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Titanium-anchored gold on silica for enhanced catalytic activity in aqueous ethanol oxidation

DOI: 10.1021/acs.iecr.0c02939 DOI Help

Authors: Sotiria Mostrou (ETH Zürich) , Mark Newton (ETH Zürich) , Andreas Tarcevski (ETH Zürich) , Andreas Nagl (TU Wien) , Karin Foettinger (TU Wien) , Jeroen A. Van Bokhoven (ETH Zürich)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Industrial & Engineering Chemistry Research

State: Published (Approved)
Published: December 2020

Open Access Open Access

Abstract: The heterogeneously catalyzed oxidation of bioethanol offers a promising route to bio-based acetic acid. Here, we assess an alternative method to support gold nanoparticles, which aims to improve selectivity to acetic acid through minimizing over-oxidation to carbon dioxide. The most promising support system is 5 wt % titanium on silica, which combines the high surface area of silica with the stabilizing effect of titania on the gold particles. Compared to gold–silica systems, which require a complex synthesis method, small quantities of titanium promoted the formation of gold nanoparticles during a simple deposition–precipitation. Characterization of the catalyst with X-ray absorption spectroscopy shows that titanium is highly dispersed in the form of small, possibly dimeric, titanium(IV) structures, which are isolated and stabilize gold nanoparticles, possibly minimizing sintering effects during synthesis. The size of the gold particles depends on the pre-treatment of the titanium–silica support before gold deposition, with larger titanium structures hosting larger gold particles. Acetic acid yield over the titanium–silica-supported gold systems improved by about 1.6 times, compared to pure titania-supported gold. The high activity of those catalysts suggests that bulk, crystalline titania is not required for the reaction, encouraging the use of mixed supports to combine their benefits. Those support systems, besides improving selectivity, offer high surface area and a low-cost filler material, which brings ethanol oxidation one step further to the industry. Additionally, the low loading of titanium permits studying the reaction mechanisms on the gold–titanium interface with bulk characterization techniques.

Journal Keywords: Catalysts; Oxides; Titanium; Gold; Silica

Subject Areas: Chemistry

Instruments: I20-Scanning-X-ray spectroscopy (XAS/XES)

Added On: 14/12/2020 09:19

Discipline Tags:

Physical Chemistry Catalysis Chemistry Inorganic Chemistry Organic Chemistry Nanoscience/Nanotechnology

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS)