Tailoring the Surface Structure of Silicon Carbide Support for Copper Catalyzed Ethanol Dehydrogenation

Abstract

The production of acetaldehyde through biomass‐derived ethanol dehydrogenation is a sustainable alternative compared to the fossil‐feedstock based process, for which Cu‐based catalysts are considered to be the most efficient. Herein, we modified the surface of silicon carbide (SiC) to alter the properties of the interface from SiO2‐rich to C‐rich, and we prepared a series of Cu‐supported catalysts (Cu/SiC, Cu/SiO2/SiC, and Cu/C/SiC) with the aim of insight into the effect of the interface structure and composition on catalytic dehydrogenation of ethanol. At 280 °C, the Cu/SiO2/SiC catalyst exhibits high ethanol conversion due to the excellent dispersion of Cu nanoparticles promoted by SiO2‐rich interface. In contrast, Cu nanoparticles dispersed on C/SiC shows somewhat lower activity but excellent acetaldehyde selectivity with trace amounts of by‐products under identical reaction conditions. This difference is attributed to the fast removal of acetaldehyde because of its low affinity for the relatively inert C‐rich interface (C/SiC). This work provides an in‐depth understanding of Cu−Si−C multi‐interfacial structure and the ethanol dehydrogenation behavior, which may shed light on the design of novel catalysts with tailored interfacial structures.

Ethanol Dehydrogenation: A Reaction Path Study by Means of Temporal Analysis of Products

“…This discrepancy might be due to the ultra-high vacuum reaction conditions of the TAP experiments in this work. shown in Figure 10b, is in contrast to the experimental results of many papers in the literature working with Cu catalysts, which report on high selectivities towards acetaldehyde of in parts 100% [17,19,21,23,25]. This discrepancy might be due to the ultra-high vacuum reaction conditions of the TAP experiments in this work.…”

“…Many research groups have found Cu catalysts to be highly active for ethanol dehydrogenation, revealing selectivities towards acetaldehyde of almost 100% in some cases [16][17][18][19][20][21][22][23][24][25]. A positive effect is reported when the Cu content increased in the range of 1-5 wt % [26].…”

Atomic Carbon Layers Supported Pt Nanoparticles for Minimized CO Poisoning and Maximized Methanol Oxidation

“…By these treatments, the residual carbon and SiO 2 generated on the surface of SiC NPs were removed. The in situ formation of atomic carbon layers on the surface of SiC NPs was conducted by dry etching with CCl 4 gas where surface silica atoms were selectively etched . Such a process is schematically shown in Scheme S1 (Supporting Information).…”

Stabilizing copper species using zeolite for ethanol catalytic dehydrogenation to acetaldehyde

“…A good support should ensure a suitable dispersion of the Cu active phase, possibly stabilizing it during the high-temperature reaction [28]. Inert SiO2 [11,12], mesoporous carbon [13], silicon carbide [29], and carbon layer-coated SiO2 [15] as well as rice husk ash [17] have already been tested as candidate supports.…”