Promoting the oxidative coupling of methanol and dimethylamine using group 1 alkali metals on palladium-gold nanoparticles

Minne, Alexander P.; Garton, Treycen D.; Iaia, Ethan P.; Stavitski, Eli; Harris, James W.

doi:10.1016/j.apcatb.2025.125533

Promoting the oxidative coupling of methanol and dimethylamine using group 1 alkali metals on palladium-gold nanoparticles

Journal Article · Mon May 26 00:00:00 EDT 2025 · Applied Catalysis. B, Environmental

DOI:https://doi.org/10.1016/j.apcatb.2025.125533· OSTI ID:2570586

^[1]; Garton, Treycen D. ^[1]; Iaia, Ethan P. ^[1]; ^[2]; ^[1]

Univ. of Alabama, Tuscaloosa, AL (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

PdAu/SiO₂ catalysts were synthesized by strong electrostatic adsorption (SEA) and characterized by TEM, DRIFTS, XRD, XAS, and O₂-TPD. The use of group 1 alkali salt solutions to control pH during SEA syntheses led to uptake of alkali metals observed reductions in the densities of terminal silanol groups of the SiO₂ support. In the absence of alkali metals, PdAu/SiO₂ catalyzes oxidative C-N bond formation between methanol and dimethylamine (DMA), yielding dimethylformamide (DMF) with ∼95 % carbon selectivity (CO₂ ∼5 %) at temperatures below 413 K. When Na, K, and Cs were present on the catalyst, methyl formate (MF) and tetramethylurea (TMU) were observed as additional products (combined ∼30 % carbon selectivity) while only TMU was detected for the Li-promoted catalyst. Total coupling product rate increased for promoted samples in the order Li < Na < Cs < K, and the apparent kinetics over the Cs-promoted catalyst were distinct from those over the alkali-free catalyst as the apparent reaction order with respect to DMA decreased and the apparent activation energy increased. Finally, this work demonstrates the sensitivity of oxidative coupling reactions to alkali metal promoters and the opportunity to achieve alkali promotion of metal catalysts during SEA synthesis.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

Grant/Contract Number:: AC02-76SF00515; SC0012704

OSTI ID:: 2570586

Report Number(s):: BNL--228370-2025-JAAM

Journal Information:: Applied Catalysis. B, Environmental, Journal Name: Applied Catalysis. B, Environmental Vol. 378; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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