Catalyst design for enhanced sustainability through fundamental surface chemistry

Personick, Michelle L.; Montemore, Matthew M.; Kaxiras, Efthimios; Madix, Robert J.; Biener, Juergen; Friend, Cynthia M.

doi:10.1098/rsta.2015.0077

Title: Catalyst design for enhanced sustainability through fundamental surface chemistry

Journal Article · Mon Jan 11 00:00:00 EST 2016 · Philosophical Transactions of the Royal Society. A, Mathematical, Physical and Engineering Sciences

DOI:https://doi.org/10.1098/rsta.2015.0077· OSTI ID:1251068

Personick, Michelle L. ^[1]; Montemore, Matthew M. ^[2]; Kaxiras, Efthimios ^[2]; Madix, Robert J. ^[2]; Biener, Juergen ^[3]; Friend, Cynthia M. ^[4]

Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology
Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nanoscale Synthesis and Characterization Lab.
Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology. School of Engineering and Applied Sciences

Decreasing energy consumption in the production of platform chemicals is necessary to improve the sustainability of the chemical industry, which is the largest consumer of delivered energy. The majority of industrial chemical transformations rely on catalysts, and therefore designing new materials that catalyse the production of important chemicals via more selective and energy-efficient processes is a promising pathway to reducing energy use by the chemical industry. Efficiently designing new catalysts benefits from an integrated approach involving fundamental experimental studies and theoretical modelling in addition to evaluation of materials under working catalytic conditions. In this paper, we outline this approach in the context of a particular catalyst—nanoporous gold (npAu)—which is an unsupported, dilute AgAu alloy catalyst that is highly active for the selective oxidative transformation of alcohols. Fundamental surface science studies on Au single crystals and AgAu thin-film alloys in combination with theoretical modelling were used to identify the principles which define the reactivity of npAu and subsequently enabled prediction of new reactive pathways on this material. Specifically, weak van der Waals interactions are key to the selectivity of Au materials, including npAu. Finally, we also briefly describe other systems in which this integrated approach was applied.

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Research Organization:: Harvard Univ., Cambridge, MA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC)

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

Grant/Contract Number:: AC52-07NA27344; SC0012573

OSTI ID:: 1251068

Report Number(s):: LLNL-JRNL-675456

Journal Information:: Philosophical Transactions of the Royal Society. A, Mathematical, Physical and Engineering Sciences, Vol. 374, Issue 2061; ISSN 1364-503X

Publisher:: The Royal Society PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica Shirman, Tanya; Lattimer, Judith; Luneau, Mathilde Chemistry - A European Journal, Vol. 24, Issue 8 https://doi.org/10.1002/chem.201704552	journal	November 2017
New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica Shirman, Tanya; Lattimer, Judith; Luneau, Mathilde Chemistry - A European Journal, Vol. 24, Issue 8 https://doi.org/10.1002/chem.201705514	journal	November 2017
O ₂ Activation by Metal Surfaces: Implications for Bonding and Reactivity on Heterogeneous Catalysts Montemore, Matthew M.; van Spronsen, Matthijs A.; Madix, Robert J. Chemical Reviews, Vol. 118, Issue 5 https://doi.org/10.1021/acs.chemrev.7b00217	journal	November 2017

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE
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