Yanlong Qi,Shijun Liu,Long Cui,Quanquan Dai,Jianyun He,Wei Dong,Chenxi Bai
The synthesis of functionalized 1,3-dienes has received increasing attention due to their importance in the practical development of high-performance elastomers. In the present work, furfural and acetone, acting as renewable feedstocks, are first employed to produce a functionalized 1,3-diene containing a furan group (1-(2-furyl)-1,3-butadiene, F-diene). After selective hydrogenation of the CO group, the aldol adduct (4-(2-furanyl)-3-buten-2-ol, FAH) shows a nearly complete conversion, with an excellent selectivity (as high as 92%) towards F-diene over ceria-based catalysts in a fixed bed. BET, TEM, XRD, XPS, Raman, TPD, TPR and TGA were conducted to identify the relationship between the catalytic performance and catalyst structure. A plausible reaction pathway for the dehydration of FAH over ceria-based catalysts was proposed using a radical mechanism, which suggested the importance of the Ce4+–Ce3+ redox cycle for the dehydration of FAH to F-diene. Furthermore, the ceria-based catalysts exhibited a notable carbon resistance.
Clinical application of hepatocyte transplantation has been halted due to the low engraftment efficiency and limited proliferation capacity of donor hepatocytes in the host liver. Here, we developed a magneto-plasmonic nanohybrid to spatiotemporally drive the primary hepatocytes into the host liver under the external magnetic field that significantly improves the engraftment efficiency of donor hepatocytes. A magnetic lipid-coated-gold-nanorods/iron-oxide nanocluster (GNR-IO) (LGI) was designed for efficient magneto-actuation and photoacoustic imaging-guided cell tracking during the hepatocyte transplantation. By optimizing the concentration of LGI (100 μg /mL) and the configuration of a magnetic field (260 mT), we were able to increase the engraftment efficiency of primary hepatocytes into the host livers of Fah -/- mice, a model with the genetic deficit of fumarylacetoacetate hydrolase (FAH) resulting in liver injuries, for 3.89-fold of the control by one week of the transplantation. Further assessment of repopulation of hepatocytes in the host liver indicated the LGI (100 μg /mL) + magnetic field (260 mT) group had up to 15 % repopulation of the host liver by three-weeks-post-transplantation and reached full repopulation by 6-weeks-post-transplantation. This was 3 ∼ 5 times more rapid than the Fah -/- mice transplanted with hepatocytes without the LGI and the magnetic field. RNA-sequencing of the hepatocytes incubated with LGI indicated that the loading of LGIs enhanced the migration, survival, and engraftment of hepatocytes by regulating the tumor necrosis factor (TNF)-signaling pathway and reducing the macrophage in host liver. Furthermore, LGI-labeled hepatocytes could be tracked in host livers with photoacoustic imaging for at least one week post transplantation. Most of the LGI were cleared from the host systems via the kidneys by six weeks. The novel strategy established in this study, which utilized nanoparticles combined with the magnetic field to improve the efficiency of primary hepatocyte engraftment and repopulation, can provide a feasible scheme for the clinical application of hepatocyte transplantation in the treatment of liver failure.
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