Selectivity of Synthesis Gas Conversion to C2+ Oxygenates on fcc(111) Transition-Metal Surfaces

Schumann, Julia; Medford, Andrew J.; Yoo, Jong Suk; Zhao, Zhi -Jian; Bothra, Pallavi; Cao, Ang; Studt, Felix; Abild-Pedersen, Frank; Norskov, Jens K.

doi:10.1021/acscatal.8b00201

Selectivity of Synthesis Gas Conversion to C₂₊ Oxygenates on fcc(111) Transition-Metal Surfaces

Journal Article · Tue Mar 13 00:00:00 EDT 2018 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.8b00201· OSTI ID:1457170

^[1]; ^[2]; ^[3]; Zhao, Zhi -Jian ^[4]; Bothra, Pallavi ^[1]; Cao, Ang ^[5]; Studt, Felix ^[6]; ^[7]; Norskov, Jens K. ^[1]

Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); Georgia Inst. of Technology, Atlanta, GA (United States)
Stanford Univ., Stanford, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); Tianjin Univ., Tianjin (China)
Stanford Univ., Stanford, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Karlsruhe Institute of Technology, Karlsruhe (Germany)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

Using a combined density functional theory and descriptor based microkinetic model approach, we predict production rate volcanos for higher oxygenate formation on (111) transition-metal surfaces. Despite their lower activity for CO conversion compared to stepped surfaces, (111) transition metal surfaces bring the potential for selectivity toward C₂₊ oxygenates. As a result, the volcano plots can be used to rationalize and predict activity and selectivity trends for transition-metal-based catalysts.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

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

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1457170

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 4 Vol. 8; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (29)

Design and Synthesis of Copper-Cobalt Catalysts for the Selective Conversion of Synthesis Gas to Ethanol and Higher Alcohols Prieto, Gonzalo; Beijer, Steven; Smith, Miranda L. Angewandte Chemie International Edition, Vol. 53, Issue 25 https://doi.org/10.1002/anie.201402680	journal	May 2014
CO ₂ Recycling: A Key Strategy to Introduce Green Energy in the Chemical Production Chain Perathoner, Siglinda; Centi, Gabriele ChemSusChem, Vol. 7, Issue 5 https://doi.org/10.1002/cssc.201300926	journal	March 2014
High Pressure CO Hydrogenation Over Bimetallic Pt–Co Catalysts Christensen, Jakob M.; Medford, Andrew J.; Studt, Felix Catalysis Letters, Vol. 144, Issue 5 https://doi.org/10.1007/s10562-014-1220-x	journal	March 2014
CatMAP: A Software Package for Descriptor-Based Microkinetic Mapping of Catalytic Trends Medford, Andrew J.; Shi, Chuan; Hoffmann, Max J. Catalysis Letters, Vol. 145, Issue 3 https://doi.org/10.1007/s10562-015-1495-6	journal	February 2015
Discovery of technical methanation catalysts based on computational screening Sehested, Jens; Larsen, Kasper Emil; Kustov, Arkady L. Topics in Catalysis, Vol. 45, Issue 1-4 https://doi.org/10.1007/s11244-007-0232-9	journal	August 2007
Activity and Selectivity Trends in Synthesis Gas Conversion to Higher Alcohols Medford, Andrew J.; Lausche, Adam C.; Abild-Pedersen, Frank Topics in Catalysis, Vol. 57, Issue 1-4 https://doi.org/10.1007/s11244-013-0169-0	journal	October 2013
Synthesis of higher alcohols by Fischer–Tropsch synthesis over alkali metal-modified cobalt catalysts Ishida, Tamao; Yanagihara, Tatsuya; Liu, Xiaohao Applied Catalysis A: General, Vol. 458 https://doi.org/10.1016/j.apcata.2013.03.042	journal	May 2013
Fe-promotion of supported Rh catalysts for direct conversion of syngas to ethanol Haider, M.; Gogate, M.; Davis, R. Journal of Catalysis, Vol. 261, Issue 1 https://doi.org/10.1016/j.jcat.2008.10.013	journal	January 2009
Effect of multiscale model uncertainty on identification of optimal catalyst properties Ulissi, Z.; Prasad, V.; Vlachos, D. G. Journal of Catalysis, Vol. 281, Issue 2 https://doi.org/10.1016/j.jcat.2011.05.019	journal	July 2011
On the effect of coverage-dependent adsorbate–adsorbate interactions for CO methanation on transition metal surfaces Lausche, Adam C.; Medford, Andrew J.; Khan, Tuhin Suvra Journal of Catalysis, Vol. 307 https://doi.org/10.1016/j.jcat.2013.08.002	journal	November 2013
Effect of errors in linear scaling relations and Brønsted–Evans–Polanyi relations on activity and selectivity maps Sutton, Jonathan E.; Vlachos, Dionisios G. Journal of Catalysis, Vol. 338 https://doi.org/10.1016/j.jcat.2016.03.013	journal	June 2016
Role of ZrO ₂ in Promoting the Activity and Selectivity of Co-Based Fischer–Tropsch Synthesis Catalysts Johnson, Gregory R.; Bell, Alexis T. ACS Catalysis, Vol. 6, Issue 1 https://doi.org/10.1021/acscatal.5b02205	journal	December 2015
Effects of Sodium on the Catalytic Performance of CoMn Catalysts for Fischer–Tropsch to Olefin Reactions Li, Zhengjia; Zhong, Liangshu; Yu, Fei ACS Catalysis, Vol. 7, Issue 5 https://doi.org/10.1021/acscatal.6b03478	journal	April 2017
Adsorption Energy Correlations at the Metal–Support Boundary Mehta, Prateek; Greeley, Jeffrey; Delgass, W. Nicholas ACS Catalysis, Vol. 7, Issue 7 https://doi.org/10.1021/acscatal.7b00979	journal	June 2017
A Review of Recent Literature to Search for an Efficient Catalytic Process for the Conversion of Syngas to Ethanol Subramani, Velu; Gangwal, Santosh K. Energy & Fuels, Vol. 22, Issue 2 https://doi.org/10.1021/ef700411x	journal	March 2008
Intrinsic Selectivity and Structure Sensitivity of Rhodium Catalysts for C ₂₊ Oxygenate Production Yang, Nuoya; Medford, Andrew J.; Liu, Xinyan Journal of the American Chemical Society, Vol. 138, Issue 11 https://doi.org/10.1021/jacs.5b12087	journal	March 2016
CO Adsorption Behavior of Cu/SiO ₂ , Co/SiO ₂ , and CuCo/SiO ₂ Catalysts Studied by in Situ DRIFTS Smith, Miranda L.; Kumar, Nitin; Spivey, James J. The Journal of Physical Chemistry C, Vol. 116, Issue 14 https://doi.org/10.1021/jp301197s	journal	March 2012
CO Hydrogenation on Pd(111): Competition between Fischer–Tropsch and Oxygenate Synthesis Pathways Lin, Sen; Ma, Jianyi; Ye, Xinxin The Journal of Physical Chemistry C, Vol. 117, Issue 28 https://doi.org/10.1021/jp404509v	journal	July 2013
Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol Studt, Felix; Sharafutdinov, Irek; Abild-Pedersen, Frank Nature Chemistry, Vol. 6, Issue 4 https://doi.org/10.1038/nchem.1873	journal	March 2014
Effects of correlated parameters and uncertainty in electronic-structure-based chemical kinetic modelling Sutton, Jonathan E.; Guo, Wei; Katsoulakis, Markos A. Nature Chemistry, Vol. 8, Issue 4 https://doi.org/10.1038/nchem.2454	journal	February 2016
Alloy catalysts designed from first principles Greeley, Jeff; Mavrikakis, Manos Nature Materials, Vol. 3, Issue 11 https://doi.org/10.1038/nmat1223	journal	October 2004
Status and prospects in higher alcohols synthesis from syngas Luk, Ho Ting; Mondelli, Cecilia; Ferré, Daniel Curulla Chemical Society Reviews, Vol. 46, Issue 5 https://doi.org/10.1039/C6CS00324A	journal	January 2017
Heterogeneous catalytic synthesis of ethanol from biomass-derived syngas Spivey, James J.; Egbebi, Adefemi Chemical Society Reviews, Vol. 36, Issue 9 https://doi.org/10.1039/b414039g	journal	January 2007
Perspective on density functional theory Burke, Kieron The Journal of Chemical Physics, Vol. 136, Issue 15 https://doi.org/10.1063/1.4704546	journal	April 2012
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
Density functionals for surface science: Exchange-correlation model development with Bayesian error estimation Wellendorff, Jess; Lundgaard, Keld T.; Møgelhøj, Andreas Physical Review B, Vol. 85, Issue 23 https://doi.org/10.1103/PhysRevB.85.235149	journal	June 2012
Scaling Properties of Adsorption Energies for Hydrogen-Containing Molecules on Transition-Metal Surfaces Abild-Pedersen, F.; Greeley, J.; Studt, F. Physical Review Letters, Vol. 99, Issue 1 https://doi.org/10.1103/PhysRevLett.99.016105	journal	July 2007
Assessing the reliability of calculated catalytic ammonia synthesis rates Medford, A. J.; Wellendorff, J.; Vojvodic, A. Science, Vol. 345, Issue 6193 https://doi.org/10.1126/science.1253486	journal	July 2014
EFFECT OF METAL DISPERSION ON THE ACTIVITY AND SELECTIVITY OF Rh/SiO ₂ CATALYST FOR HIGH PRESSURE CO HYDROGENATION Arakawa, Hironori; Takeuchi, Kazuhiko; Matsuzaki, Takehiko Chemistry Letters, Vol. 13, Issue 9 https://doi.org/10.1246/cl.1984.1607	journal	September 1984

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High-throughput calculations of catalytic properties of bimetallic alloy surfaces Mamun, Osman; Winther, Kirsten T.; Boes, Jacob R. Scientific Data, Vol. 6, Issue 1 https://doi.org/10.1038/s41597-019-0080-z	journal	May 2019
Catalysis-Hub.org, an open electronic structure database for surface reactions Winther, Kirsten T.; Hoffmann, Max J.; Boes, Jacob R. Scientific Data, Vol. 6, Issue 1 https://doi.org/10.1038/s41597-019-0081-y	journal	May 2019
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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalyst design
density functional theory
heterogeneous catalysis
higher alcohol synthesis
microkinetic modeling
probability
syngas conversion