Effect of nanoscale flows on the surface structure of nanoporous catalysts

Montemore, Matthew M.; Montessori, Andrea; Succi, Sauro; Barroo, Cédric; Falcucci, Giacomo; Bell, David C.; Kaxiras, Efthimios

doi:10.1063/1.4984614

Title: Effect of nanoscale flows on the surface structure of nanoporous catalysts

Journal Article · Thu Jun 01 00:00:00 EDT 2017 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4984614· OSTI ID:1388894

^[1]; Montessori, Andrea ^[2];

^[3];

^[1];

^[4]; Bell, David C. ^[5]; Kaxiras, Efthimios ^[1]

Harvard Univ., Cambridge, MA (United States)
Univ. of Rome “Roma Tre,” Rome (Italy)
Harvard Univ., Cambridge, MA (United States); Istituto per le Applicazioni del Calcolo - CNR, Rome (Italy)
Harvard Univ., Cambridge, MA (United States); Univ. of Rome "Tor Vergata", Rome (Italy)
Harvard Univ., Cambridge, MA (United States); Center for Nanoscale Systems, Cambridge, MA (United States)

Here, the surface structure and composition of a multi-component catalyst are critical factors in determining its catalytic performance. The surface composition can depend on the local pressure of the reacting species, leading to the possibility that the flow through a nanoporous catalyst can affect its structure and reactivity. Here, we explore this possibility for oxidation reactions on nanoporous gold, an AgAu bimetallic catalyst. We use microscopy and digital reconstruction to obtain the morphology of a two-dimensional slice of a nanoporous gold sample. Using lattice Boltzmann fluid dynamics simulations along with thermodynamic models based on first-principles total-energy calculations, we show that some sections of this sample have low local O₂ partial pressures when exposed to reaction conditions, which leads to a pure Au surface in these regions, instead of the active bimetallic AgAu phase. We also explore the effect of temperature on the surface structure and find that moderate temperatures (≈300–450 K) should result in the highest intrinsic catalytic performance, in apparent agreement with experimental results.

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Research Organization:: Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC)

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

Grant/Contract Number:: SC0012573

OSTI ID:: 1388894

Alternate ID(s):: OSTI ID: 1365429

Journal Information:: Journal of Chemical Physics, Vol. 146, Issue 21; Related Information: IMASC partners with Harvard University (lead); Fritz Haber Institute; Lawrence Berkeley National Laboratory; Lawrence Livermore National Laboratory; University of Kansas; Tufts University; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 21 works

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