Silica-Supported Nanoscale Hydrotalcite-Derived Oxides for C4 Chemicals from Ethanol Condensation

Abstract

We demonstrated that the surface nature of nanoscale hydrotalcite-derived oxide (HTO) can be simply tailored through the addition of amorphous silica during the coprecipitation process of material preparation. The change in physical/chemical properties of the modified surface has been carefully scrutinized by a series of surface characterization techniques. The results showed that the HTO nanocomposite has molecular interactions with amorphous silica to form ternary Mg, Al, and Si interfaces, in accordance with enhancing chemically accessible aluminum (Al 3+ tetra ) as acidic sites. Moreover, the silica-supported HTO (HTO/SiO 2 -X) could catalyze ethanol condensation to foster C4 chemicals at 250 °C through the flow reactor. HTO with a strong basic nature promoted 1-butanol production (66% selectivity), while HTO/SiO 2 -5 with more well-distributed acidic sites favored 1,3-butadiene production (43% selectivity). This difference in catalytic performance could be attributed to the redistribution of acidic and basic sites upon the newly formed ternary interfaces, which could facilitate the surface-mediated Meerwein−Ponndorf−Verley (MPV) reduction reaction due to the relatively high ethanol affinity.

Zirconia Nanoparticles Uniformly Supported on Mesoporous Alumina–Carbon as a Highly Efficient Catalyst for the Direct Ethanol-to-Butadiene Reaction

“…The 27 Al MAS NMR spectra also provided more detailed information about the coordination structure of Al 3+ , as shown in Figure c. The sample exhibited three peaks at ∼10, ∼35, and ∼68 ppm, representing the Al 3+ ions in octahedral Al(VI), pentahedral Al(V), and tetrahedral Al(IV) coordination, respectively . After zirconia is loaded, the intensity of octahedral Al(VI) and tetrahedral Al(IV) is obviously weakened, which might indicate the interaction between zirconia and alumina.…”

“…The sample exhibited three peaks at ∼10, ∼35, and ∼68 ppm, representing the Al 3+ ions in octahedral Al(VI), pentahedral Al(V), and tetrahedral Al(IV) coordination, respectively. 48 After zirconia is loaded, the intensity of octahedral Al(VI) and tetrahedral Al(IV) is obviously weakened, which might indicate the interaction between zirconia and alumina. Obtained from the XRD results, the zirconia−alumina solid solution could be formed after loading zirconia; therefore, the interaction between zirconia and alumina may lead to a change in peak intensity.…”