Impact of Particle Size on the Vapor-Phase Oxidative Coupling of Methanol and Dimethylamine over Palladium–Gold Nanoparticles

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

doi:10.1021/acscatal.4c05022

Impact of Particle Size on the Vapor-Phase Oxidative Coupling of Methanol and Dimethylamine over Palladium–Gold Nanoparticles

Journal Article · Thu Nov 07 00:00:00 EST 2024 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.4c05022· OSTI ID:2481337

Minne, Alexander P. ^[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)

Oxidative coupling of methanol and dimethylamine in the presence of O₂ in the vapor phase over dilute Pd in Au bimetallic catalysts occurs via the dissociation of O₂ on Pd and selective oxidation of methanol on Au. Here, we synthesize a series of silica-supported PdAu alloy nanoparticle catalysts of varied Pd:Au ratios with ~5 nm particle diameter and show that these catalysts have increased selectivity to dimethylformamide across all Pd:Au ratios (~95%), distinct from observations over larger PdAu nanoparticles (~15–25 nm diameter) of similar Pd:Au ratios. Small monometallic Pd particles are more selective than large monometallic Pd particles, and small Au nanoparticles are reactive and selective for oxidative coupling (while large Au nanoparticles are inactive). Rates per surface metal atom were similar over PdAu nanoparticles of all sizes and increased monotonically with increasing Pd content for the small nanoparticles. Further, apparent reaction kinetics demonstrate distinct apparent methanol reaction order and apparent activation energy relative to those reported over larger nanoparticles of similar Pd:Au ratios. Unlike larger PdAu nanoparticles, the rate of dimethylformamide formation is not promoted by cofed water over small PdAu nanoparticles. The results of the kinetic studies are used to propose a series of elementary steps, derive a plausible rate expression, and regress rate and equilibrium constants. These results suggest high coverages of surface methoxy species and low coverages of adsorbates derived from dimethylamine. Taken together, these results demonstrate the sensitivity of the rates, selectivities, and kinetics of oxidative coupling reactions to the size of bimetallic nanoparticles.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

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

OSTI ID:: 2481337

Report Number(s):: BNL--226401-2024-JAAM

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 23 Vol. 14; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Impact of Particle Size on the Vapor-Phase Oxidative Coupling of Methanol and Dimethylamine over Palladium–Gold Nanoparticles

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