, Vol. 8, Issue 1 https://doi.org/10.1007/BF03246209	journal	March 2011
DFT Computation of Relative Spin-State Energetics of Transition Metal Compounds Harvey, Jeremy N. Principles and Applications of Density Functional Theory in Inorganic Chemistry I https://doi.org/10.1007/b97939	book	January 2004
Ethanol Conversion to 1,3-Butadiene on ZnO/MgO–SiO2 Catalysts: Effect of ZnO Content and MgO:SiO2 Ratio Larina, Olga V.; Kyriienko, Pavlo I.; Soloviev, Sergiy O. Catalysis Letters, Vol. 145, Issue 5 https://doi.org/10.1007/s10562-015-1509-4	journal	March 2015
X-ray absorption near edge structures (xanes) of Cu/ZnO/Al2O3 Co shift catalysts Vlaic, G.; Bart, J. C. J.; Cavigiolo, W. Chemical Physics Letters, Vol. 76, Issue 3 https://doi.org/10.1016/0009-2614(80)80646-4	journal	December 1980
In situ cell for combined XRD and on-line catalysis tests: Studies of Cu-based water gas shift and methanol catalysts Clausen, B. Journal of Catalysis, Vol. 132, Issue 2 https://doi.org/10.1016/0021-9517(91)90168-4	journal	December 1991
The hydroxylated surface of MgO powders and the formation of surface sites Coluccia, S.; Lavagnino, S.; Marchese, L. Materials Chemistry and Physics, Vol. 18, Issue 5-6 https://doi.org/10.1016/0254-0584(88)90016-8	journal	January 1988
A structure model as the origin of catalytic properties of metal-doped MgO systems Asakura, K.; Iwasawa, Y. Materials Chemistry and Physics, Vol. 18, Issue 5-6 https://doi.org/10.1016/0254-0584(88)90019-3	journal	January 1988
Surface complexation and precipitate geometry for aqueous Zn(II) sorption on ferrihydrite: II. XANES analysis and simulation Waychunas, G. A.; Fuller, C. C.; Davis, J. A. Geochimica et Cosmochimica Acta, Vol. 67, Issue 5 https://doi.org/10.1016/S0016-7037(02)01280-2	journal	March 2003
Isomerization of n-butane and of n-pentane in the presence of sulfated zirconia: formation of surface deposits investigated by in situ UV–vis diffuse reflectance spectroscopy Ahmad, Rafat; Melsheimer, Jörg; Jentoft, Friederike C. Journal of Catalysis, Vol. 218, Issue 2 https://doi.org/10.1016/S0021-9517(03)00144-1	journal	September 2003
Highly dispersed zinc oxide species on silica as active sites for photoepoxidation of propene by molecular oxygen Yoshida, H. Journal of Catalysis, Vol. 220, Issue 1 https://doi.org/10.1016/S0021-9517(03)00292-6	journal	November 2003
Environment of Ni, Co and Zn in low alkali borate glasses: information from EXAFS and XANES spectra Galoisy, Laurence; Cormier, Laurent; Calas, Georges Journal of Non-Crystalline Solids, Vol. 293-295 https://doi.org/10.1016/S0022-3093(01)00659-7	journal	November 2001
An X-ray absorption spectroscopic investigation of the nature of the zinc complex accumulated in Datura innoxia plant tissue culture Kelly, Rebekah A.; Andrews, Joy C.; DeWitt, Jane G. Microchemical Journal, Vol. 71, Issue 2-3 https://doi.org/10.1016/S0026-265X(02)00015-2	journal	April 2002
In situ X-ray absorption measurements of the Cu/MgO() interface Colonna, S.; Arciprete, F.; Balzarotti, A. Surface Science, Vol. 512, Issue 1-2 https://doi.org/10.1016/S0039-6028(02)01493-0	journal	June 2002
Adsorption of transition metal atoms on oxygen vacancies and regular sites of the MgO(001) surface Matveev, Alexei V.; Neyman, Konstantin M.; Yudanov, Ilya V. Surface Science, Vol. 426, Issue 1 https://doi.org/10.1016/S0039-6028(99)00327-1	journal	May 1999
Transformation of ethanol into 1,3-butadiene over magnesium oxide/silica catalysts Kvisle, S.; Aguero, A.; Sneeden, R. P. A. Applied Catalysis, Vol. 43, Issue 1 https://doi.org/10.1016/S0166-9834(00)80905-7	journal	January 1988
Formation of alkenyl carbenium ions by adsorption of cyclic precursors on zeolites Yang, Shuwu; Kondo, Junko N.; Domen, Kazunari Catalysis Today, Vol. 73, Issue 1-2 https://doi.org/10.1016/S0920-5861(01)00504-1	journal	April 2002
Dehydrogenation of ethanol over copper catalysts on rice husk ash prepared by incipient wetness impregnation Chang, Feg-Wen; Kuo, Wen-Yao; Lee, Kuen-Chan Applied Catalysis A: General, Vol. 246, Issue 2 https://doi.org/10.1016/S0926-860X(03)00050-4	journal	June 2003
Adsorption and Activation of NH3 during Selective Catalytic Reduction of NO by NH3 Liu, Qingya; Liu, Zhenyu; Li, Chengyue Chinese Journal of Catalysis, Vol. 27, Issue 7 https://doi.org/10.1016/S1872-2067(06)60035-1	journal	July 2006
Synthesis of Nanosized ZnO/MgO Solid and Its Catalytic Activity for CO Oxidation Didenko, Olga Z.; Kosmambetova, Gulnara R.; Strizhak, Peter E. Chinese Journal of Catalysis, Vol. 29, Issue 11 https://doi.org/10.1016/S1872-2067(09)60004-8	journal	November 2008
Ethanol dehydrogenation over copper catalysts on rice husk ash prepared by ion exchange Chang, Feg-Wen; Yang, Hsien-Chang; Roselin, L. Selva Applied Catalysis A: General, Vol. 304 https://doi.org/10.1016/j.apcata.2006.02.017	journal	May 2006
Ethanol dehydrogenation by gold catalysts: The effect of the gold particle size and the presence of oxygen Guan, Yejun; Hensen, Emiel J. M. Applied Catalysis A: General, Vol. 361, Issue 1-2 https://doi.org/10.1016/j.apcata.2009.03.033	journal	June 2009
Mechanistic study of ethanol conversion into butadiene over silver promoted zirconia catalysts Sushkevich, Vitaly L.; Ivanova, Irina I. Applied Catalysis B: Environmental, Vol. 215 https://doi.org/10.1016/j.apcatb.2017.05.060	journal	October 2017
Generalized molybdenum oxide surface chemical state XPS determination via informed amorphous sample model Baltrusaitis, Jonas; Mendoza-Sanchez, Beatriz; Fernandez, Vincent Applied Surface Science, Vol. 326 https://doi.org/10.1016/j.apsusc.2014.11.077	journal	January 2015
Potential of bioethanol as a chemical building block for biorefineries: Preliminary sustainability assessment of 12 bioethanol-based products Posada, John A.; Patel, Akshay D.; Roes, Alexander Bioresource Technology, Vol. 135 https://doi.org/10.1016/j.biortech.2012.09.058	journal	May 2013
One-step catalytic conversion of ethanol into 1,3-butadiene using zinc-containing talc Sekiguchi, Yasumasa; Akiyama, Sohta; Urakawa, Wataru Catalysis Communications, Vol. 68 https://doi.org/10.1016/j.catcom.2015.04.023	journal	August 2015
Cu–Mn mixed oxides for low temperature NO reduction with NH3 Kang, Min; Park, Eun Duck; Kim, Ji Man Catalysis Today, Vol. 111, Issue 3-4 https://doi.org/10.1016/j.cattod.2005.10.032	journal	February 2006
Catalytic study of the conversion of ethanol into 1,3-butadiene Makshina, E. V.; Janssens, W.; Sels, B. F. Catalysis Today, Vol. 198, Issue 1 https://doi.org/10.1016/j.cattod.2012.05.031	journal	December 2012
Conversion of ethanol to 1,3-butadiene over Na doped Zn Zr O mixed metal oxides Baylon, Rebecca A. L.; Sun, Junming; Wang, Yong Catalysis Today, Vol. 259 https://doi.org/10.1016/j.cattod.2015.04.010	journal	January 2016
XAS study of Zn-doped Al2O3 after thermal treatment Wang, Hsi-Chih; Wei, Yu-Ling; Yang, Yao-Wen Journal of Electron Spectroscopy and Related Phenomena, Vol. 144-147 https://doi.org/10.1016/j.elspec.2005.01.264	journal	June 2005
Evolution of carbonaceous deposits on H-mordenite and Pt-doped H-mordenite during n-butane conversion Wulfers, Matthew J.; Tzolova-Müller, Genka; Villegas, José Ignacio Journal of Catalysis, Vol. 296 https://doi.org/10.1016/j.jcat.2012.09.015	journal	December 2012
Catalytic conversion of ethanol to 1,3-butadiene on MgO: A comprehensive mechanism elucidation using DFT calculations Taifan, William E.; Bučko, Tomáš; Baltrusaitis, Jonas Journal of Catalysis, Vol. 346 https://doi.org/10.1016/j.jcat.2016.11.042	journal	February 2017
Electronic spectroscopy and methyl internal rotation dynamics of 9,10-dimethylanthracene Stepanenko, Y.; Sobolewski, A. L.; Mordziński, A. Journal of Molecular Spectroscopy, Vol. 233, Issue 1 https://doi.org/10.1016/j.jms.2005.05.011	journal	September 2005
In situ MAS NMR–UV/Vis investigation of H-SAPO-34 catalysts partially coked in the methanol-to-olefin conversion under continuous-flow conditions and of their regeneration Jiang, Yijiao; Huang, Jun; Reddy Marthala, V. R. Microporous and Mesoporous Materials, Vol. 105, Issue 1-2 https://doi.org/10.1016/j.micromeso.2007.05.028	journal	September 2007
Fe modified CuMnZrO2 catalysts for higher alcohols synthesis from syngas: Effect of calcination temperature Xu, Run; Wei, Wei; Li, Wen-huai Journal of Molecular Catalysis A: Chemical, Vol. 234, Issue 1-2 https://doi.org/10.1016/j.molcata.2005.01.048	journal	June 2005
Study of acetaldehyde condensation chemistry over magnesia and zirconia supported on silica Ordomsky, V. V.; Sushkevich, V. L.; Ivanova, I. I. Journal of Molecular Catalysis A: Chemical, Vol. 333, Issue 1-2 https://doi.org/10.1016/j.molcata.2010.10.001	journal	December 2010
Adsorption of single Ag and Cu atoms on regular and defective MgO(001) substrates: an ab initio study Zhukovskii, Yu. F.; Kotomin, E. A.; Borstel, G. Vacuum, Vol. 74, Issue 2 https://doi.org/10.1016/j.vacuum.2003.12.131	journal	May 2004
Cu and Cu-Based Nanoparticles: Synthesis and Applications in Catalysis Gawande, Manoj B.; Goswami, Anandarup; Felpin, François-Xavier Chemical Reviews, Vol. 116, Issue 6 https://doi.org/10.1021/acs.chemrev.5b00482	journal	March 2016
In Situ Spectroscopic Insights on the Molecular Structure of the MgO/SiO ₂ Catalytic Active Sites during Ethanol Conversion to 1,3-Butadiene Taifan, William E.; Baltrusaitis, Jonas The Journal of Physical Chemistry C, Vol. 122, Issue 36 https://doi.org/10.1021/acs.jpcc.8b06767	journal	August 2018
Bimetallic Zn and Hf on Silica Catalysts for the Conversion of Ethanol to 1,3-Butadiene De Baerdemaeker, Trees; Feyen, Mathias; Müller, Ulrich ACS Catalysis, Vol. 5, Issue 6 https://doi.org/10.1021/acscatal.5b00376	journal	May 2015
Ex Situ and Operando Studies on the Role of Copper in Cu-Promoted SiO ₂ –MgO Catalysts for the Lebedev Ethanol-to-Butadiene Process Angelici, Carlo; Meirer, Florian; van der Eerden, Ad M. J. ACS Catalysis, Vol. 5, Issue 10 https://doi.org/10.1021/acscatal.5b00755	journal	September 2015
With Open Arms: Open Sites of ZrBEA Zeolite Facilitate Selective Synthesis of Butadiene from Ethanol Sushkevich, Vitaly L.; Palagin, Dennis; Ivanova, Irina I. ACS Catalysis, Vol. 5, Issue 8 https://doi.org/10.1021/acscatal.5b01024	journal	July 2015
Role of Magnesium Silicates in Wet-Kneaded Silica–Magnesia Catalysts for the Lebedev Ethanol-to-Butadiene Process Chung, Sang-Ho; Angelici, Carlo; Hinterding, Stijn O. M. ACS Catalysis, Vol. 6, Issue 6 https://doi.org/10.1021/acscatal.5b02972	journal	May 2016
Mechanistic Study on the Lewis Acid Catalyzed Synthesis of 1,3-Butadiene over Ta-BEA Using Modulated Operando DRIFTS-MS Müller, Philipp; Burt, Samuel P.; Love, Alyssa M. ACS Catalysis, Vol. 6, Issue 10 https://doi.org/10.1021/acscatal.6b01642	journal	September 2016
Role of the Cu-ZrO ₂ Interfacial Sites for Conversion of Ethanol to Ethyl Acetate and Synthesis of Methanol from CO ₂ and H ₂ Ro, Insoo; Liu, Yifei; Ball, Madelyn R. ACS Catalysis, Vol. 6, Issue 10 https://doi.org/10.1021/acscatal.6b01805	journal	September 2016
Ethanol Conversion into 1,3-Butadiene by the Lebedev Method over MTaSiBEA Zeolites (M = Ag, Cu, Zn) Kyriienko, Pavlo I.; Larina, Olga V.; Soloviev, Sergiy O. ACS Sustainable Chemistry & Engineering, Vol. 5, Issue 3 https://doi.org/10.1021/acssuschemeng.6b01728	journal	January 2017
Generation, Characterization, and Transformations of Unsaturated Carbenium Ions in Zeolites Kiricsi, Imre; Förster, Horst; Tasi, Gyula Chemical Reviews, Vol. 99, Issue 8 https://doi.org/10.1021/cr9600767	journal	July 1999
The Role of Cyclopentadienium Ions in Methanol-to-Hydrocarbons Chemistry Wulfers, Matthew J.; Jentoft, Friederike C. ACS Catalysis, Vol. 4, Issue 10 https://doi.org/10.1021/cs500722m	journal	September 2014
Acetaldehyde: a chemical whose fortunes have changed Wittcoff, Harold A. Journal of Chemical Education, Vol. 60, Issue 12 https://doi.org/10.1021/ed060p1044	journal	December 1983
Infrared Characterization of Hydroxyl Groups on MgO: A Periodic and Cluster Density Functional Theory Study Chizallet, Céline; Costentin, Guylène; Che, Michel Journal of the American Chemical Society, Vol. 129, Issue 20 https://doi.org/10.1021/ja068720e	journal	April 2007
Interaction of SO ₂ with MgO(100) and Cu/MgO(100): Decomposition Reactions and the Formation of SO ₃ and SO ₄ Rodriguez, José A.; Jirsak, Tomas; Freitag, Andrea The Journal of Physical Chemistry B, Vol. 104, Issue 31 https://doi.org/10.1021/jp000806l	journal	August 2000
Relevance of the Drying Step in the Preparation by Impregnation of Zn/SiO₂ Supported Catalysts Chouillet, Cyril; Villain, Françoise; Kermarec, Maggy The Journal of Physical Chemistry B, Vol. 107, Issue 15 https://doi.org/10.1021/jp022481+	journal	March 2003
Ultraviolet–Visible Spectroscopy and Temperature-Programmed Techniques as Tools for Structural Characterization of Cu in CuMgAlO _x Mixed Metal Oxides Bravo-Suárez, Juan J.; Subramaniam, Bala; Chaudhari, Raghunath V. The Journal of Physical Chemistry C, Vol. 116, Issue 34 https://doi.org/10.1021/jp303631v	journal	August 2012
Pronounced catalytic activity and selectivity of MgO–SiO ₂ –Na ₂ O for synthesis of buta-1,3-diene from ethanol Ohnishi, Ryuichiro; Akimoto, Takao; Tanabe, Kozo J. Chem. Soc., Chem. Commun., Issue 22 https://doi.org/10.1039/C39850001613	journal	January 1985
Study on key step of 1,3-butadiene formation from ethanol on MgO/SiO ₂ Zhang, Minhua; Gao, Meixiang; Chen, Jianyue RSC Advances, Vol. 5, Issue 33 https://doi.org/10.1039/C4RA17070A	journal	January 2015
Experimental and computational studies of the roles of MgO and Zn in talc for the selective formation of 1,3-butadiene in the conversion of ethanol Hayashi, Yoshihiro; Akiyama, Sohta; Miyaji, Akimitsu Physical Chemistry Chemical Physics, Vol. 18, Issue 36 https://doi.org/10.1039/C6CP04171J	journal	January 2016
A DFT study on the aldol condensation reaction on MgO in the process of ethanol to 1,3-butadiene: understanding the structure–activity relationship Fan, Dan; Dong, Xiuqin; Yu, Yingzhe Physical Chemistry Chemical Physics, Vol. 19, Issue 37 https://doi.org/10.1039/C7CP04502F	journal	January 2017
Surface chemistry of MgO/SiO ₂ catalyst during the ethanol catalytic conversion to 1,3-butadiene: in-situ DRIFTS and DFT study Taifan, William E.; Yan, George X.; Baltrusaitis, Jonas Catalysis Science & Technology, Vol. 7, Issue 20 https://doi.org/10.1039/C7CY01556A	journal	January 2017
Parameter-free calculations of X-ray spectra with FEFF9 Rehr, John J.; Kas, Joshua J.; Vila, Fernando D. Physical Chemistry Chemical Physics, Vol. 12, Issue 21 https://doi.org/10.1039/b926434e	journal	January 2010
Investigations into the conversion of ethanol into 1,3-butadiene Jones, Matthew D.; Keir, Callum G.; Iulio, Carlo Di Catalysis Science & Technology, Vol. 1, Issue 2 https://doi.org/10.1039/c0cy00081g	journal	January 2011
Physicochemical properties of copper oxide loaded alumina in methane combustion Marion, Marie C.; Garbowski, Edouard; Primet, Michel Journal of the Chemical Society, Faraday Transactions, Vol. 86, Issue 17 https://doi.org/10.1039/ft9908603027	journal	January 1990
Supported nickel and copper clusters on MgO(100): A first‐principles calculation on the metal/oxide interface Pacchioni, Gianfranco; Rösch, Notker The Journal of Chemical Physics, Vol. 104, Issue 18 https://doi.org/10.1063/1.471400	journal	May 1996
First principles study of adsorbed Cun (n=1–4) microclusters on MgO(100): Structural and electronic properties Musolino, V.; Selloni, A.; Car, R. The Journal of Chemical Physics, Vol. 108, Issue 12 https://doi.org/10.1063/1.475911	journal	March 1998
Reaction of H2S with MgO(100) and Cu/MgO(100) surfaces: Band-gap size and chemical reactivity Rodriguez, José A.; Jirsak, Tomas; Chaturvedi, Sanjay The Journal of Chemical Physics, Vol. 111, Issue 17 https://doi.org/10.1063/1.480141	journal	November 1999
Catalysis by Gold Bond, Geoffrey C.; Thompson, David T. Catalysis Reviews, Vol. 41, Issue 3-4 https://doi.org/10.1081/CR-100101171	journal	January 1999
Cu K -edge x-ray-absorption spectroscopic study on the octahedrally coordinated trivalent copper in the perovskite-related compounds La 2 Li 0.5 Cu 0.5 O 4 and LaCuO 3 Choy, Jin-Ho; Kim, Dong-Kuk; Hwang, Sung-Ho Physical Review B, Vol. 50, Issue 22 https://doi.org/10.1103/PhysRevB.50.16631	journal	December 1994
Electronic absorption spectra of Cu 2 + in MgO : Ab initio theory and experiment Pascual, José Luis; Savoini, B.; González, R. Physical Review B, Vol. 70, Issue 4 https://doi.org/10.1103/PhysRevB.70.045109	journal	July 2004
Orientation-Dependent Local Structural Properties of Zn_1−xMgxO Nanorods Studied by Extended X-Ray Absorption Fine Structure Jeong, E. -S.; Park, Changin; Jin, Zhenlan Journal of Nanoscience and Nanotechnology, Vol. 13, Issue 3 https://doi.org/10.1166/jnn.2013.6966	journal	March 2013
Recent Breakthroughs in the Conversion of Ethanol to Butadiene Pomalaza, Guillaume; Capron, Mickaël; Ordomsky, Vitaly Catalysts, Vol. 6, Issue 12 https://doi.org/10.3390/catal6120203	journal	December 2016

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1
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Operando Structure Determination of Cu and Zn on Supported MgO/SiO2 Catalysts during Ethanol Conversion to 1,3-Butadiene

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Title: Operando Structure Determination of Cu and Zn on Supported MgO/SiO₂ Catalysts during Ethanol Conversion to 1,3-Butadiene