We demonstrate a one-pot hydrothermal cohydrolysis-carbonization process using glucose and iron nitrate as starting materials for the fabrication of carbonaceous spheres embedded with iron oxide nanoparticles. It is verified by TEM, (57)Fe Mossbauer, and Fe K-edge XAS that iron oxide nanoparticles are highly dispersed in the carbonaceous spheres, leading to a unique microstructure. A formation mechanism is also proposed. This route is also applicable to a range of other naturally occurring saccharides and metal nitrates. A catalytic study revealed the remarkable stability and selectivity of the reduced Fe(x)O(y)@C spheres in the Fischer-Tropsch synthesis, which clearly exemplifies the promising application of such materials.
e-Iron carbide has been predicted to be promising for low-temperature Fischer-Tropsch synthesis (LTFTS) targeting liquid fuel production. However, directional carbidation of metallic iron to e-iron carbide is challenging due to kinetic hindrance. Here we show how rapidly quenched skeletal iron featuring nanocrystalline dimensions, low coordination number and an expanded lattice may solve this problem. We find that the carbidation of rapidly quenched skeletal iron occurs readily in situ during LTFTS at 423-473 K, giving an e-iron carbidedominant catalyst that exhibits superior activity to literature iron and cobalt catalysts, and comparable to more expensive noble ruthenium catalyst, coupled with high selectivity to liquid fuels and robustness without the aid of electronic or structural promoters. This finding may permit the development of an advanced energy-efficient and clean fuel-oriented FTS process on the basis of a cost-effective iron catalyst.
Fischer–Tropsch
synthesis to lower olefins (FTO) opens up
a compact and economical way to the production of lower olefin directly
from syngas (CO and H2) derived from natural gas, coal,
or renewable biomass. The present work is dedicated to a systematic
study on the effect of K in the reduced graphene oxide (rGO) supported
iron catalysts on the catalytic performance in FTO. It is revealed
that the activity, expressed as moles of CO converted to hydrocarbons
per gram Fe per second (iron time yield to hydrocarbons, termed as
FTY), increased first with the content of K, passed through a maximum
at 646 μmolCO gFe
–1 s–1 over the FeK1/rGO catalyst, and then decreased at
higher K contents. Unlike the evolution of the activity, the selectivity
to lower olefins increased steadily with K, giving the highest selectivity
to lower olefins of 68% and an olefin/paraffin (O/P) ratio of 11 in
the C2–C4 hydrocarbons over the FeK2/rGO
catalyst. The volcanic evolution of the activity is attributed to
the interplay among the positive effect of K on the formation of Hägg
carbide, the active phase for FTO, and the negative roles of K in
increasing the size of Hägg carbide at high content and blocking
the active phase by K-induced carbon deposition. The monotonic increase
in the selectivity to lower olefins is ascribed to the improved chain-growth
ability and surface CO/H2 ratio in the presence of K, which
favorably suppressed the unwanted CH4 production and secondary
hydrogenation of lower olefins.
Single-crystal Cr2O3 with regular mesopores has been synthesized using mesoporous silica KIT-6 as a template and characterized by using XRD, HRTEM and nitrogen adsorption/desorption.
Understanding the factors that contribute to loss of genetic diversity in fragmented populations is crucial for conservation measurements. Land-bridge archipelagoes offer ideal model systems for identifying the long-term effects of these factors on genetic variations in wild populations. In this study, we used nine microsatellite markers to quantify genetic diversity and differentiation of 810 pond frogs (Pelophylax nigromaculatus) from 24 islands of the Zhoushan Archipelago and three sites on nearby mainland China and estimated the effects of the island area, population size, time since island isolation, distance to the mainland and distance to the nearest larger island on reduced genetic diversity of insular populations. The mainland populations displayed higher genetic diversity than insular populations. Genetic differentiations and no obvious gene flow were detected among the frog populations on the islands. Hierarchical partitioning analysis showed that only time since island isolation (square-root-transformed) and population size (log-transformed) significantly contributed to insular genetic diversity. These results suggest that decreased genetic diversity and genetic differentiations among insular populations may have been caused by random genetic drift following isolation by rising sea levels during the Holocene. The results provide strong evidence for a relationship between retained genetic diversity and population size and time since island isolation for pond frogs on the islands, consistent with the prediction of the neutral theory for finite populations. Our study highlights the importance of the size and estimated isolation time of populations in understanding the mechanisms of genetic diversity loss and differentiation in fragmented wild populations.
We devised iron-based catalysts with honeycomb-structured graphene (HSG) as the support and potassium as the promoter for CO direct hydrogenation to light olefins (CO-FTO). Over the optimal FeK1.5/HSG catalyst, the iron time yield of light olefins amounted to 73 μmol g s with high selectivity of 59%. No obvious deactivation occurred within 120 h on stream. The excellent catalytic performance is attributed to the confinement effect of the porous HSG on the sintering of the active sites and the promotion effect of potassium on the activation of inert CO and the formation of iron carbide active for CO-FTO.
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