Background:PANoptosis has been identified as a robust inflammatory cell death pathway triggered upon host defense against invaded pathogens such as bacteria and viruses,however,pathogen-free tumor PANoptosis has not b...Background:PANoptosis has been identified as a robust inflammatory cell death pathway triggered upon host defense against invaded pathogens such as bacteria and viruses,however,pathogen-free tumor PANoptosis has not been achieved yet.Reactive oxygen and nitrogen species capable of inducing robust and diverse cell death pathways such as pyroptosis,apoptosis,and necroptosis are supposed to be the potential triggers for tumor PANoptosis by ultrasound(US)-controlled sono-piezodynamic therapy.Methods:S-nitrosothiols(SNO)-zinc peroxide(ZnO_(2))@cyclic dinucleotide(CDN)@mesoporous tetragonal barium titanate(mtBTO)nanoparticles(NZCB NPs)were synthesized by hydrothermal method with subsequent annealing,in situ growth,and finally surface functionalization.Scanning electron microscopy,transmission electron microscopy,X-ray diffraction,atomic force microscopy,Fourier transform infrared spectroscopy,and electron spin resonance were used for materials characterizations.Murine melanoma B16 cells are employed to investigate the in vitro US-initiated tumor PANoptosis by NZCB NPs.In vivo US-initiated tumor PANoptosis was investigated on B16 tumor-bearing C57BL/6J mice.Results:A“boiling-bubbling”strategy is developed to endow the piezoelectric BTO nanocatalysts,with mesoporous architecture,which enables the encapsulation of the immune-agonist CDN(9.4 wt%)to initiate innate immunity of the host.Then,SNO-functionalized ZnO_(2)was further employed to cap the mesoporous nanocatalysts,forming multifunctional piezocatalytic NZCB NPs.Under US irradiation,intracellular massive reactive oxygen and nitrogen species such as superoxide anion radicals,nitric oxide(NO),and peroxynitrite(ONOO-)could be produced from the piezoelectric NZCB NPs,which,synergized with CDN-triggered anti-tumoral immunity,lead to highly immunogenic tumor PANoptosis by NZCB NPs through the tumor microenvironment remodeling.Intratumoral injection of NZCB NPs leads to substantial tumor PANoptosis with immune potentiation,ultimately destroying the tumor xenografts effectively.Conclusion:The present work presents the mesostructure design of piezocatalytic nanomaterials and the crosstalk between oxidative stress and anti-tumor immunity within the tumor,facilitating promising tumor PANoptosis by nanocatalytic oxidation with high effectiveness and biocompatibility.展开更多
With the continuous development of nanomaterials in recent years,the application of nanocatalysts in catalytic ozone oxidation has attracted more and more researchers’attention due to their excellent catalytic proper...With the continuous development of nanomaterials in recent years,the application of nanocatalysts in catalytic ozone oxidation has attracted more and more researchers’attention due to their excellent catalytic properties.In this review,we systematically summarized the current research status of nanocatalysts mainly involving material categories,mechanisms and catalytic efficiency.Based on summary and analysis,we found most of the reported nanocatalysts were in the stage of laboratory research,which was caused by the nanocatalysts defects such as easy aggregation,difficult separation,and easy leakage.These defects might result in severe resource waste,economic loss and potentially adverse effects imposed on the ecosystem and human health.Aiming at solving these defects,we further analyzed the reasons and the existing reports,and revealed that coupling nano-catalyst and membrane,supported nanocatalysts and magnetic nanocatalysts had promising potential in solving these problems and promoting the actual application of nanocatalysts in wastewater treatment.Furthermore,the advantages,shortages and our perspectives of these methods are summarized and discussed.展开更多
This study focuses on drawing a hydrothermal synthesis process map for Co3O4 nanoparticles with various morphologies and investigating the effects of Co3O4 nanocatalyst morphology on CO oxidation.A series of cobalt-hy...This study focuses on drawing a hydrothermal synthesis process map for Co3O4 nanoparticles with various morphologies and investigating the effects of Co3O4 nanocatalyst morphology on CO oxidation.A series of cobalt-hydroxide-carbonate nanoparticles with various morphologies（i.e.,nanorods,nanosheets,and nanocubes） were successfully synthesized,and Co3O4 nanoparticles were obtained by thermal decomposition of the cobalt-hydroxide-carbonate precursors.The results suggest that the cobalt source is a key factor for controlling the morphology of cobalt-hydroxide-carbonate at relatively low hydrothermal temperatures（≤ 140℃）.Nanorods can be synthesized in CoCl2 solution,while Co（NO3）2 solution promotes the formation of nanosheets.Further increasing the synthesis temperature（higher than 140 ℃） results in the formation of nanocubes in either Co（NO3）2 or CoCl2 solution.The reaction time only affects the size of the obtained nanoparticles.The presence of CTAB could improve the uniformity and dispersion of particles.Co3O4 nanosheets showed much higher catalytic activity for CO oxidation than nanorods and nanocubes because it has more abundant Co^（3＋） on the surface,much higher reducibility,and better oxygen desorption capacity.展开更多
A simple and practical ultrasonically synthetic strategy for the preparation of rare-earth based catalyst, nanostructured NiFe2-xEuxO4 was developed. The structtre of NiFe2-xEuxO4 was characterized by various analyses...A simple and practical ultrasonically synthetic strategy for the preparation of rare-earth based catalyst, nanostructured NiFe2-xEuxO4 was developed. The structtre of NiFe2-xEuxO4 was characterized by various analyses such as X-ray diffraction （XRD）, scanning electron microscopy （SEM） and fourier transform infrared spectroscopy （FT-IR）. The catalytic performance of NiFe2-xEuxO4 was evaluated for the synthesis of benzimidazoles, benzoxazoles and benzothiazoles under ultrasonic irradiation. All reactions were completed in short times and all products were obtained in good to excellent yields in presence of the rare-earth based catalyst. Besides, NiFe2-xEuxO4 could be recovered for 6 times without noticeably decreasing the catalytic activity.展开更多
In the present study,CNFs,ZnO and Al2O3 were deposited on the SMFs panels to investigate the deactivation mechanism of Pd-based catalysts in selective acetylene hydrogenation reaction.The examined supports were charac...In the present study,CNFs,ZnO and Al2O3 were deposited on the SMFs panels to investigate the deactivation mechanism of Pd-based catalysts in selective acetylene hydrogenation reaction.The examined supports were characterized by SEM,NH3-TPD and N2adsorption-desorption isotherms to indicate their intrinsic characteristics.Furthermore,in order to understand the mechanism of deactivation,the resulted green oil was characterized using FTIR and SIM DIS.FTIR results confirmed the presence of more unsaturated constituents and then,more branched hydrocarbons formed upon the reaction over alumina-supported catalyst in comparison with the ones supported on CNFs and ZnO,which in turn,could block the pores mouths.Besides the limited hydrogen transfer,N2 adsorption-desorption isotherms results supported that the lowest pore diameters of Al2O3/SMFs close to the surface led to fast deactivation,compared with the other catalysts,especially at higher temperatures.展开更多
The engineering of carbon nanocatalysts for the persulfate activated elimination of emerging organic contaminants(EOCs)demonstrates promising potential compared with metal-based counterparts due to their unique advant...The engineering of carbon nanocatalysts for the persulfate activated elimination of emerging organic contaminants(EOCs)demonstrates promising potential compared with metal-based counterparts due to their unique advantage of high stability and low toxicity.The early reviews introduced the theoretical background of persulfate activation together with a detailed summary of different mechanisms responsible for degradation of EOCs.To further unify the state of knowledge,identify the research gaps,and prompt new research in this area,we present a thorough review on current trends in research on metal-free carbon nanocatalysts(e.g.,0D nanodiamond,1D carbon nanotubes and carbon nanofibers,2D graphene and graphitic carbon nitride,and 3D carbon nanocatalysts),with emphasis on their applications in persulfate activation and EOCs decontamination.We also discuss the current challenges and future perspectives in practically relevant applications.Last,we highlight that the development of sustainable carbon nanocatalysts/persulfate systems lies at the interface of multiple disciplines,which calls for future in-depth interdisciplinary collaborations.展开更多
We developed an in situ synthesis strategy for preparing well-dispersed CuO nanoparticles as aquathermolysis catalyst for viscosity reduction in Shengli heavy oil(China). A Cu(OH)_2-contained microemulsion was employe...We developed an in situ synthesis strategy for preparing well-dispersed CuO nanoparticles as aquathermolysis catalyst for viscosity reduction in Shengli heavy oil(China). A Cu(OH)_2-contained microemulsion was employed as a carrier to disperse the precursor Cu(OH)_2 to the heavy oil phase. Under aquathermolysis condition(240 ℃, 2.5 MPa of N_2), the Cu(OH)_2 precursors would first be converted in situ to well-crystallized and size-homogeneous CuO nanoparticles naturally, catalyzed by which the viscosity of Shengli heavy oil could be reduced as much as 94.6%; simultaneously, 22.4% of asphaltenes were converted to light components. The agglomeration of the in situ prepared monoclinic CuO nanoparticles could be negligible throughout the catalytic reaction. Based on the characterization results of ~1 H NMR, elemental analysis and GC-MS of oil samples before and after catalytic aquathermolysis, the mechanism for viscosity reduction of heavy oil in the catalytic system was investigated.展开更多
Nano titania-supported sulfonic acid（n-TSA） has found to be a highly efficient, eco-friendly and recyclable heterogeneous nanocatalyst for the solvent-free synthesis of 2,4,6-triarylpyridines through one-pot three-c...Nano titania-supported sulfonic acid（n-TSA） has found to be a highly efficient, eco-friendly and recyclable heterogeneous nanocatalyst for the solvent-free synthesis of 2,4,6-triarylpyridines through one-pot three-component reaction of acetophenones, aryl aldehydes and ammonium acetate. This reported method illustrates several advantages such as environmental friendliness reaction conditions,simplicity, short reaction time, easy work up, reusability of catalyst and high yields of the products. One new compound is reported too. Furthermore, the catalyst could be recycled after a simple work-up, and reused at least six times without substantial reduction in its catalytic activity.展开更多
Red blood cells(RBCs)have recently emerged as promosing candidates for cancer treatment in terms of relieving tumor hypoxia and inducing oxidative damage against cancer cells,but they are still far from satisfactory d...Red blood cells(RBCs)have recently emerged as promosing candidates for cancer treatment in terms of relieving tumor hypoxia and inducing oxidative damage against cancer cells,but they are still far from satisfactory due to their limited oxygen transport and reactive oxygen species generation rate in tumor tissue.Herein,artificial RBCs(designated FTP@RBCM)with radical storm production ability were developed for oncotherapy through multidimensional reactivity pathways of Fe-protoporphyrin-based hybrid metal-organic frameworks(FTPs,as the core),including photodynamic/chemodynamic-like,catalase-like and glutathione peroxidase-like activities.Meanwhile,owing to the advantages of long circulation abilities of RBCs provided by their cell membranes(RBCMs),FTP with a surface coated with RBCMs(FTP@RBCM)could enormously accumulate at tumor site to achieve remarkably enhanced therapeutic efficiency.Intriguingly,this ROS-mediated dynamic therapy was demonstrated to induce acute local inflammation and high immunogenic cancer death,which evoked a systemic antitumor immune response when combined with the newly identified T cell immunoglobulin and mucin-containing molecule 3(Tim-3)checkpoint blockade,leading to not only effective elimination of primary tumors but also an abscopal effect of growth suppression of distant tumors.Therefore,such RBC-mimic nanocatalysts with multidimensional catalytic capacities might provide a promising new insight into synergistic cancer treatment.展开更多
In this paper,highly stable,powerful,and recyclable magnetic nanoparticles tethered Nheterocyclic carbene-palladium(Ⅱ)((CH_(3))_(3)-NHC-Pd@Fe_(3)O_(4))as magnetic nanocatalyst was successfully synthesized from a simp...In this paper,highly stable,powerful,and recyclable magnetic nanoparticles tethered Nheterocyclic carbene-palladium(Ⅱ)((CH_(3))_(3)-NHC-Pd@Fe_(3)O_(4))as magnetic nanocatalyst was successfully synthesized from a simplistic multistep synthesis under aerobic conditions through easily available low-cost chemicals.Newly synthesized(CH_(3))_(3)-NHC-Pd@Fe_(3)O_(4) magnetic nanocatalyst was characterized from various analytical tools and catalytic potential of the(CH_(3))_(3)-NHC-Pd@Fe_3 O_4 magnetic nanocatalyst was studied for the catalytic reduction of toxic 4-nitrophenol(4-NP),hexavalent chromium(Cr(Ⅵ)),Methylene Blue(MB)and Methyl Orange(MO)at room temperature in aqueous media.UV-Visible spectroscopy was employed to monitor the reduction reactions.New(CH_(3))_(3)-NHC-Pd@Fe_(3)O_(4) magnetic nanocatalyst exhibited excellent catalytic activity for the reduction of toxic environmental pollutants.Moreover,(CH_(3))_(3)-NHC-Pd@Fe_(3)O_(4) magnetic nanocatalyst could be easily and rapidly separated from the reaction mixture with the help of an external magnet and recycled minimum five times in reduction of 4-NP,MB,MO and four times in Cr(Ⅵ)without significant loss of catalytic potential and remains stable even after reuse.展开更多
MoS2 has emerged for catalyzing the hydrogen evolution reaction.Various notable strategies have been developed to downsize the MoS2 particles and expose more active edges.However,the restacking issue,which reduces the...MoS2 has emerged for catalyzing the hydrogen evolution reaction.Various notable strategies have been developed to downsize the MoS2 particles and expose more active edges.However,the restacking issue,which reduces the exposure degree,has rarely been taken into account.Herein,we report on a facile proton-induced fast hydrothermal approach to produce size-controllable MoS2 nanocatalysts and demonstrate that along the varying of sheet sizes,there is a trade-off between the intrinsic catalytic activity(mainly determined by the unsaturated sulfur on the sheet edges)and the active edge accessibility(influenced by the assembly structure).The size-optimized catalyst delivers a high performance of a low overpotential of~200 mV at 10 mA/cm^(2),a Tafel slope of 46.3 mV/dec,and a stable working state,which is comparable to the recent notable works.Our findings will provide a pathway for its large-scale application and enhance the water electrolysis performance.展开更多
Benzimidazoles, benzoxazoles, and benzothiazoles derivatives were synthesized from condensation of aldehydes and 1,2-phenylenediamine or ortho-aminophenol or ortho-aminothiophenol in the presence of catalytic amount o...Benzimidazoles, benzoxazoles, and benzothiazoles derivatives were synthesized from condensation of aldehydes and 1,2-phenylenediamine or ortho-aminophenol or ortho-aminothiophenol in the presence of catalytic amount of Fe（Ⅲ）-Schiff base/SBA-15 in water medium. Short reaction times, good to excellent yields, easy availability, reusability, and use of an eco-friendly catalyst are some of the significant attributes of the present method.展开更多
Pt/C catalysts were prepared by ethylene glycol （EG） method in weakly acidic solutions adjusted by sodium citrate （NasCit）, sodium acetate （NaAc） and sodium hydroxide （NaOH）, separately. The effects of alkaliz...Pt/C catalysts were prepared by ethylene glycol （EG） method in weakly acidic solutions adjusted by sodium citrate （NasCit）, sodium acetate （NaAc） and sodium hydroxide （NaOH）, separately. The effects of alkalizing agent, pH and temperature were investigated by transmission electron microscopy （TEM） and CV. The composition and structure of Pt/C catalyst prepared at optimal conditions of 140℃ and pH=6.7 adjusted by NasCit was further characterized by X-ray photoelectron microscopy （XPS） and X-ray diffraction （XRD）, respectively. The average particle size of Pt/C catalyst prepared using Na3Cit is 2.1 nm, smaller than that of Pt/C catalyst （2.9 nm） prepared using NaAc, much smaller than that of Pt/C catalyst （100 nm） prepared using NaOH. The electrocatalytic activity of Pt/C catalysts prepared using Na3Cit and NaAc for ethanol oxidation are 456.6 and 419.2 mA/mgPt, comparative to those of Pt/C catalyst prepared by typical EG method and commercial E-TEK Pt/C catalyst. Finally, the size control mechanism of Pt nanoparticles was discussed.展开更多
CeO2/ZnO nanocatalysts were prepared from the coupling route of homogeneous precipita-tion with microemulsion and the impregnation method. The catalytic performance of these two kinds of catalysts on the oxidative cou...CeO2/ZnO nanocatalysts were prepared from the coupling route of homogeneous precipita-tion with microemulsion and the impregnation method. The catalytic performance of these two kinds of catalysts on the oxidative coupling of methane with carbon dioxide was tested and compared; the frac-tal behavior of the nanocatalysts was analyzed using fractal theory. The CeO2/ZnO nanocatalysts had much higher activity than the catalysts prepared by impregnation method. There was no regular relation-ship between the average size of CeO2/ZnO nanocatalysts and their catalytic performance; however, the conversion of methane increased with the increase of the fractal dimension of CeO2/ZnO nanocatalysts.展开更多
Novel pyrido[2,3-d]pyrimidine derivatives were synthesized through a one-pot three-component approach using HAp-encapsulated-γ-Fe2O3[γ-Fe2O3@HAp-SO3H]catalyzed condensation of 6-arnino-2-（methylthio or ethylthio）p...Novel pyrido[2,3-d]pyrimidine derivatives were synthesized through a one-pot three-component approach using HAp-encapsulated-γ-Fe2O3[γ-Fe2O3@HAp-SO3H]catalyzed condensation of 6-arnino-2-（methylthio or ethylthio）pyrimidin-4（3H）-one,Meldrum＇s acid and aryl aldehydes at 60 ℃ and under solvent-free conditions.In this protocol the use of nanocatalyst provided a green,useful and rapid method to generate the products in short reaction times and excellent yields（88%-94%）.展开更多
Encapsulation of Fe nanoparticles in zeolite is a promising way to significantly improve the catalytic activity and stability of Fe-based catalysts during the degradation process of organic pollutants.Herein,Fe nanoca...Encapsulation of Fe nanoparticles in zeolite is a promising way to significantly improve the catalytic activity and stability of Fe-based catalysts during the degradation process of organic pollutants.Herein,Fe nanocatalysts were encapsulated into silicalite-1(S-1)zeolite by using a ligand-protected method(with dicyandiamide(DCD)as a organic ligand)under direct hydrothermal synthesis condition.High-resolution transmission electron microscopy(HRTEM)results confirmed the high dispersion of Fe nanocatalysts which were successfully encapsulated within the voids among the primary particles of the S-1 zeolite.The developed S-1 zeolite encapsulated Fe nanocatalyst(Fe@S-1)exhibited significantly improved catalytic activity and reusability in the catalytic degradation process of methylene blue(MB).Specifically,the developed Fe0.021@S-1 catalyst showed high catalytic degradation activity,giving a high MB degradation efficiency of 100%in 30 min,outperformed the conventional impregnated catalyst(Fe/S-1).Moreover,the Fe@S-1 catalyst afforded an outstanding stability,showing only ca.7.9%activity loss after five cycling tests,while the Fe/S-1 catalyst presented a significantly activity loss of 50.9%after only three cycles.Notably,the encapsulation strategy enabled a relatively lower Fe loading in the Fe@S-1 catalyst in comparison with that of the Fe/S-1 catalyst,i.e.,0.35%vs.0.81%(mass).Radical scavenging experiments along with electron spin resonance(ESR)measurements confirmed that the major role ofOH in the MB degradation process.Specifically,Fe@S-1 catalyst with high molar ratio of[Fe(DCD)]Cl3 is beneficial to form Fe complexes/nanoclusters in the voids(which has large pore size of 1–2 nm)among the primary particles of the zeolite,and thus improving the diffusion and accessibility of reactants to Fe active sites,and thus exhibiting a relatively higher degradation efficiency.This work demonstrates that zeolite-encapsulated Fe nanocatalysts present potential applications in the advanced oxidation of wastewater treatment.展开更多
Heterogeneous Pd nanocatalysts are efficient catalysts for the Heck reaction but require multi-step,sophisticated procedures and harsh reaction conditions.In this work,a green and facile strategy has been developed to...Heterogeneous Pd nanocatalysts are efficient catalysts for the Heck reaction but require multi-step,sophisticated procedures and harsh reaction conditions.In this work,a green and facile strategy has been developed to decorate Pd nanoparticles on polydopamine(PDA)-coated multi-walled carbon nanotubes(Pd/CNTs-PDA)via a one-pot method.The obtained nanoparticles were characterized by various techniques including transmission electron microscopy,X-ray diffraction,and X-ray photoelectron spectroscopy,which proved that Pd NPs are well-dispersed on the PDA and between the surfaces of the PDA and CNTs.The resultant Pd/CNTs-PDA catalysts exhibit excellent catalytic reactivity toward the Heck reaction at low temperatures.Moreover,by DFT simulation,we found that during the PDA polymerization process,a large number of unsaturated—N=and C=O species are more active than the groups on the PDA end product to anchor Pd NPs.The results provide evidence that the catalyst synthesized by the onepot method exhibited good activity because sufficient active sites could be created to effectively promote Pd NPs dispersion during the dopamine polymerization process.Additionally,the Pd/CNTs-PDA catalyst was successfully employed in Heck cross-coupling reactions with various functionalized substrates.This method opens a window for the fabrication of high-performance nanocomposite catalysts under mild conditions using simple methods and has several potential applications.展开更多
The Li/MgO catalyst and nanocatalyst were prepared by the incipient wetness impregnation and sol-gel method, respectively. The catalytic performance of the Li/MgO catalyst and nanocatalyst on oxidative coupling of met...The Li/MgO catalyst and nanocatalyst were prepared by the incipient wetness impregnation and sol-gel method, respectively. The catalytic performance of the Li/MgO catalyst and nanocatalyst on oxidative coupling of methane was compared. The catalysts prepared in two ways were characterized by X-ray powder diffraction, Brunauer-Emmett-Teller surface and transmission electron microscope. The catalyst was tested at temperature of 973-1073 K with constant total pressure of 101 kPa. Experimental results showed that Li/MgO nanocatalyst in the oxidative coupling of methane would result in higher conversion of methane, higher selectivity, and higher yield of main products （ethane and ethylene） compared to ordinary catalyst. The results show the improved influence of nanoscale Li/MgO catalyst performance on oxidative coupling of methane.展开更多
The multiple metal catalyst as a promising nanomaterial has shown excellent activity in the peroxymonosulfate(PMS)activation for pollutant degradation.However,the role of special sites and in-depth understanding of th...The multiple metal catalyst as a promising nanomaterial has shown excellent activity in the peroxymonosulfate(PMS)activation for pollutant degradation.However,the role of special sites and in-depth understanding of the PMS activation mechanism are not fully studied.In this study,a Cu-doped CoFe_(2)O_(4)nanocatalyst(0.5CCF)was synthesized by a sol-gel and calcination method,and used for PMS activation to remove Rhodamine B(RhB).The results showed that the Cu doping obviously enhanced the catalytic performance of CoFe_(2)O_(4),with 99.70%of RhB removed by 0.5CCF while 74.91%in the CoFe_(2)O_(4)within 15 min.Based on the X-ray photoelectron spectroscopy and electrochemical analysis,this could be ascribed to the more low valence of Co and Fe species generated on the 0.5CCF and faster electron transfers occurred in the 0.5CCF due to the Cu doping.In addition,Cu doping could provide more reaction sites for the 0.5CCF to activate PMS for RhB removal.The metal species and the surface hydroxyl were the reaction sites of PMS activation,and the surface hydroxyl played an important role in surface-bound reactive species generation.During the PMS activation,the Cu not only activated PMS to produce reactive oxygen species(ROS),but also regenerated Co^(2+)and Fe^(2+)to accelerate the PMS activation.The non-radical of ^(1)O_(2)was the main ROS with a 99.35%of contribution rate,and the SO_(5)^(·–)self-reaction was its major source.This study provides a new insight to enhance the PMS activation performance of multiple metal catalysts by Cu doping in wastewater treatment.展开更多
This paper reports a stable heterogeneous nanoparticles catalyst MnFe2O4@PANI@Ag for the degradation of azo dyes. In this synthesizing method, MnFe204 is used as magnetic core and polyaniline （PANI） a linker to stab...This paper reports a stable heterogeneous nanoparticles catalyst MnFe2O4@PANI@Ag for the degradation of azo dyes. In this synthesizing method, MnFe204 is used as magnetic core and polyaniline （PANI） a linker to stabilize the Ag nanoparticles （NPs） on the surface of catalyst. The method has a high ability to prevent Ag NPs from aggregation on the PANI surface, thus resulting in small size and highly dispersed Ag NPs. The composition and nano-structural features of polycrystalline sample were studied by X-ray powder diffractometry, Fourier transform infrared spectroscopy, and scanning electron microsco- py. Vibrating sample magnetometer measurements proved the super-paramagnetic property of the catalyst, and UV results demonstrated that MnFe2O4@PANI@Ag has a high ability to reduce the azo dyes, which come from industrial wastes in the form of pollutant. The nanocomposites could be readily separated by magnet and reused for the next four reductions with high generation efficiency.展开更多
基金supported by the Shanghai Rising-Star Program(23QA1407600,23QA1409500)the National Natural Science Foundation of China(82272135,82372121)the National Natural Science Foundation of Shanghai(22ZR1448200).
文摘Background:PANoptosis has been identified as a robust inflammatory cell death pathway triggered upon host defense against invaded pathogens such as bacteria and viruses,however,pathogen-free tumor PANoptosis has not been achieved yet.Reactive oxygen and nitrogen species capable of inducing robust and diverse cell death pathways such as pyroptosis,apoptosis,and necroptosis are supposed to be the potential triggers for tumor PANoptosis by ultrasound(US)-controlled sono-piezodynamic therapy.Methods:S-nitrosothiols(SNO)-zinc peroxide(ZnO_(2))@cyclic dinucleotide(CDN)@mesoporous tetragonal barium titanate(mtBTO)nanoparticles(NZCB NPs)were synthesized by hydrothermal method with subsequent annealing,in situ growth,and finally surface functionalization.Scanning electron microscopy,transmission electron microscopy,X-ray diffraction,atomic force microscopy,Fourier transform infrared spectroscopy,and electron spin resonance were used for materials characterizations.Murine melanoma B16 cells are employed to investigate the in vitro US-initiated tumor PANoptosis by NZCB NPs.In vivo US-initiated tumor PANoptosis was investigated on B16 tumor-bearing C57BL/6J mice.Results:A“boiling-bubbling”strategy is developed to endow the piezoelectric BTO nanocatalysts,with mesoporous architecture,which enables the encapsulation of the immune-agonist CDN(9.4 wt%)to initiate innate immunity of the host.Then,SNO-functionalized ZnO_(2)was further employed to cap the mesoporous nanocatalysts,forming multifunctional piezocatalytic NZCB NPs.Under US irradiation,intracellular massive reactive oxygen and nitrogen species such as superoxide anion radicals,nitric oxide(NO),and peroxynitrite(ONOO-)could be produced from the piezoelectric NZCB NPs,which,synergized with CDN-triggered anti-tumoral immunity,lead to highly immunogenic tumor PANoptosis by NZCB NPs through the tumor microenvironment remodeling.Intratumoral injection of NZCB NPs leads to substantial tumor PANoptosis with immune potentiation,ultimately destroying the tumor xenografts effectively.Conclusion:The present work presents the mesostructure design of piezocatalytic nanomaterials and the crosstalk between oxidative stress and anti-tumor immunity within the tumor,facilitating promising tumor PANoptosis by nanocatalytic oxidation with high effectiveness and biocompatibility.
基金financially supported by the China special Science and Technology project on treatment and control of water pollution(No.2017ZX07402002)
文摘With the continuous development of nanomaterials in recent years,the application of nanocatalysts in catalytic ozone oxidation has attracted more and more researchers’attention due to their excellent catalytic properties.In this review,we systematically summarized the current research status of nanocatalysts mainly involving material categories,mechanisms and catalytic efficiency.Based on summary and analysis,we found most of the reported nanocatalysts were in the stage of laboratory research,which was caused by the nanocatalysts defects such as easy aggregation,difficult separation,and easy leakage.These defects might result in severe resource waste,economic loss and potentially adverse effects imposed on the ecosystem and human health.Aiming at solving these defects,we further analyzed the reasons and the existing reports,and revealed that coupling nano-catalyst and membrane,supported nanocatalysts and magnetic nanocatalysts had promising potential in solving these problems and promoting the actual application of nanocatalysts in wastewater treatment.Furthermore,the advantages,shortages and our perspectives of these methods are summarized and discussed.
基金supported by the National Natural Science Foundation of China (51374004,51204083)the Candidate Talents Training Fund of Yun-nan Province (2012HB009,2014HB006)+2 种基金the Applied Basic Research Program of Yunnan Province (2014FB123)a School-Enterprise Cooperation Project from Jinchuan Corporation (Jinchuan 201115)the Talents Training Program of Kunming University of Science and Technology (KKZ3201352038)~~
文摘This study focuses on drawing a hydrothermal synthesis process map for Co3O4 nanoparticles with various morphologies and investigating the effects of Co3O4 nanocatalyst morphology on CO oxidation.A series of cobalt-hydroxide-carbonate nanoparticles with various morphologies（i.e.,nanorods,nanosheets,and nanocubes） were successfully synthesized,and Co3O4 nanoparticles were obtained by thermal decomposition of the cobalt-hydroxide-carbonate precursors.The results suggest that the cobalt source is a key factor for controlling the morphology of cobalt-hydroxide-carbonate at relatively low hydrothermal temperatures（≤ 140℃）.Nanorods can be synthesized in CoCl2 solution,while Co（NO3）2 solution promotes the formation of nanosheets.Further increasing the synthesis temperature（higher than 140 ℃） results in the formation of nanocubes in either Co（NO3）2 or CoCl2 solution.The reaction time only affects the size of the obtained nanoparticles.The presence of CTAB could improve the uniformity and dispersion of particles.Co3O4 nanosheets showed much higher catalytic activity for CO oxidation than nanorods and nanocubes because it has more abundant Co^（3＋） on the surface,much higher reducibility,and better oxygen desorption capacity.
基金University of TehranImam Hosseign University for supporting this work
文摘A simple and practical ultrasonically synthetic strategy for the preparation of rare-earth based catalyst, nanostructured NiFe2-xEuxO4 was developed. The structtre of NiFe2-xEuxO4 was characterized by various analyses such as X-ray diffraction （XRD）, scanning electron microscopy （SEM） and fourier transform infrared spectroscopy （FT-IR）. The catalytic performance of NiFe2-xEuxO4 was evaluated for the synthesis of benzimidazoles, benzoxazoles and benzothiazoles under ultrasonic irradiation. All reactions were completed in short times and all products were obtained in good to excellent yields in presence of the rare-earth based catalyst. Besides, NiFe2-xEuxO4 could be recovered for 6 times without noticeably decreasing the catalytic activity.
文摘In the present study,CNFs,ZnO and Al2O3 were deposited on the SMFs panels to investigate the deactivation mechanism of Pd-based catalysts in selective acetylene hydrogenation reaction.The examined supports were characterized by SEM,NH3-TPD and N2adsorption-desorption isotherms to indicate their intrinsic characteristics.Furthermore,in order to understand the mechanism of deactivation,the resulted green oil was characterized using FTIR and SIM DIS.FTIR results confirmed the presence of more unsaturated constituents and then,more branched hydrocarbons formed upon the reaction over alumina-supported catalyst in comparison with the ones supported on CNFs and ZnO,which in turn,could block the pores mouths.Besides the limited hydrogen transfer,N2 adsorption-desorption isotherms results supported that the lowest pore diameters of Al2O3/SMFs close to the surface led to fast deactivation,compared with the other catalysts,especially at higher temperatures.
基金supported by the Open Project of State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(No.QAK202108)the National Natural Science Foundation of China(No.51822806)。
文摘The engineering of carbon nanocatalysts for the persulfate activated elimination of emerging organic contaminants(EOCs)demonstrates promising potential compared with metal-based counterparts due to their unique advantage of high stability and low toxicity.The early reviews introduced the theoretical background of persulfate activation together with a detailed summary of different mechanisms responsible for degradation of EOCs.To further unify the state of knowledge,identify the research gaps,and prompt new research in this area,we present a thorough review on current trends in research on metal-free carbon nanocatalysts(e.g.,0D nanodiamond,1D carbon nanotubes and carbon nanofibers,2D graphene and graphitic carbon nitride,and 3D carbon nanocatalysts),with emphasis on their applications in persulfate activation and EOCs decontamination.We also discuss the current challenges and future perspectives in practically relevant applications.Last,we highlight that the development of sustainable carbon nanocatalysts/persulfate systems lies at the interface of multiple disciplines,which calls for future in-depth interdisciplinary collaborations.
基金supported by PetroChina Innovation Foundation (Grant 2017D-5007-0211)National Natural Science Foundation of China (Grant 51174179)
文摘We developed an in situ synthesis strategy for preparing well-dispersed CuO nanoparticles as aquathermolysis catalyst for viscosity reduction in Shengli heavy oil(China). A Cu(OH)_2-contained microemulsion was employed as a carrier to disperse the precursor Cu(OH)_2 to the heavy oil phase. Under aquathermolysis condition(240 ℃, 2.5 MPa of N_2), the Cu(OH)_2 precursors would first be converted in situ to well-crystallized and size-homogeneous CuO nanoparticles naturally, catalyzed by which the viscosity of Shengli heavy oil could be reduced as much as 94.6%; simultaneously, 22.4% of asphaltenes were converted to light components. The agglomeration of the in situ prepared monoclinic CuO nanoparticles could be negligible throughout the catalytic reaction. Based on the characterization results of ~1 H NMR, elemental analysis and GC-MS of oil samples before and after catalytic aquathermolysis, the mechanism for viscosity reduction of heavy oil in the catalytic system was investigated.
基金the Faculty of Chemistry of Semnan University for supporting this work
文摘Nano titania-supported sulfonic acid（n-TSA） has found to be a highly efficient, eco-friendly and recyclable heterogeneous nanocatalyst for the solvent-free synthesis of 2,4,6-triarylpyridines through one-pot three-component reaction of acetophenones, aryl aldehydes and ammonium acetate. This reported method illustrates several advantages such as environmental friendliness reaction conditions,simplicity, short reaction time, easy work up, reusability of catalyst and high yields of the products. One new compound is reported too. Furthermore, the catalyst could be recycled after a simple work-up, and reused at least six times without substantial reduction in its catalytic activity.
基金supported by the National Natural Science Foundation of China(Grant Nos.62175198)the Natural Science Foundation of Fujian Province of China(Grant No.2020J02010)+1 种基金the Joint Funds for the innovation of science and Technology,Fujian province(Grant No.2019Y9046)the Fundamental Research Funds for the Central Universities(Grant No.xzy022020037).
文摘Red blood cells(RBCs)have recently emerged as promosing candidates for cancer treatment in terms of relieving tumor hypoxia and inducing oxidative damage against cancer cells,but they are still far from satisfactory due to their limited oxygen transport and reactive oxygen species generation rate in tumor tissue.Herein,artificial RBCs(designated FTP@RBCM)with radical storm production ability were developed for oncotherapy through multidimensional reactivity pathways of Fe-protoporphyrin-based hybrid metal-organic frameworks(FTPs,as the core),including photodynamic/chemodynamic-like,catalase-like and glutathione peroxidase-like activities.Meanwhile,owing to the advantages of long circulation abilities of RBCs provided by their cell membranes(RBCMs),FTP with a surface coated with RBCMs(FTP@RBCM)could enormously accumulate at tumor site to achieve remarkably enhanced therapeutic efficiency.Intriguingly,this ROS-mediated dynamic therapy was demonstrated to induce acute local inflammation and high immunogenic cancer death,which evoked a systemic antitumor immune response when combined with the newly identified T cell immunoglobulin and mucin-containing molecule 3(Tim-3)checkpoint blockade,leading to not only effective elimination of primary tumors but also an abscopal effect of growth suppression of distant tumors.Therefore,such RBC-mimic nanocatalysts with multidimensional catalytic capacities might provide a promising new insight into synergistic cancer treatment.
基金DST-SERB(Department of Science and Technology-Science and Engineering Research Board),India(SERB/F/1423/2017–18(No.YSS/2015/000010))Department of Science and Technology-Nanomission,India(No.SR/NM/NS20/2014)Jain University,India for financial support。
文摘In this paper,highly stable,powerful,and recyclable magnetic nanoparticles tethered Nheterocyclic carbene-palladium(Ⅱ)((CH_(3))_(3)-NHC-Pd@Fe_(3)O_(4))as magnetic nanocatalyst was successfully synthesized from a simplistic multistep synthesis under aerobic conditions through easily available low-cost chemicals.Newly synthesized(CH_(3))_(3)-NHC-Pd@Fe_(3)O_(4) magnetic nanocatalyst was characterized from various analytical tools and catalytic potential of the(CH_(3))_(3)-NHC-Pd@Fe_3 O_4 magnetic nanocatalyst was studied for the catalytic reduction of toxic 4-nitrophenol(4-NP),hexavalent chromium(Cr(Ⅵ)),Methylene Blue(MB)and Methyl Orange(MO)at room temperature in aqueous media.UV-Visible spectroscopy was employed to monitor the reduction reactions.New(CH_(3))_(3)-NHC-Pd@Fe_(3)O_(4) magnetic nanocatalyst exhibited excellent catalytic activity for the reduction of toxic environmental pollutants.Moreover,(CH_(3))_(3)-NHC-Pd@Fe_(3)O_(4) magnetic nanocatalyst could be easily and rapidly separated from the reaction mixture with the help of an external magnet and recycled minimum five times in reduction of 4-NP,MB,MO and four times in Cr(Ⅵ)without significant loss of catalytic potential and remains stable even after reuse.
基金supported by the National Natural Science Foundation of China(No.21905206)Shanghai Sail Program(No.19YF1450800)。
文摘MoS2 has emerged for catalyzing the hydrogen evolution reaction.Various notable strategies have been developed to downsize the MoS2 particles and expose more active edges.However,the restacking issue,which reduces the exposure degree,has rarely been taken into account.Herein,we report on a facile proton-induced fast hydrothermal approach to produce size-controllable MoS2 nanocatalysts and demonstrate that along the varying of sheet sizes,there is a trade-off between the intrinsic catalytic activity(mainly determined by the unsaturated sulfur on the sheet edges)and the active edge accessibility(influenced by the assembly structure).The size-optimized catalyst delivers a high performance of a low overpotential of~200 mV at 10 mA/cm^(2),a Tafel slope of 46.3 mV/dec,and a stable working state,which is comparable to the recent notable works.Our findings will provide a pathway for its large-scale application and enhance the water electrolysis performance.
基金Payame Noor University for its financial support of this study
文摘Benzimidazoles, benzoxazoles, and benzothiazoles derivatives were synthesized from condensation of aldehydes and 1,2-phenylenediamine or ortho-aminophenol or ortho-aminothiophenol in the presence of catalytic amount of Fe（Ⅲ）-Schiff base/SBA-15 in water medium. Short reaction times, good to excellent yields, easy availability, reusability, and use of an eco-friendly catalyst are some of the significant attributes of the present method.
基金supported by the National Basic Research Program of China (Grant No.2009CB220100)the Beijing Excellent Talent Support Program (Grant No.20071D1600300396)
文摘Pt/C catalysts were prepared by ethylene glycol （EG） method in weakly acidic solutions adjusted by sodium citrate （NasCit）, sodium acetate （NaAc） and sodium hydroxide （NaOH）, separately. The effects of alkalizing agent, pH and temperature were investigated by transmission electron microscopy （TEM） and CV. The composition and structure of Pt/C catalyst prepared at optimal conditions of 140℃ and pH=6.7 adjusted by NasCit was further characterized by X-ray photoelectron microscopy （XPS） and X-ray diffraction （XRD）, respectively. The average particle size of Pt/C catalyst prepared using Na3Cit is 2.1 nm, smaller than that of Pt/C catalyst （2.9 nm） prepared using NaAc, much smaller than that of Pt/C catalyst （100 nm） prepared using NaOH. The electrocatalytic activity of Pt/C catalysts prepared using Na3Cit and NaAc for ethanol oxidation are 456.6 and 419.2 mA/mgPt, comparative to those of Pt/C catalyst prepared by typical EG method and commercial E-TEK Pt/C catalyst. Finally, the size control mechanism of Pt nanoparticles was discussed.
文摘CeO2/ZnO nanocatalysts were prepared from the coupling route of homogeneous precipita-tion with microemulsion and the impregnation method. The catalytic performance of these two kinds of catalysts on the oxidative coupling of methane with carbon dioxide was tested and compared; the frac-tal behavior of the nanocatalysts was analyzed using fractal theory. The CeO2/ZnO nanocatalysts had much higher activity than the catalysts prepared by impregnation method. There was no regular relation-ship between the average size of CeO2/ZnO nanocatalysts and their catalytic performance; however, the conversion of methane increased with the increase of the fractal dimension of CeO2/ZnO nanocatalysts.
基金the Research Council of University of Guilan for the financial support of this research work
文摘Novel pyrido[2,3-d]pyrimidine derivatives were synthesized through a one-pot three-component approach using HAp-encapsulated-γ-Fe2O3[γ-Fe2O3@HAp-SO3H]catalyzed condensation of 6-arnino-2-（methylthio or ethylthio）pyrimidin-4（3H）-one,Meldrum＇s acid and aryl aldehydes at 60 ℃ and under solvent-free conditions.In this protocol the use of nanocatalyst provided a green,useful and rapid method to generate the products in short reaction times and excellent yields（88%-94%）.
基金support from the Jiangsu Province Dual Creative Phds Program(JSSCBS20210400)the Jiangsu Specially-Appointed Professors Program.
文摘Encapsulation of Fe nanoparticles in zeolite is a promising way to significantly improve the catalytic activity and stability of Fe-based catalysts during the degradation process of organic pollutants.Herein,Fe nanocatalysts were encapsulated into silicalite-1(S-1)zeolite by using a ligand-protected method(with dicyandiamide(DCD)as a organic ligand)under direct hydrothermal synthesis condition.High-resolution transmission electron microscopy(HRTEM)results confirmed the high dispersion of Fe nanocatalysts which were successfully encapsulated within the voids among the primary particles of the S-1 zeolite.The developed S-1 zeolite encapsulated Fe nanocatalyst(Fe@S-1)exhibited significantly improved catalytic activity and reusability in the catalytic degradation process of methylene blue(MB).Specifically,the developed Fe0.021@S-1 catalyst showed high catalytic degradation activity,giving a high MB degradation efficiency of 100%in 30 min,outperformed the conventional impregnated catalyst(Fe/S-1).Moreover,the Fe@S-1 catalyst afforded an outstanding stability,showing only ca.7.9%activity loss after five cycling tests,while the Fe/S-1 catalyst presented a significantly activity loss of 50.9%after only three cycles.Notably,the encapsulation strategy enabled a relatively lower Fe loading in the Fe@S-1 catalyst in comparison with that of the Fe/S-1 catalyst,i.e.,0.35%vs.0.81%(mass).Radical scavenging experiments along with electron spin resonance(ESR)measurements confirmed that the major role ofOH in the MB degradation process.Specifically,Fe@S-1 catalyst with high molar ratio of[Fe(DCD)]Cl3 is beneficial to form Fe complexes/nanoclusters in the voids(which has large pore size of 1–2 nm)among the primary particles of the zeolite,and thus improving the diffusion and accessibility of reactants to Fe active sites,and thus exhibiting a relatively higher degradation efficiency.This work demonstrates that zeolite-encapsulated Fe nanocatalysts present potential applications in the advanced oxidation of wastewater treatment.
基金supported by the National Natural Science Foundation of China(Nos.21506174,21406039)the Fundamental Research Funds for the Central Universities,Southwest Minzu University(2020NYBPY04)+1 种基金the China Scholarship Council Program(201908510082)Guangdong Natural Science Foundation(2017A030307038)。
文摘Heterogeneous Pd nanocatalysts are efficient catalysts for the Heck reaction but require multi-step,sophisticated procedures and harsh reaction conditions.In this work,a green and facile strategy has been developed to decorate Pd nanoparticles on polydopamine(PDA)-coated multi-walled carbon nanotubes(Pd/CNTs-PDA)via a one-pot method.The obtained nanoparticles were characterized by various techniques including transmission electron microscopy,X-ray diffraction,and X-ray photoelectron spectroscopy,which proved that Pd NPs are well-dispersed on the PDA and between the surfaces of the PDA and CNTs.The resultant Pd/CNTs-PDA catalysts exhibit excellent catalytic reactivity toward the Heck reaction at low temperatures.Moreover,by DFT simulation,we found that during the PDA polymerization process,a large number of unsaturated—N=and C=O species are more active than the groups on the PDA end product to anchor Pd NPs.The results provide evidence that the catalyst synthesized by the onepot method exhibited good activity because sufficient active sites could be created to effectively promote Pd NPs dispersion during the dopamine polymerization process.Additionally,the Pd/CNTs-PDA catalyst was successfully employed in Heck cross-coupling reactions with various functionalized substrates.This method opens a window for the fabrication of high-performance nanocomposite catalysts under mild conditions using simple methods and has several potential applications.
文摘The Li/MgO catalyst and nanocatalyst were prepared by the incipient wetness impregnation and sol-gel method, respectively. The catalytic performance of the Li/MgO catalyst and nanocatalyst on oxidative coupling of methane was compared. The catalysts prepared in two ways were characterized by X-ray powder diffraction, Brunauer-Emmett-Teller surface and transmission electron microscope. The catalyst was tested at temperature of 973-1073 K with constant total pressure of 101 kPa. Experimental results showed that Li/MgO nanocatalyst in the oxidative coupling of methane would result in higher conversion of methane, higher selectivity, and higher yield of main products （ethane and ethylene） compared to ordinary catalyst. The results show the improved influence of nanoscale Li/MgO catalyst performance on oxidative coupling of methane.
基金supported by the National key research and development program of China (No.2016YFC04007022)the National Natural Science Foundation of China (No.21377041)the Guangdong Science and Technology Program (No.2020B121201003)。
文摘The multiple metal catalyst as a promising nanomaterial has shown excellent activity in the peroxymonosulfate(PMS)activation for pollutant degradation.However,the role of special sites and in-depth understanding of the PMS activation mechanism are not fully studied.In this study,a Cu-doped CoFe_(2)O_(4)nanocatalyst(0.5CCF)was synthesized by a sol-gel and calcination method,and used for PMS activation to remove Rhodamine B(RhB).The results showed that the Cu doping obviously enhanced the catalytic performance of CoFe_(2)O_(4),with 99.70%of RhB removed by 0.5CCF while 74.91%in the CoFe_(2)O_(4)within 15 min.Based on the X-ray photoelectron spectroscopy and electrochemical analysis,this could be ascribed to the more low valence of Co and Fe species generated on the 0.5CCF and faster electron transfers occurred in the 0.5CCF due to the Cu doping.In addition,Cu doping could provide more reaction sites for the 0.5CCF to activate PMS for RhB removal.The metal species and the surface hydroxyl were the reaction sites of PMS activation,and the surface hydroxyl played an important role in surface-bound reactive species generation.During the PMS activation,the Cu not only activated PMS to produce reactive oxygen species(ROS),but also regenerated Co^(2+)and Fe^(2+)to accelerate the PMS activation.The non-radical of ^(1)O_(2)was the main ROS with a 99.35%of contribution rate,and the SO_(5)^(·–)self-reaction was its major source.This study provides a new insight to enhance the PMS activation performance of multiple metal catalysts by Cu doping in wastewater treatment.
基金supported by Fatih University under BAP(Grant No:P50021301-Y(3146)
文摘This paper reports a stable heterogeneous nanoparticles catalyst MnFe2O4@PANI@Ag for the degradation of azo dyes. In this synthesizing method, MnFe204 is used as magnetic core and polyaniline （PANI） a linker to stabilize the Ag nanoparticles （NPs） on the surface of catalyst. The method has a high ability to prevent Ag NPs from aggregation on the PANI surface, thus resulting in small size and highly dispersed Ag NPs. The composition and nano-structural features of polycrystalline sample were studied by X-ray powder diffractometry, Fourier transform infrared spectroscopy, and scanning electron microsco- py. Vibrating sample magnetometer measurements proved the super-paramagnetic property of the catalyst, and UV results demonstrated that MnFe2O4@PANI@Ag has a high ability to reduce the azo dyes, which come from industrial wastes in the form of pollutant. The nanocomposites could be readily separated by magnet and reused for the next four reductions with high generation efficiency.
