Dilute Pd-in-Au alloy RCT-SiO2 catalysts for enhanced oxidative methanol coupling

Filie, Amanda; Shirman, Tanya; Foucher, Alexandre C.; Stach, Eric A.; Aizenberg, Michael; Aizenberg, Joanna; Friend, Cynthia M.; Madix, Robert J.

doi:10.1016/j.jcat.2021.06.003

Dilute Pd-in-Au alloy RCT-SiO₂ catalysts for enhanced oxidative methanol coupling

Journal Article · Wed Jun 09 04:00:00 EDT 2021 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2021.06.003· OSTI ID:1977245

^[1]; Shirman, Tanya ^[2]; Foucher, Alexandre C. ^[3]; ^[3]; Aizenberg, Michael ^[2]; Aizenberg, Joanna ^[2]; Friend, Cynthia M. ^[2]; Madix, Robert J. ^[2]

Harvard Univ., Cambridge, MA (United States); OSTI
Harvard Univ., Cambridge, MA (United States)
Univ. of Pennsylvania, Philadelphia, PA (United States)

Dilute alloy catalysts have the potential to enhance selectivity and activity for large-scale reactions. Highly dilute Pd-in-Au nanoparticle alloys partially embedded in porous silica (“raspberry colloid templated” (RCT)-SiO₂) prove to be robust and selective catalysts for oxidative coupling of methanol. Palladium concentrations in the bimetallic nanoparticles as low as ~3.4 at.% catalyze the production of methyl formate with a selectivity of ~95% at conversions of ~55%, whereas conversions are low (<10%) for ~1.7 at.% Pd-in-Au nanoparticle and pure Au nanoparticle catalysts. Fractional reaction orders for both CH₃OH and O₂ measured for ~3.4 at.% Pd-in-Au nanoparticles supported on RCT-SiO₂ indicated a complex mechanism in which the sites for O₂ dissociation are not saturated. Optimal methyl formate production was found for an equimolar mixture. There is no conversion of methanol in the absence of O₂ between 360 and 450 K. Finally, all observations are consistent with a mechanism derived from model studies, requiring that clusters of Pd be available on the catalyst for O₂ dissociation.

View Accepted Manuscript (DOE)

Research Organization:: Harvard Univ., Cambridge, MA (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:: SC0012573

OSTI ID:: 1977245

Alternate ID(s):: OSTI ID: 1836130

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Journal Issue: C Vol. 404; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Dilute Pd-in-Au alloy RCT-SiO2 catalysts for enhanced oxidative methanol coupling

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