In this work, manganese well-dispersed
on Fe3O4 microsphere (Mn–Fe3O4) catalyst was
synthesized. It exhibited excellent catalytic performance for the
direct conversion of carbon dioxide (CO2) into light olefins.
A CO2 conversion of 44.7% with high selectivity of light
olefin (46.2%, yield of 18.7%), high O/P ratio (6.5), and low selectivity
of CO (9.4%) was obtained over the 10Mn–Fe3O4 catalyst. The Mn–Fe3O4 catalyst
was studied by XRD, SEM, (HR)TEM, STEM–EDS, H2-TPR,
and CO2-TPD. The result indicated that the manganese promoter
could facilitate the adsorption of CO2 and the activation
of CO bonds as well as inhibit the secondary hydrogenation.
This work offered a novel Fe-based catalyst system to the utilization
of CO2 and an understanding in promoting CO bond
activation in the first step of CO2 hydrogenation to hydrocarbon
reaction.
Efficient and one-pot conversion of biomass-derived carbohydrate into highly value-added 5-hydroxymethylfurfural (HMF) is a crucial reaction step for the valorization of biomass resources toward bio-based chemicals and fuels. In this work, a series of Sn/SAPO-34 catalysts were prepared through impregnation and evaluated in glucose conversion to HMF. The physicochemical properties of Sn/SAPO-34 catalysts were systematically characterized by SEM, XRD, N 2 physisorption, XPS, solid-state 119 Sn, 29 Si, and 31 P NMR, XRF, UV−vis, NH 3 -TPD, and pyridine-FTIR techniques. It was demonstrated that controlling the Sn loading amount could facilely adjust the acid strength and acid amount of the SAPO-34 zeolite. The incorporation of Sn species could induce the formation of a tetrahedrally coordinated Sn 4+ site and Sn-OH site to improve the amounts of Brønsted and Lewis acid sites of the catalyst. However, modification with sufficiently high Sn loading could decrease the acid strength and performance of the catalyst owing to its structure damage. The 5%Sn/SAPO-34 catalyst (i.e., Sn loading calculated based on the mass ratio of SnCl 4 • 5H 2 O as a precursor to the parent SAPO-34) was found to exhibit the superior catalytic performance under mild conditions and could afford an HMF yield of 64.4% at 98.5% glucose conversion in a biphasic 35 wt % NaCl-H 2 O/tetrahydrofuran (THF) system at 150 °C within 1.5 h. Additionally, a catalytic reaction pathway was proposed, involving the adsorption of glucose molecules by the −Cl group on the catalyst via a hydrogen bond, followed by glucose isomerization to fructose over the Lewis acid Sn 4+ and Al 3+ sites and, finally, fructose dehydration to HMF catalyzed by the Brønsted acid Sn-OH and Si-OH-Al sites. The activity of the catalyst decreased due to the leaching of the active site Sn after several consecutive cycles. This work provides insights into the improvement in the Sn-containing zeolite catalyst for tandem conversion of glucose to HMF.
Photocatalysis
is one of the most promising technologies in wastewater
treatment. However, the inactivity to visible light and the inconvenience
to recycle severely limit its practical application. In this work,
via a facile hydrothermal method, Fe3O4 NPs
were integrated onto the surfaces of 3D ball-flower-like MoS2 microspheres as efficiently visible light responsive and magnetically
recyclable photocatalysts. Experimental results indicate that, an
optimal loading amount (20 wt %) of Fe3O4 NPs
can not only effectively enhance the photocatalytic ability of the
MoS2/Fe3O4 (MF) hybrid composite
with approximately 2 times better than pure MoS2, but also
make it conveniently recycle from water by an external magnetic field.
The photoelectrochemical studies also reveal that the incorporation
of Fe3O4 NPs can effectively enhance the charge
transfer rate and accelerate separation of photoinduced charge carriers.
The surface catalytic mechanism of MF hybrid composite was also explored
through XPS spectra. With both the excellent photocatalytic performance
and magnetical recyclability, the 20 wt %-MF hybrid composite is considered
to be a promising and competitive photocatalyst for wastewater treatment
utilizing solar energy.
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