NiAu single atom alloys for the selective oxidation of methacrolein with methanol to methyl methacrylate

Trimpalis, Antonios; Giannakakis, Georgios; Cao, Sufeng; Flytzani-Stephanopoulos, Maria

doi:10.1016/j.cattod.2019.04.021

NiAu single atom alloys for the selective oxidation of methacrolein with methanol to methyl methacrylate

Journal Article · Mon Apr 08 00:00:00 EDT 2019 · Catalysis Today

DOI:https://doi.org/10.1016/j.cattod.2019.04.021· OSTI ID:1595093

Trimpalis, Antonios ^[1]; Giannakakis, Georgios ^[2]; Cao, Sufeng ^[2]; Flytzani-Stephanopoulos, Maria ^[2]

Tufts Univ., Medford, MA (United States); Harvard University
Tufts Univ., Medford, MA (United States)

In this work, the oxidative cross-coupling of unsaturated aldehydes and alcohols with methanol is catalyzed by O-activated gold surfaces in both ambient pressure and UHV conditions. From liquid-phase studies it has been found that either the addition of a base or the use of a basic support is necessary for high yields of the corresponding methyl ester. Here we demonstrate that addition of a small amount of Ni, at the single atom limit, on supported Au nanoparticles, without the aid of a base in the reaction solution or the use of a basic support, is sufficient to activate Au for the selective oxidative esterification of methacrolein with methanol. The Ni concentration and dispersion are followed by ICP-AES and in situ DRIFTS, respectively. The active site appears to be the same for both NiAu and Au NPs; namely, an [Au-O_x]- species, as similar apparent activation energies of the reaction were found in kinetic studies over these two catalysts. Ni was also shown to allow for lower methanol concentrations to be used without affecting the catalytic activity and selectivity to the desired product, methyl methacrylate. In situ vibrational spectroscopy studies were conducted in an ATR-IR cell, where the reaction progress was monitored by detecting the gradual conversion of adsorbed reactants on the catalytic surface to intermediates and finally to the desired product, which was produced at close to 100% selectivity at conversions exceeding 25% at 60 C on NiAu single atom alloy nanoparticles.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: SC0012573

OSTI ID:: 1595093

Alternate ID(s):: OSTI ID: 1681077

Journal Information:: Catalysis Today, Journal Name: Catalysis Today Vol. 355; ISSN 0920-5861

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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