To date,some questions about medium-entropy carbide ceramics and the corresponding multi-phase carbide ceramics with the same cations and proportions remain unclear.Regarding oxidation behavior,do both have synergisti...To date,some questions about medium-entropy carbide ceramics and the corresponding multi-phase carbide ceramics with the same cations and proportions remain unclear.Regarding oxidation behavior,do both have synergistic oxidation abilities and what role does entropy stabilization play in medium-entropy carbides?In this work,the oxidation behaviors of HfC-ZrC-TiC multi-phase carbide(HZT-MPC)and(Hf_(1/3)Zr_(1/3)Ti_(1/3))C medium-entropy carbide(HZT-MEC)powders were investigated.After thermogravimetry(TG)oxidation,the TG curve of HZT-MPC had a bimodal distribution.The"preferential oxidation"of HfC/ZrC occurred within HZT-MPC,followed by the formation of multi-phase oxides(HfO_(2),ZrO_(2),and TiO_(2)).The uneven compositional distribution slowed their solid solution reactions to form Ti-doped(Hf,Zr)O_(2) and(Hf,Zr)TiO_(4).The TG curve of HZT-MEC had a single peak.A uniform compositional distribution at the atomic scale promoted the rapid interdiffusion of oxides,forming Ti-doped(Hf,Zr)O_(2) and(Hf,Zr)TiO_(4) without ZrO_(2),HfO_(2),and TiO_(2) after TG oxidation.Additionally,HZT-MEC had a higher onset oxidation temperature(To;470℃)than did HZT-MPC(430℃),and the TG single peak of HZT-MEC was between the TG bimodal peaks of HZT-MPC.Therefore,HZT-MEC showed superior oxidation resistance compared to HZT-MPC,which was attributed to the entropy stabilization effect of HZT-MEC suppressing the"preferential oxidation"of HfC/ZrC and the"delayed oxidation"of TiC,promoting the synergistic oxidation ability of multiple principal elements.展开更多
We have designed and prepared β-cyclodextrin （β-CD）-functionalized multi-walled nanotubes （MWCNTs-g-CD） for the oxidation of cinnamon oil to natural benzaldehyde under aqueous condi- tions. The synergistic effec...We have designed and prepared β-cyclodextrin （β-CD）-functionalized multi-walled nanotubes （MWCNTs-g-CD） for the oxidation of cinnamon oil to natural benzaldehyde under aqueous condi- tions. The synergistic effect of combining MWCNTs with β-CD led to a remarkable increase in the performance of the MWCNTs-g-CD for the catalytic oxidation of cinnamaldehyde, which exhibited 95% cinnamaldehyde conversion and 85% selectivity to natural benzaldehyde with a short reaction time of 10 rain. The MWCNTs-g-CD also exhibited outstanding recyclability with good stability, showing no discernible decrease in their catalytic activity over five reaction cycles.展开更多
A series of Mn-Mo-W-O_x/TiO_2-SiO_2 catalysts was modified with CeO_2 using an extrusion molding method. The catalytic activities of the obtained catalysts were tested for the synergistic catalytic removals of CO, NO ...A series of Mn-Mo-W-O_x/TiO_2-SiO_2 catalysts was modified with CeO_2 using an extrusion molding method. The catalytic activities of the obtained catalysts were tested for the synergistic catalytic removals of CO, NO and C_3H_8. The ratio of catalyst composition on catalytic activities for NH_3-SCR was optimized, which reveals that the molar ratio of Ti/Si was 9：1 and the catalyst containing 1.5 wt% CeO_2 and 12 wt% Mn-Mo-W-O_x exhibits the best catalytic performances. These samples were characterized by XRD, N_2-BET, Py-IR, NH_3-TPD, SEM/element mapping, H_2-TPR and XPS, respectively. Results show that the optimal catalyst exhibits more than 99% NO conversion, 86% CO conversion and 100% C_3H_8 conversion under GHSV of 5000 h^（-1）. In addition, the GHSV has little influence on removal of NO when it is less than 15,000 h^（-1）. Furthermore, the addition of CeO_2 will enhance the surface acidity, increase Mn^（4＋）concentration and inhibit the grain growth, which are favorable for the excellent catalytic performance.Anyway,the 1.5 wt% CeO_2-12 wt% Mn-Mo-W-O_x/TiO_2-SiO_2 possesses outstanding redox properties,abundant acid sites and high Mn^（4＋） concentration, which provide a guarantee for synergistic catalytic removal of CO, NO and HC.展开更多
Synergistic effect of FeVO_4 withα-Fe_2O_3 was found in Fe-V-O catalyst,which was responsible for the high apparent formation rate（A.F.R.） of benzaldehyde in liquid phase oxidation of toluene by hydrogen peroxide.T...Synergistic effect of FeVO_4 withα-Fe_2O_3 was found in Fe-V-O catalyst,which was responsible for the high apparent formation rate（A.F.R.） of benzaldehyde in liquid phase oxidation of toluene by hydrogen peroxide.The synergistic effect might create VO_πspecies as active sites;moreover,it improved the reducibility and the reactivity of Fe-V-O catalyst.In order to gain the high A.F.R. of benzaldehyde,the catalyst should have the moderate reducibihty.展开更多
In this study,a series of Co_3O_4/ mildly oxidized graphite oxide(mGO) nanocatalysts(Co_3O_4/ mGO-l,Co_3O_4/ mGO-2 and Co_3O_4/mGO-3) were synthesized through solvothermal method and used as a mediator for the heterog...In this study,a series of Co_3O_4/ mildly oxidized graphite oxide(mGO) nanocatalysts(Co_3O_4/ mGO-l,Co_3O_4/ mGO-2 and Co_3O_4/mGO-3) were synthesized through solvothermal method and used as a mediator for the heterogeneous peroxymonosulfate(PMS)activation.The performance of CO_3O_4 / mGO/PMS system was investigated using acid orange 7(AO7).Results showed that Co_3O_4/mGO-3 had the best degradation efficiency of AO7 and the removal rate was above 90%in about 6 min.The phenomenon indicated the catalytic activity of Co_3O_4/mGO composites was related to the oxidation degree of graphite oxide(GO).In addition,experiments showed the content of Co_3O_4 had an effect on the catalytic activity.The composites were characterized with X-ray powder diffraction(XRD),FTIR,Raman,X-ray photoelectron spectroscopy(XPS) and transmission electron microscopy(TEM).According to the charactrization and synergistic catalytic mechanism,the generation of Co—OH complexes found to be the initial step to activate PMS in the heterogeneous system of Co_3O_4/mGO hybrid.展开更多
Advanced oxidation processes(AOPs) have been applied to address multiple environmental concerns including antibiotic resistance genes(ARGs). ARGs have shown an increasing threat to human health,and they are either har...Advanced oxidation processes(AOPs) have been applied to address multiple environmental concerns including antibiotic resistance genes(ARGs). ARGs have shown an increasing threat to human health,and they are either harbored by antibiotic-resistant bacteria(ARB) or free in the environment.However, the control of ARGs has been substantially limited by their low concentration and the limited knowledge about their interfacial behavior. Herein, a novel AOP catalyst, Ag/TiO_(2)/graphene oxide(GO),combined with a polyvinylidene fluoride(PVDF) ultrafiltration membrane was designed with a synergistic interfacial adsorption and oxidation function to inactivate ARGs with high efficiency in both model solutions and in secondary wastewater effluent, especially when the residue concentration was low.Further analysis showed that the mineralization of bases and phosphodiesters mainly caused the inactivation of ARGs. Moreover, the interfacial adsorption and oxidation processes of ARGs were studied at the molecular level. The results showed that GO was rich in sp^(2) backbones and functional oxygen groups,which efficiently captured and enriched the ARGs via p-p interactions and hydrogen bonds. Therefore,the photogenerated active oxygen species attack the ARGs by partially overcoming the kinetic problems in this process. The Ag/Ti O2/GO catalyst was further combined with a PVDF membrane to test its potential in wastewater treatment applications. This work offers an efficient method and a corresponding material for the inactivation and mineralization of intra/extracellular ARGs. Moreover, the molecularlevel understanding of ARG behaviors on a solid–liquid interface will inspire further control strategies of ARGs in the future.展开更多
Visible light irradiation combined with homogeneous iron and/or hydrogen peroxide to degrade organic dye rhodamine B (RhB) and small molecular compound 2,4-dichlorophenol (2,4-DCP) in a home-made bottle reactor was as...Visible light irradiation combined with homogeneous iron and/or hydrogen peroxide to degrade organic dye rhodamine B (RhB) and small molecular compound 2,4-dichlorophenol (2,4-DCP) in a home-made bottle reactor was assessed. The concen-tration of oxidize species, Fe3+ and Fe2+ were determined during the degradation process. The results demonstrated that visible light irradiation combined with electro-Fenton improved the degradation efficiency. Moreover, both RhB and 2,4-DCP were mineralized during visible light synergistic electro-Fenton oxidation process. 95.0% TOC (total organic carbon) removal rate of RhB occurred after 90 min and 96.7% of COD (chemical oxygen demand) removal rate after 65 min of irradiation. 91.3% TOC removal rate of 2,4-DCP occurred after 16 h of irradiation and 99.9% COD removal rate occurred after 12 h of illumination. The degradation and oxidation process was dominated by the hydroxyl radical ( · OH) generated in the system. Both the impressed electricity and dye sensitization by visible light facilitated the conversion between Fe3+ and Fe 2+ , thus, improving Fenton reaction efficiency.展开更多
Microcystin-LR attracts attention due to its high toxicity, high concentration and high frequency. The removal characteristics of UV/H2O2 and O3/H2O2 advanced oxidation processes and their individual process for MC-LR...Microcystin-LR attracts attention due to its high toxicity, high concentration and high frequency. The removal characteristics of UV/H2O2 and O3/H2O2 advanced oxidation processes and their individual process for MC-LR were investigated and compared in this study. Both the removal efficiencies and rates of MC-LR as well as the biotoxicity of degradation products was analyzed. Results showed that the UV/H2O2 process and O3/H2O2 were effective methods to remove MC-LR from water, and they two performed better than UV-, O3-, H2O2-alone processes under the same conditions. The effects of UV intensity, H2O2 concentration and O3 concentration on the removal perfomlance were explored. The synergistic effects between UV and H2O2, O3 and H2O2 were observed. UV dosage of 1800 mJ·cm^-2 was required to remove 90% of 100μg.L^-1 MC-LR, which amount significantly decreased to 500 mJ.cm^-2 when 1.7mg·L^-1 H2O2 was added. 0.25 mg.L^-1 O3, or 0.125 mg·L^-1 O9 with 1.7 mg·L^-1 H2O2 was needed to reach 90% removal efficiency. Furthermore, the biotoxicity results about these UV/H2O2, O3/H2O2 and O3-alone processes all present rising trends with oxidation degree of MC-LR. Biotoxicity of solution, equ valent to 0.01 mg·L^-1 Zn^2＋,ratsed to 0.05 mg.L Zn after UV/H2O2 or O3/H2O2 reaction. This phenomenon may be attributed to the aldehydes and ketones with small molecular weight generated during reaction. Advice about the selection of MC-LR removal methods in real cases was provided.展开更多
Near infrared(NIR) light-driven nitric oxide(NO) release nano-platform based on upconversion nanoparticles(UCNPs) and light sensitive NO precursor Roussin's black salt(RBS) was fabricated to generate NO upon 808 n...Near infrared(NIR) light-driven nitric oxide(NO) release nano-platform based on upconversion nanoparticles(UCNPs) and light sensitive NO precursor Roussin's black salt(RBS) was fabricated to generate NO upon 808 nm irradiation. The application of 808 nm laser as the excitation source could achieve better penetration depth and avoid overheating problem. The combination of UCNPs and RBS could realize the on-demand release of NO at desired time and location by simply controlling the output of NIR laser.Cellular uptake results showed that more nanoparticles were internalized in cancer stem-like cells(CSCs)rather than non-CSCs. Therefore, a synergistic cancer therapy strategy to eradicate both CSCs and nonCSCs simultaneously was developed. Traditional chemo-drug could inhibit non-CSCs but has low killing efficiency in CSCs. However, we found that the combination of NO and chemotherapy could efficiently inhibit CSCs in bulk cells, including inhibiting mammosphere formation ability, decreasing CD44^+/CD24^- subpopulation and reducing tumorigenic ability. The mechanism studies confirmed that NO could not only induce apoptosis but also increase drug sensitivity by declining drug efflux in CSCs. This UCNPsbased platform may provide a new combinatorial strategy of NO and chemotherapy to improve cancer treatment.展开更多
One-pot direct conversion of cheap and abundant fructose to 2,5-diformylfuran (DFF) is highly desirable to achieve hundreds-fold value-increase and high atomic economy,yet it is still challenging due to the lack of su...One-pot direct conversion of cheap and abundant fructose to 2,5-diformylfuran (DFF) is highly desirable to achieve hundreds-fold value-increase and high atomic economy,yet it is still challenging due to the lack of suitable catalysts with cascade conversion ability.In this work,we developed a porous hybrid catalyst (i.e.PMo_(10)V_(2)@2Br-PIL) based on the assembly of polyoxometalates and porous polyionic liquids that can be applied in the one-pot conversion of fructose to DFF.The integration of PMo_(10)V_(2) with 2Br-PIL can impart both Brønsted acid and oxidation sites in the porous structure,thereby enabling the one-pot cascade conversion.As a result,PMo_(10)V_(2)@2Br-PIL demonstrated a remarkable DFF yield (95% yield),satisfying stability,recyclability and scale-up production ability (≈12.3 g in a batch experiment),demonstrating great potential for industrial production of DFF from fructose.Theoretical calculations revealed a synergistic effect of Brønsted acid sites and oxidation sites in PMo_(10)V_(2)@2Br-PIL,which promoted the one-pot conversion of fructose to DFF.This study enhances the understanding of biomass transformation over hybrid catalysts through synergetic acidic/oxidative catalysis,contributing to the development of highly active,selective,and multifunctional catalysts for one-pot biomass conversion.展开更多
基金This work was supported by the National Natural Science Foundation of China(Nos.52130205,52302091,and 52293373)the National Key R&D Program of China(No.2021YFA0715803)+1 种基金the Joint Fund of Henan Province Science and Technology R&D Program(No.225200810105)the ND Basic Research Funds of Northwestern Polytechnical University(No.G20022WD).
文摘To date,some questions about medium-entropy carbide ceramics and the corresponding multi-phase carbide ceramics with the same cations and proportions remain unclear.Regarding oxidation behavior,do both have synergistic oxidation abilities and what role does entropy stabilization play in medium-entropy carbides?In this work,the oxidation behaviors of HfC-ZrC-TiC multi-phase carbide(HZT-MPC)and(Hf_(1/3)Zr_(1/3)Ti_(1/3))C medium-entropy carbide(HZT-MEC)powders were investigated.After thermogravimetry(TG)oxidation,the TG curve of HZT-MPC had a bimodal distribution.The"preferential oxidation"of HfC/ZrC occurred within HZT-MPC,followed by the formation of multi-phase oxides(HfO_(2),ZrO_(2),and TiO_(2)).The uneven compositional distribution slowed their solid solution reactions to form Ti-doped(Hf,Zr)O_(2) and(Hf,Zr)TiO_(4).The TG curve of HZT-MEC had a single peak.A uniform compositional distribution at the atomic scale promoted the rapid interdiffusion of oxides,forming Ti-doped(Hf,Zr)O_(2) and(Hf,Zr)TiO_(4) without ZrO_(2),HfO_(2),and TiO_(2) after TG oxidation.Additionally,HZT-MEC had a higher onset oxidation temperature(To;470℃)than did HZT-MPC(430℃),and the TG single peak of HZT-MEC was between the TG bimodal peaks of HZT-MPC.Therefore,HZT-MEC showed superior oxidation resistance compared to HZT-MPC,which was attributed to the entropy stabilization effect of HZT-MEC suppressing the"preferential oxidation"of HfC/ZrC and the"delayed oxidation"of TiC,promoting the synergistic oxidation ability of multiple principal elements.
基金supported by the National Natural Science Foundation of China (21376279, 21276102, 21425627)Guangdong Technology Research Center for Synthesis and Separation of Thermosensitive Chemicals (2015B090903061)+1 种基金the Fundamental Research Funds for the Central Universities (14lgpy28)Guangzhou Science and Technology Plan Projects (2014J4100125)~~
文摘We have designed and prepared β-cyclodextrin （β-CD）-functionalized multi-walled nanotubes （MWCNTs-g-CD） for the oxidation of cinnamon oil to natural benzaldehyde under aqueous condi- tions. The synergistic effect of combining MWCNTs with β-CD led to a remarkable increase in the performance of the MWCNTs-g-CD for the catalytic oxidation of cinnamaldehyde, which exhibited 95% cinnamaldehyde conversion and 85% selectivity to natural benzaldehyde with a short reaction time of 10 rain. The MWCNTs-g-CD also exhibited outstanding recyclability with good stability, showing no discernible decrease in their catalytic activity over five reaction cycles.
基金Project supported by the National Key Research and Development Program of China(2016YFC0205500)National Natural Science Foundation of China(51772149)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘A series of Mn-Mo-W-O_x/TiO_2-SiO_2 catalysts was modified with CeO_2 using an extrusion molding method. The catalytic activities of the obtained catalysts were tested for the synergistic catalytic removals of CO, NO and C_3H_8. The ratio of catalyst composition on catalytic activities for NH_3-SCR was optimized, which reveals that the molar ratio of Ti/Si was 9：1 and the catalyst containing 1.5 wt% CeO_2 and 12 wt% Mn-Mo-W-O_x exhibits the best catalytic performances. These samples were characterized by XRD, N_2-BET, Py-IR, NH_3-TPD, SEM/element mapping, H_2-TPR and XPS, respectively. Results show that the optimal catalyst exhibits more than 99% NO conversion, 86% CO conversion and 100% C_3H_8 conversion under GHSV of 5000 h^（-1）. In addition, the GHSV has little influence on removal of NO when it is less than 15,000 h^（-1）. Furthermore, the addition of CeO_2 will enhance the surface acidity, increase Mn^（4＋）concentration and inhibit the grain growth, which are favorable for the excellent catalytic performance.Anyway,the 1.5 wt% CeO_2-12 wt% Mn-Mo-W-O_x/TiO_2-SiO_2 possesses outstanding redox properties,abundant acid sites and high Mn^（4＋） concentration, which provide a guarantee for synergistic catalytic removal of CO, NO and HC.
基金supported by Ministry of Education(NoNCET-10-878,20096101120018,2009-37th of SRFROCS)Shaanxi Province(No2009ZDKG-70,09JK793)+1 种基金Northwest University(NoPR09005,10YSY08)State Key Lab for SSPC(2009)
文摘Synergistic effect of FeVO_4 withα-Fe_2O_3 was found in Fe-V-O catalyst,which was responsible for the high apparent formation rate（A.F.R.） of benzaldehyde in liquid phase oxidation of toluene by hydrogen peroxide.The synergistic effect might create VO_πspecies as active sites;moreover,it improved the reducibility and the reactivity of Fe-V-O catalyst.In order to gain the high A.F.R. of benzaldehyde,the catalyst should have the moderate reducibihty.
基金Innovation Program of Shanghai Municipal Education Commission,China(No.12ZZ069)Research Fund for the Doctoral Program of Higher Education,China(No.20130075110006)
文摘In this study,a series of Co_3O_4/ mildly oxidized graphite oxide(mGO) nanocatalysts(Co_3O_4/ mGO-l,Co_3O_4/ mGO-2 and Co_3O_4/mGO-3) were synthesized through solvothermal method and used as a mediator for the heterogeneous peroxymonosulfate(PMS)activation.The performance of CO_3O_4 / mGO/PMS system was investigated using acid orange 7(AO7).Results showed that Co_3O_4/mGO-3 had the best degradation efficiency of AO7 and the removal rate was above 90%in about 6 min.The phenomenon indicated the catalytic activity of Co_3O_4/mGO composites was related to the oxidation degree of graphite oxide(GO).In addition,experiments showed the content of Co_3O_4 had an effect on the catalytic activity.The composites were characterized with X-ray powder diffraction(XRD),FTIR,Raman,X-ray photoelectron spectroscopy(XPS) and transmission electron microscopy(TEM).According to the charactrization and synergistic catalytic mechanism,the generation of Co—OH complexes found to be the initial step to activate PMS in the heterogeneous system of Co_3O_4/mGO hybrid.
基金supported by the National Natural Science Foundation of China (21722702 and 21872102)Tianjin Municipal Science and Technology Bureau (18YFZCSF00730, 18YFZCSF00770, 18ZXSZSF00230 and 19YFZCSF00740)。
文摘Advanced oxidation processes(AOPs) have been applied to address multiple environmental concerns including antibiotic resistance genes(ARGs). ARGs have shown an increasing threat to human health,and they are either harbored by antibiotic-resistant bacteria(ARB) or free in the environment.However, the control of ARGs has been substantially limited by their low concentration and the limited knowledge about their interfacial behavior. Herein, a novel AOP catalyst, Ag/TiO_(2)/graphene oxide(GO),combined with a polyvinylidene fluoride(PVDF) ultrafiltration membrane was designed with a synergistic interfacial adsorption and oxidation function to inactivate ARGs with high efficiency in both model solutions and in secondary wastewater effluent, especially when the residue concentration was low.Further analysis showed that the mineralization of bases and phosphodiesters mainly caused the inactivation of ARGs. Moreover, the interfacial adsorption and oxidation processes of ARGs were studied at the molecular level. The results showed that GO was rich in sp^(2) backbones and functional oxygen groups,which efficiently captured and enriched the ARGs via p-p interactions and hydrogen bonds. Therefore,the photogenerated active oxygen species attack the ARGs by partially overcoming the kinetic problems in this process. The Ag/Ti O2/GO catalyst was further combined with a PVDF membrane to test its potential in wastewater treatment applications. This work offers an efficient method and a corresponding material for the inactivation and mineralization of intra/extracellular ARGs. Moreover, the molecularlevel understanding of ARG behaviors on a solid–liquid interface will inspire further control strategies of ARGs in the future.
基金supported by China National Funds for Distinguished Young Scientists (50925932)the National Natural Science Foundation of China (21177072, 21207079)Open Foundation about Key Laboratory of Catalysis and Materials Science of the State Ethnic Affairs Commission& Ministry of Education of Hubei Province (CHCL10007)
文摘Visible light irradiation combined with homogeneous iron and/or hydrogen peroxide to degrade organic dye rhodamine B (RhB) and small molecular compound 2,4-dichlorophenol (2,4-DCP) in a home-made bottle reactor was assessed. The concen-tration of oxidize species, Fe3+ and Fe2+ were determined during the degradation process. The results demonstrated that visible light irradiation combined with electro-Fenton improved the degradation efficiency. Moreover, both RhB and 2,4-DCP were mineralized during visible light synergistic electro-Fenton oxidation process. 95.0% TOC (total organic carbon) removal rate of RhB occurred after 90 min and 96.7% of COD (chemical oxygen demand) removal rate after 65 min of irradiation. 91.3% TOC removal rate of 2,4-DCP occurred after 16 h of irradiation and 99.9% COD removal rate occurred after 12 h of illumination. The degradation and oxidation process was dominated by the hydroxyl radical ( · OH) generated in the system. Both the impressed electricity and dye sensitization by visible light facilitated the conversion between Fe3+ and Fe 2+ , thus, improving Fenton reaction efficiency.
文摘Microcystin-LR attracts attention due to its high toxicity, high concentration and high frequency. The removal characteristics of UV/H2O2 and O3/H2O2 advanced oxidation processes and their individual process for MC-LR were investigated and compared in this study. Both the removal efficiencies and rates of MC-LR as well as the biotoxicity of degradation products was analyzed. Results showed that the UV/H2O2 process and O3/H2O2 were effective methods to remove MC-LR from water, and they two performed better than UV-, O3-, H2O2-alone processes under the same conditions. The effects of UV intensity, H2O2 concentration and O3 concentration on the removal perfomlance were explored. The synergistic effects between UV and H2O2, O3 and H2O2 were observed. UV dosage of 1800 mJ·cm^-2 was required to remove 90% of 100μg.L^-1 MC-LR, which amount significantly decreased to 500 mJ.cm^-2 when 1.7mg·L^-1 H2O2 was added. 0.25 mg.L^-1 O3, or 0.125 mg·L^-1 O9 with 1.7 mg·L^-1 H2O2 was needed to reach 90% removal efficiency. Furthermore, the biotoxicity results about these UV/H2O2, O3/H2O2 and O3-alone processes all present rising trends with oxidation degree of MC-LR. Biotoxicity of solution, equ valent to 0.01 mg·L^-1 Zn^2＋,ratsed to 0.05 mg.L Zn after UV/H2O2 or O3/H2O2 reaction. This phenomenon may be attributed to the aldehydes and ketones with small molecular weight generated during reaction. Advice about the selection of MC-LR removal methods in real cases was provided.
基金supported by the National Basic Research Program of China(2016YFA2021600,2016YFA0202104,and2015CB932104)the National Natural Science Foundation of China(31571015,11621505,and 21320102003)Chinese Academy of Sciences Youth Innovation Promotion Association(2013007)
文摘Near infrared(NIR) light-driven nitric oxide(NO) release nano-platform based on upconversion nanoparticles(UCNPs) and light sensitive NO precursor Roussin's black salt(RBS) was fabricated to generate NO upon 808 nm irradiation. The application of 808 nm laser as the excitation source could achieve better penetration depth and avoid overheating problem. The combination of UCNPs and RBS could realize the on-demand release of NO at desired time and location by simply controlling the output of NIR laser.Cellular uptake results showed that more nanoparticles were internalized in cancer stem-like cells(CSCs)rather than non-CSCs. Therefore, a synergistic cancer therapy strategy to eradicate both CSCs and nonCSCs simultaneously was developed. Traditional chemo-drug could inhibit non-CSCs but has low killing efficiency in CSCs. However, we found that the combination of NO and chemotherapy could efficiently inhibit CSCs in bulk cells, including inhibiting mammosphere formation ability, decreasing CD44^+/CD24^- subpopulation and reducing tumorigenic ability. The mechanism studies confirmed that NO could not only induce apoptosis but also increase drug sensitivity by declining drug efflux in CSCs. This UCNPsbased platform may provide a new combinatorial strategy of NO and chemotherapy to improve cancer treatment.
基金financially supported by the National Natural Science Foundation of China(No.21871125,22475074,22171139 and 22201116)Natural Science Foundation of Guangdong Province(No.2023B1515020076)+2 种基金Natural Science Foundation of Shandong Province(No.ZR2022QB066 and ZR2023MB018)Dongying City School Cooperation Fund Key Project(SXHZ-2023-02-15)college Student Innovation and Entrepreneurship Training Plan of Liaocheng University(cxcy089).
文摘One-pot direct conversion of cheap and abundant fructose to 2,5-diformylfuran (DFF) is highly desirable to achieve hundreds-fold value-increase and high atomic economy,yet it is still challenging due to the lack of suitable catalysts with cascade conversion ability.In this work,we developed a porous hybrid catalyst (i.e.PMo_(10)V_(2)@2Br-PIL) based on the assembly of polyoxometalates and porous polyionic liquids that can be applied in the one-pot conversion of fructose to DFF.The integration of PMo_(10)V_(2) with 2Br-PIL can impart both Brønsted acid and oxidation sites in the porous structure,thereby enabling the one-pot cascade conversion.As a result,PMo_(10)V_(2)@2Br-PIL demonstrated a remarkable DFF yield (95% yield),satisfying stability,recyclability and scale-up production ability (≈12.3 g in a batch experiment),demonstrating great potential for industrial production of DFF from fructose.Theoretical calculations revealed a synergistic effect of Brønsted acid sites and oxidation sites in PMo_(10)V_(2)@2Br-PIL,which promoted the one-pot conversion of fructose to DFF.This study enhances the understanding of biomass transformation over hybrid catalysts through synergetic acidic/oxidative catalysis,contributing to the development of highly active,selective,and multifunctional catalysts for one-pot biomass conversion.
