The oxidative condensation between renewable furfural and fatty alcohols is a crucial avenue for producing high-quality liquid fuels and valuable furan derivatives.The selectivity control in this reaction process rema...The oxidative condensation between renewable furfural and fatty alcohols is a crucial avenue for producing high-quality liquid fuels and valuable furan derivatives.The selectivity control in this reaction process remains a significant challenge.Herein,we report the strategy of confining well dispersed gold species within ZSM-5 structure to construct highly active Au@ZSM-5 zeolite catalysts for the oxidative condensation of furfural.Characterization results and spectroscopy analyses demonstrate the efficient encapsulation of isolated and cationic Au clusters in zeolite structure.Au@ZSM-5(K)catalyst shows remarkable performance with 69.7%furfural conversion and 90.2%furan-2-acrolein selectivity as well as good recycle stability.It is revealed that the microstructure of ZSM-5 zeolite can significantly promote oxidative condensation activity through confinement effects.This work presents an explicit example of constructing zeolite encaged noble metal catalysts toward targeted chemical transformations.展开更多
Magnesium and rare earth mixed oxides(Mg3 REOx(RE=La, Y. Ce)) were prepared and characterized by Xray diffraction(XRD), N_2 adsorption-desorption, infrared spectra and microcalorimetry of CO_2. The results revea...Magnesium and rare earth mixed oxides(Mg3 REOx(RE=La, Y. Ce)) were prepared and characterized by Xray diffraction(XRD), N_2 adsorption-desorption, infrared spectra and microcalorimetry of CO_2. The results reveal that the Mg_3 CeO_x catalyst is present in the form of Mg-Ce-O solid solution,while the Mg3 LaOx and Mg_3 YO_x catalysts are probably rare earth oxides dispersed on MgO surface. As a result, among the calcined Mg_3 REO_x catalysts, the Mg_3 CeO_x catalyst presents the highest rate constant for acetone aldolization, which is well correlated to its more homogeneous distribution of basic sites. In contrary, the Mg_3 YO_x catalyst exhibit the lowest catalytic activity for acetone aldolization. Upon hydration pre-treatment, the basic properties on the surface of the Mg_3 REO_x catalysts were changed markedly. The Mg_3 YO_x catalyst after hydration treatment shows the highest amount of basic sites on catalyst surface, and then exhibits the highest activity among the hydrated Mg_3 REO_x catalysts. These results make it possible to fine-tune basic sites for acetone aldolization.展开更多
An efficient approach has been developed for the synthesis of naturally occurring prenylated chalcones viz. kanzonol C (1), stipulin (2), crotaorixin (3), medicagenin (4), licoagrochalcone A (5) and abyssino...An efficient approach has been developed for the synthesis of naturally occurring prenylated chalcones viz. kanzonol C (1), stipulin (2), crotaorixin (3), medicagenin (4), licoagrochalcone A (5) and abyssinone D (6) along with the pyranochalcones paratocarpin C (7), anthyllisone (8) and 3-O-methylabyssinone A (9). The key step of the synthesis is a Claisen-Schmidt condensation. Subsequently, their anti-inflammatory effects were investigated in lipopolysaccharides (LPSs)-induced RAW-264.7 macrophages. Of the synthesized chalcones, compounds 5 (IC50= 10.41 μmol[L), 6 (IC50= 9.65 μmol/L) and 8 (IC50= 15.34 μmol/L) show remarkable activity with no cytotoxicity. Compound 9 (IC50 = 4.5 μmol/L) exhibits maximum (83.6%) nitric oxide (NO) inhibition, but shows slight cytotoxicity. The results reveal that the chalcones bearing the prenyl group at 3- and/or 5-position on ring A (acetophenone moiety), i.e., 1-4 and 7 show weak, or no inhibition activity, whereas chalcones having the prenyl group only on ring B (aldehyde part), i.e., 5, 6 and 8 show significant activity on the production of inflammatory mediated NO with no cytotoxicity.展开更多
Various tungsten oxide-based nanomaterials have been prepared by a modified plasma arc gas condensation technique without the use of catalysts or substrates. These products could be obtained by controlling the process...Various tungsten oxide-based nanomaterials have been prepared by a modified plasma arc gas condensation technique without the use of catalysts or substrates. These products could be obtained by controlling the processing parameters during experiment. All the as-obtained samples were characterized by field emission gun scanning electron microscopy, high-resolution transmission electron microscopy, and X- ray diffraction techniques. The results revealed that as-prepared tungsten oxide nanomaterials (WO3, W190s5 and WsO14) with different phases and morphologies could be obtained by decreasing the oxygen content in the chamber. In addition, W18049 nanotubes and nanorod bundles were fabricated by con- trolling the Ar/O2 ratio under He plasma gas. W18Q9/TiO2 core-shell nanoparticles were also prepared by evaporating a dual target. The experimental results showed that the present technique is unique and feasible for the fabrication of nanomaterials for use in different applications.展开更多
基金supported by the National Natural Science Fund of China(Grant Nos.22025203 and 22121005).
文摘The oxidative condensation between renewable furfural and fatty alcohols is a crucial avenue for producing high-quality liquid fuels and valuable furan derivatives.The selectivity control in this reaction process remains a significant challenge.Herein,we report the strategy of confining well dispersed gold species within ZSM-5 structure to construct highly active Au@ZSM-5 zeolite catalysts for the oxidative condensation of furfural.Characterization results and spectroscopy analyses demonstrate the efficient encapsulation of isolated and cationic Au clusters in zeolite structure.Au@ZSM-5(K)catalyst shows remarkable performance with 69.7%furfural conversion and 90.2%furan-2-acrolein selectivity as well as good recycle stability.It is revealed that the microstructure of ZSM-5 zeolite can significantly promote oxidative condensation activity through confinement effects.This work presents an explicit example of constructing zeolite encaged noble metal catalysts toward targeted chemical transformations.
基金Project supported by National Basic Research Program of China(2010CB732300)111 Project(B08021)China Scholarship Council for the Joint-Training Scholarship Program with Institut de Recherches sur la Catalyse et l'Environnement de Lyon(IRCELYON)and Universite Claude Bernard Lyon 1(UCBL1)
文摘Magnesium and rare earth mixed oxides(Mg3 REOx(RE=La, Y. Ce)) were prepared and characterized by Xray diffraction(XRD), N_2 adsorption-desorption, infrared spectra and microcalorimetry of CO_2. The results reveal that the Mg_3 CeO_x catalyst is present in the form of Mg-Ce-O solid solution,while the Mg3 LaOx and Mg_3 YO_x catalysts are probably rare earth oxides dispersed on MgO surface. As a result, among the calcined Mg_3 REO_x catalysts, the Mg_3 CeO_x catalyst presents the highest rate constant for acetone aldolization, which is well correlated to its more homogeneous distribution of basic sites. In contrary, the Mg_3 YO_x catalyst exhibit the lowest catalytic activity for acetone aldolization. Upon hydration pre-treatment, the basic properties on the surface of the Mg_3 REO_x catalysts were changed markedly. The Mg_3 YO_x catalyst after hydration treatment shows the highest amount of basic sites on catalyst surface, and then exhibits the highest activity among the hydrated Mg_3 REO_x catalysts. These results make it possible to fine-tune basic sites for acetone aldolization.
基金financially supported by Priority Research Centers Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education, Science and Technology (No. NRF-2009-0094071), South Korea
文摘An efficient approach has been developed for the synthesis of naturally occurring prenylated chalcones viz. kanzonol C (1), stipulin (2), crotaorixin (3), medicagenin (4), licoagrochalcone A (5) and abyssinone D (6) along with the pyranochalcones paratocarpin C (7), anthyllisone (8) and 3-O-methylabyssinone A (9). The key step of the synthesis is a Claisen-Schmidt condensation. Subsequently, their anti-inflammatory effects were investigated in lipopolysaccharides (LPSs)-induced RAW-264.7 macrophages. Of the synthesized chalcones, compounds 5 (IC50= 10.41 μmol[L), 6 (IC50= 9.65 μmol/L) and 8 (IC50= 15.34 μmol/L) show remarkable activity with no cytotoxicity. Compound 9 (IC50 = 4.5 μmol/L) exhibits maximum (83.6%) nitric oxide (NO) inhibition, but shows slight cytotoxicity. The results reveal that the chalcones bearing the prenyl group at 3- and/or 5-position on ring A (acetophenone moiety), i.e., 1-4 and 7 show weak, or no inhibition activity, whereas chalcones having the prenyl group only on ring B (aldehyde part), i.e., 5, 6 and 8 show significant activity on the production of inflammatory mediated NO with no cytotoxicity.
基金the financial support of this work by the National Science Council of Taiwan, China under grant number NSC 98-2221-E-027-035-MY3
文摘Various tungsten oxide-based nanomaterials have been prepared by a modified plasma arc gas condensation technique without the use of catalysts or substrates. These products could be obtained by controlling the processing parameters during experiment. All the as-obtained samples were characterized by field emission gun scanning electron microscopy, high-resolution transmission electron microscopy, and X- ray diffraction techniques. The results revealed that as-prepared tungsten oxide nanomaterials (WO3, W190s5 and WsO14) with different phases and morphologies could be obtained by decreasing the oxygen content in the chamber. In addition, W18049 nanotubes and nanorod bundles were fabricated by con- trolling the Ar/O2 ratio under He plasma gas. W18Q9/TiO2 core-shell nanoparticles were also prepared by evaporating a dual target. The experimental results showed that the present technique is unique and feasible for the fabrication of nanomaterials for use in different applications.