Plasma-Enabled Ligand Removal for Improved Catalysis: Furfural Conversion on Pd/SiO2

Abstract
A nonthermal, atmospheric He/O2 plasma (NTAP) successfully removed polyvinylpyrrolidone (PVP) from Pd cubic nanoparticles supported on SiO2 quickly and controllably. Transmission electron microscopy (TEM) revealed that the shape and size of Pd nanoparticles remain intact during plasma treatment, unlike mild calcination, which causes sintering and polycrystallinity. Using Fourier transform infrared (FTIR) spectroscopy and X-ray photoelectron spectroscopy (XPS), we demonstrate the quantitative estimation of the PVP plasma removal rate and control of the nanoparticle synthesis. First-principles calculations of the XPS and CO FTIR spectra elucidate electron transfer from the ligand to the metal and allow for estimates of ligand coverages. Reactivity testing indicated that PVP surface crowding inhibits furfural conversion but does not alter furfural selectivity. Overall, the data demonstrate NTAP as a more efficient method than traditional calcination for organic ligand removal in nanoparticle synthesis.
Description
This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Nano, copyright © 2023 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsnano.3c06310. This article will be embargoed until 11/14/2024.
Keywords
ligand coverage, nonthermal atmospheric plasma, PVP removal, metal nanoparticles, catalysis
Citation
Nguyen, Darien K., Vibin Vargheese, Vinson Liao, Panagiotis Dimitrakellis, Sagar Sourav, Weiqing Zheng, and Dionisios G. Vlachos. “Plasma-Enabled Ligand Removal for Improved Catalysis: Furfural Conversion on Pd/SiO 2.” ACS Nano 17, no. 21 (November 14, 2023): 21480–92. https://doi.org/10.1021/acsnano.3c06310.