The water gas shift(WGS) reaction is a standard reaction that is widely used in industrial hydrogen production and removal of carbon monoxide. The improved catalytic performance of WGS reaction also contributes to amm...The water gas shift(WGS) reaction is a standard reaction that is widely used in industrial hydrogen production and removal of carbon monoxide. The improved catalytic performance of WGS reaction also contributes to ammonia synthesis and other reactions. Advanced catalysts have been developed for both high and low-temperature reactions and are widely used in industry. In recent years, supported metal nanoparticle catalysts have been researched due to their high metal utilization. Low-temperature catalysts have shown promising results, including high selectivity, high shift rates, and higher activity potential. Additionally, significant progress has been made in removing trace CO through the redox reaction in electrolytic cell. This paper reviews the development of WGS reaction catalysts, including the reaction mechanism, catalyst design, and innovative research methods. The catalyst plays a crucial role in the WGS reaction, and this paper provides an instant of catalyst design under different conditions. The progress of catalysts is closely related to the development of advanced characterization techniques.Furthermore, modifying the catalyst surface to enhance activity and significantly increase reaction kinetics is a current research direction. This review goals to stimulate a better understanding of catalyst design, performance optimization, and driving mechanisms, leading to further progress in this field.展开更多
Efficient sterilization by a plasma photocatalytic system(PPS)requires strong synergy between plasma and photocatalyst to inactivate microorganisms while suppressing the formation of secondary pollutants.Here,we repor...Efficient sterilization by a plasma photocatalytic system(PPS)requires strong synergy between plasma and photocatalyst to inactivate microorganisms while suppressing the formation of secondary pollutants.Here,we report that a PPS constructed from a needle array corona discharge and Au/TiO2plasmonic nanocatalyst could remarkably improve the sterilization of Escherichia coli(E.coli)and alleviate formation of the discharge pollutant O3.At 6 kV,the combination of corona discharge and Au/TiO2achieves sterilization efficiency of 100%within an exposure time of 5 min.At 5 kV and an exposure time of 8 min,the presence of Au/TiO2improves sterilization efficiency of the corona discharge from 73%to 91%and reduces the O3concentration from 0.38 to 0.04 ppm,whereas the presence of TiO2reduces the sterilization efficiency and O3concentration to 66%and 0.17 ppm,respectively.The Au/TiO2in the PPS enables a uniform corona discharge,enhances the interaction between plasma,E.coli and nanocatalysts,and suppresses the formation of O3.Further,the Au/TiO2can be excited by ultraviolet-visible light emitted from the plasma to generate electron-hole pairs,and thus contributes to the formation of reactive radicals and the oxidative inactivation of E.coli.The PPS constructed from a needle array corona discharge and Au-based plasmonic nanocatalyst provides a promising approach for developing high-efficiency sterilization techniques.展开更多
Efficient use of energy is a pressing issue.Improvement of chemical processes is currently an important target for energy efficiency.Although chemical processes are independent of pathways with respect to the final en...Efficient use of energy is a pressing issue.Improvement of chemical processes is currently an important target for energy efficiency.Although chemical processes are independent of pathways with respect to the final energy output or consumption,the application of catalysts can reduce involved activation energies considerably and therefore save large amounts of energy.展开更多
Currently,under huge pressure from energy demands and environmental problems,much attention is being paid to biomass conversion,which will play an important role in meeting the requirements for a sustainable society.A...Currently,under huge pressure from energy demands and environmental problems,much attention is being paid to biomass conversion,which will play an important role in meeting the requirements for a sustainable society.As the most abundant biomass on earth, cellulose is usually used as the first research target for biomass conversion.In this review,the recalcitrant structure of cellulose is discussed and non-catalytic hydrolysis by hot-compressed water and catalytic hydrolysis using solid acids are then considered.We also review the catalytic conversion of cellulose into valuable chemicals including hexitols(sorbitol and mannitol),ethylene glycol,and related compounds using various heterogeneous catalysts.展开更多
Surface-functionalized nitrogen/carbon co-doped polymorphic TiO_(2) phase junction nanoparticles uniformly distributed in porous carbon matrix were synthesized by a simple one-step pyrolysis of titanium based metal-or...Surface-functionalized nitrogen/carbon co-doped polymorphic TiO_(2) phase junction nanoparticles uniformly distributed in porous carbon matrix were synthesized by a simple one-step pyrolysis of titanium based metal-organic framework(MOF),NH_(2)-MIL^(-1)25(Ti) at 700℃ under water vapour atmosphere.Introducing water vapour during the pyrolysis of NH_(2)-MIL^(-1)25(Ti) not only functionalizes the derived porous carbon matrix with carboxyl groups but also forms additional oxygen-rich N like interstitial/intraband states lying above the valence band of TiO2 along with the self-doped carbo n,which further narrows the energy band gaps of polymorphic TiO2 nanoparticles that enhance photocatalytic charge transfer efficiency.Without co-catalyst,sample N-C-TiO2/CArW demonstrates H_(2) evolution activity of 426 μmol gcat-1h^(-1),which remarkably outperforms commercial TiO_(2)(P-25) and N-C-TiO_(2)/CAr with a 5-fold and 3-fold H_(2) generation,respectively.This study clearly shows that water vapour atmosphere during the pyrolysis increases the hydrophilicity of the Ti-MOF derived composites by functionalizing porous carbon matrix with carboxylic groups,as well as enhancing the electrical conductivity and charge transfer efficiency due to the formation of additional localized oxygen-rich N like interstitial/intraband states.This work also demonstrates that by optimizing the anatase-rutile phase composition of the TiO2 polymorphs,tuning the energy band gaps by N/C co-doping and functionalizing the porous carbon matrix in the N-C-TiO2/C nanocomposites,the photocatalytic H_(2) generation activity can be further enhanced.展开更多
Cellulose is a renewable biomass material and natural polymer which is abundantly available on Earth,and includes agricultural wastes,forestry residues,and woody materials.The excellent and smart characteristics of ce...Cellulose is a renewable biomass material and natural polymer which is abundantly available on Earth,and includes agricultural wastes,forestry residues,and woody materials.The excellent and smart characteristics of cellulose materials,such as lightweight,biocompatibility,biodegradability,high mechanical strength/stiffness and low thermal expansibility,have made cellulose a highpotential material for various industry applications.Cellulose has recently been discovered as a smart material in the electroactive polymers family which carries the name of cellulose-based electroactive paper(EAPap).The shear piezoelectricity in cellulose polymers is able to induce large displacement output,low actuation voltage,and low power consumption in the application of biomimetic sensors/actuators and electromechanical system.The present study provides an overview of biomass pretreatment from various lignocellulosic cellulose(LC)resources and nanocellulose production via TEMPO-mediated oxidation reaction,followed by the production of different types of EAPap versus its performance,and lastly the applications of EAPap in different areas and industries.Specifically,LC biomass consists mainly of cellulose having a small content of hemicelluloses and lignins which form a defensive inner structure against the degradation of plant cell wall.Thus,selective approaches are discussed to ensure proper extraction of cellulosic fibers from complex biomass for further minimization to nano-dimensions.In addition,a comprehensive review of the development of cellulose-based EAPap as well as fabrication,characterization,performance enhancement and applications of EAPap devices are discussed herein.展开更多
The interfacial perimeter of gold nanocatalysts is popularly viewed as the active sites for a number of chemical reactions,while the geometrical structure of the interface at atomic scale is less known.Here,TiO2-nanos...The interfacial perimeter of gold nanocatalysts is popularly viewed as the active sites for a number of chemical reactions,while the geometrical structure of the interface at atomic scale is less known.Here,TiO2-nanosheets and nanospindles were adapted to accommodate Au particles(~2.2 nm),forming Au-TiO2{001}and Au-TiO2{101}interfaces.Upon calcination at 623 K in air,HAADF-STEM images evidenced that the Au particles on TiO2{101}enlarged to 3.1 nm and these on TiO2{001}remained unchanged,suggesting the stronger metal-support interaction on TiO2{001}.Au/TiO2{001}was more active for CO oxidation than Au/TiO2{101}system.展开更多
With the increasingly stringent standards for limiting sulfide content in liquid fuels,oxidative desulfurization(ODS)has become a promising ultra-deep desulfurization process in fuel desulfurization.TS-1 zeolites show...With the increasingly stringent standards for limiting sulfide content in liquid fuels,oxidative desulfurization(ODS)has become a promising ultra-deep desulfurization process in fuel desulfurization.TS-1 zeolites show great potential as catalysts for ODS reactions,due to its remarkable oxidation activity at low temperatures and pressure.However,the inherent microporous structure of conventional TS-1 zeolites restricts the mass transportation and renders the active sites in the microporous space of TS-1 zeolites inaccessible for bulky aromatic organosulfur compounds.Fabrication of hierarchical TS-1 zeolites by incorporating meso-/macropores into microporous TS-1 zeolites is an effective strategy to improve mass transportability.In recent years,abundant efforts have been dedicated to developing synthetic strategies of hierarchical TS-1 zeolite,thereby improving its catalytic performance in the ODS process.This mini-review addresses the synthetic methods of hierarchical TS-1 catalysts and their catalytic performance in the ODS reactions.In addition,some current problems and prospects of synthesis routes for constructing hierarchical TS-1 catalysts have also been revised.We expect this mini-review to shed light on the more efficient preparation strategies of hierarchical TS-1 zeolites for the ODS process.展开更多
We used a dielectric barrier discharge(DBD)plasma technique to eliminate the protective ligand of ZnAl-hydrotalcite-supported gold nanoclusters.We used X-ray powder diffraction,ultraviolet-visible spectrophotometry,th...We used a dielectric barrier discharge(DBD)plasma technique to eliminate the protective ligand of ZnAl-hydrotalcite-supported gold nanoclusters.We used X-ray powder diffraction,ultraviolet-visible spectrophotometry,thermogravimetric analysis,and high angle annular dark-field-scanning transmission electron microscopy characterization to show that the samples pretreated with/without DBD-plasma displayed different performances in CO oxidation.The enhanced activity was obtained on the plasma-treated samples,implying that the protective ligand was effectively removed via the plasma technique.The crystal structure of the plasma-treated samples changed markedly,suggesting that the plasma treatment could not only break the chemical bond between the gold and the protective agent but could also decompose the interlayer ions over the hydrotalcite support.The particle sizes of the gold after DBD-plasma treatment implied that it was a good way to control the size of the gold nanoparticles under mild conditions.展开更多
Objective:To investigate the prevalence of Cryptosporidium spp.in goat kids in selected areas of Bangladesh and to elucidate the potential zoonotic hazards.Methods:In the present study,we have used Ziehl-Neelsen stain...Objective:To investigate the prevalence of Cryptosporidium spp.in goat kids in selected areas of Bangladesh and to elucidate the potential zoonotic hazards.Methods:In the present study,we have used Ziehl-Neelsen staining and nested PCR approach to identify and characterize the Cryptosporidium sp.from diarrhoeic feces of goat kids.A total of 100 diarrhoeic feces samples were collected from Chittagong region in Southern Bangladesh.For nested PCR analysis,specific primers for amplification of 581 base pair fragments of 18 S rRNA gene were used.Results:A total of 15%and 3%samples were found positive in microscopic study and in nested PCR analysis respectively.Phylogenetic analysis of sequence data showed similarity with that of Cryptosporidium xiaoi recorded from sheep and goat.Conclusions:To our knowledge,this is the first report of Cryptosporidium xiaoi responsible for diarrhoea in goat kids in Bangladesh.Further study can highlight their zoonotic significance along with genetic diversity in other host species inside the country.展开更多
Macroscopic SiO2 spheres with a homogeneous amine distribution were synthesized by a one-step emulsion based synthesis approach in a flow column reactor. The CO2 adsorption capacity of the nanostructured amine-functio...Macroscopic SiO2 spheres with a homogeneous amine distribution were synthesized by a one-step emulsion based synthesis approach in a flow column reactor. The CO2 adsorption capacity of the nanostructured amine-functionalized silica spheres was studied in absence and presence of H2O. The structural properties were adjusted by varying solvents and surfactants during the synthesis and, at constant amine loadings, were found to be the main factor for influencing the CO2 sorption capacities. Under water-free conditions CO2 is bound to the amino groups via the formation of carbamates, which require two neighboring amino groups to adsorb one CO2 molecule. At constant amine concentrations sorbents with lower surface area allow to establish a higher amine density on the surface, which enhances the CO2 uptake capacities under dry conditions. In presence of H2O the CO2 adsorption changes to 1：1 stoichiometry due to stabilization of carbamates by protonation of H2O and formation of further species such as bicarbonates, which should in principle double the adsorption capacities. Low concentrations of physisorbed H2O（0.3 mmol/g） did not impair the adsorption capacity of the adsorbents for CO2, while at higher water uptakes（0.6 and 1.1 mmol/g） the CO2 uptake is reduced, which could be attributed to capillary condensation of H2O or formation of bulky reaction products blocking inner pores and access to active sites.展开更多
The influence of adding Fe, Cr, Co, and Ga into 3%Mo/HZSM-5 catalyst on methane aromatization, and the influence of additives ratio on methane conversion, selectivity to hydrocarbons and coke, as well as distribution ...The influence of adding Fe, Cr, Co, and Ga into 3%Mo/HZSM-5 catalyst on methane aromatization, and the influence of additives ratio on methane conversion, selectivity to hydrocarbons and coke, as well as distribution of aromatics were investigated. The experimental results showed that the addition of Fe, Cr, Co and Ga promoted the dehydrogenation and dissociation of methane. The results of NH3-TPD indicated that the acidity of HZSM-5 was changed by adding Fe and Co components, consequently the catalytic properties of Mo/HZSM-5 were changed. It was also revealed that strong acid sites were the center of methane aromatization. The results of XRD characterization showed that the crystallinity of Mo on ZSM-5 zeolite was increased after adding Fe, Co additives.展开更多
We have directly investigated the chemical state of the Pd species in a real l-gas sensor device by examining the l-fluorescence X-ray absorption fine structure. The l-gas sensor device was heavily damaged by a heatin...We have directly investigated the chemical state of the Pd species in a real l-gas sensor device by examining the l-fluorescence X-ray absorption fine structure. The l-gas sensor device was heavily damaged by a heating process in which the temperature was ill-controlled, resulting in decrease of methane selectivity. We found that the Pd O in the fresh l-gas sensor was reduced to Pd metal particles as the methane selectivity decreased. Based on the investigation results, we modified the device structure so as to heat up homogeneously. The lifetime of the sensor was then successfully increased by more than 5 years.展开更多
Three new copper（Ⅰ） complexes, namely [Cu（DPEphos）（Biq）]CF3SO3（1） and [Cu（PPh3）2（Biq）]CF3SO3（2） and [Cu（PPh3）2（Biq）]ClO4（3）（DPEphos = bis[2-（diphenylphosp hino）phenyl]ether, PPh3 = triphenylpho...Three new copper（Ⅰ） complexes, namely [Cu（DPEphos）（Biq）]CF3SO3（1） and [Cu（PPh3）2（Biq）]CF3SO3（2） and [Cu（PPh3）2（Biq）]ClO4（3）（DPEphos = bis[2-（diphenylphosp hino）phenyl]ether, PPh3 = triphenylphosphine and Biq = 2,2A-biquinoline）, are synthesized and characterized by IR, ~1H NMR, ^（31） P NMR, fluorescence spectra and terahertz time-domain spectroscopy（THz-TDS）. Complex 1 crystallizes in triclinic, space group P1 with a = 12.6997（5）, b = 13.2813（5）, c = 15.3593（6） A, α = 80.211（3）°, β = 88.752（3）°, γ = 70.113（3）°, V = 2398.85（15） A^3, C（55）H（41.2）CuF3N2O（4.6）P2S, Mr = 1018.27, Z = 2, Dc = 1.410 g/cm3, F（000） = 1048, μ = 0.628 mm-1, the final R = 0.0450 and w R = 0.1105 for 9419 observed reflections（I 〉 2σ（I））. Complex 2 crystallizes in monoclinic, space group C2/c with a = 19.9961（7）, b = 15.9774（5）, c = 17.7908（6） A, β = 119.758（4）°, V = 4982.8（3） A^3, C（56.47）H（47.88）CuF3N2O（4.47）P2S, Mr = 1040.54, Z = 4, Dc = 1.387 g/cm^3, F（000） = 2154, μ = 0.606 mm-1, the final R = 0.0430 and w R = 0.1218 for 4897 observed reflections（I 〉 2σ（I））. Complex 3 crystallizes in monoclinic, space group C2/c with a = 19.7534（8）, b = 15.0797（5）, c = 17.8097（7） A, β = 116.400（5）°, V = 4751.8（3） A^3, C（56）H（45）ClCuN3O4P2, Mr = 984.88, Z = 4, Dc = 1.377 g/cm^3, F（000） = 2040, μ = 0.635 mm-1, the final R = 0.0731 and w R = 0.2180 for 4670 observed reflections（I 〉 2σ（I））. In the emission spectra, shifts of emission peak are derived from ligand-centered（π-π＊） transition.展开更多
Date palm fiber(DPF)derived from agrowaste was utilized as a new precursor for the optimized synthesis of a costeffective,nanostructured,powderactivated carbon(nPAC)for aluminum(Al3+)removal from aqueous solutions usi...Date palm fiber(DPF)derived from agrowaste was utilized as a new precursor for the optimized synthesis of a costeffective,nanostructured,powderactivated carbon(nPAC)for aluminum(Al3+)removal from aqueous solutions using carbonization,KOH activation,response surface methodology(RSM)and central composite design(CCD).The optimum synthesis condition,activation temperature,time and impregnation ratio were found to be 650℃,1.09 hour and 1:1,respectively.Furthermore,the optimum conditions for removal were 99.5%and 9.958 mgg 1 in regard to uptake capacity.The optimum conditions of nPAC was analyzed and characterized using XRD,FTIR,FESEM,BET,TGA and Zeta potential.Moreover,the adsorption of the Al3+conditions was optimized with an integrated RSMCCD experimental design.Regression results revealed that the adsorption kinetics data was well fitted by the pseudosecond order model,whereas the adsorption isotherm data was best represented by the Freundlich isotherm model.Optimum activated carbon indicated that DPF can serve as a costeffective precursor adsorbent for Al^(3+)removal.展开更多
Interfacial reactions in lithium-ion batteries often involve gaseous reaction products.Mechanistic investigation of material degradation processes requires a technique to identify and quantify these gases in battery c...Interfacial reactions in lithium-ion batteries often involve gaseous reaction products.Mechanistic investigation of material degradation processes requires a technique to identify and quantify these gases in battery cells.Online electrochemical mass spectrometry(OEMS)is an operando gas analysis method that continuously samples the headspace of a custom battery cell.Real-time gas analysis by quantitative OEMS was used to create mechanistic understanding of battery degradation reactions,some of which will be highlight in this article.展开更多
To study the effect of adjacent hydroxyl to the active sites, several acid catalysts, i.e. substituted benzoic acids with adjacent carboxyl are employed in the fructose dehydration to 5-hydroxymethylfurfural(HMF).Expe...To study the effect of adjacent hydroxyl to the active sites, several acid catalysts, i.e. substituted benzoic acids with adjacent carboxyl are employed in the fructose dehydration to 5-hydroxymethylfurfural(HMF).Experimental results reveal that Br?nsted acid sites with adjacent carboxyl present higher catalytic ability than isolated ones. Computational results suggest that the adjacent sites lead to co-interaction on fructose, corresponding more stable transition state and faster HMF formation rate. Based on the enhancement from the adjacent sites, a novel ordered mesoporous carbon(OMC) full of carboxyls in surface is prepared and turns out to be an effective solid catalyst for HMF production from fructose derived from biomass.展开更多
In this work, the magnesium aluminum spinel (MgAl2O4) was prepared by Mg and Al as precursors through a method of sol-gel subsequent with high temperature calcination. The wide range of synthetic conditions, including...In this work, the magnesium aluminum spinel (MgAl2O4) was prepared by Mg and Al as precursors through a method of sol-gel subsequent with high temperature calcination. The wide range of synthetic conditions, including organic alcohols, ammonia content, dispersant, alkoxide concentration, hydrolysis time, hydrolysis temperature and calcination temperature were screened over as-prepared samples. This work provides a necessary experimental basis for the synthesis of MgAl2O4 with uniform particle size of spherical structure, which has a potential to be used in many industrial and military applications.展开更多
Gold clusters and small nanoparticles supported on metal oxides could be prepared by deposition‐precipitation followed by microwave irradiation as a drying method and then calcination.The drying method influenced the...Gold clusters and small nanoparticles supported on metal oxides could be prepared by deposition‐precipitation followed by microwave irradiation as a drying method and then calcination.The drying method influenced the size of the Au particles.Au(III)was partly reduced during conventional oven drying,resulting in Au aggregates.In contrast,Au(III)was preserved during microwave drying owing to rapid and uniform heating,and the Au diameter was minimized to1.4nm on Al2O3.This method can be applied to several metal oxide supports having different microwave absorption efficiencies,such as MnO2,Al2O3,and TiO2.These catalysts exhibited higher catalytic activities for CO oxidation at low temperature and for selective aerobic oxidation of sulfide than those prepared by conventional methods.展开更多
In this study, the effects of pre-carburization of catalyst, hydrogen addition to methane feed and the space velocity of methane on the catalytic performance in methane to benzene （MTB） reaction were discussed in de...In this study, the effects of pre-carburization of catalyst, hydrogen addition to methane feed and the space velocity of methane on the catalytic performance in methane to benzene （MTB） reaction were discussed in detail over Mo/HZSM-5 catalyst at 1023 K and 0.3 MPa. Compared with the non-precarburized catalyst, the Mo catalyst pre-carburized under the flow of CHa＋4H2 at 973 K was found to have the higher activity and better stability. Further 6% H2 addition to the methane feed suppressed the aromatic type of coke formation effectively, and improved the stability of catalyst markedly, moreover gave a much longer reaction life of catalyst （53 h at 1023 K and 5400 ml/（g-h）） and much more formation amounts of benzene and hydrogen. With increase of methane space velocity, both the naphthalene formation selectivity and the coke formation selectivity were decreased by the shortened contact time; the benzene formation selectivity and total formation amount before the complete deactivation of catalyst were increased markedly, while the total naphthalene and coke formation amounts did not change much. At high methane space velocity （≥5400 ml/（g·h））, a new middle temperature coke derived from the high temperature aromatic coke was formed on the catalyst; all the coke formed could be burnt off at lower temperature in oxygen, compared with those obtained at low space velocity. Considering the benzene formation amount and catalyst stability together, 5400 ml/（g·h） was proved to be the most efficient methane space velocity for benzene production.展开更多
基金financially supported by the National Natural Science Foundation of China (22279118, 22279117, 22075254,31901272)the Top-Notch Talent Program of Henan Agricultural University (30501034)。
文摘The water gas shift(WGS) reaction is a standard reaction that is widely used in industrial hydrogen production and removal of carbon monoxide. The improved catalytic performance of WGS reaction also contributes to ammonia synthesis and other reactions. Advanced catalysts have been developed for both high and low-temperature reactions and are widely used in industry. In recent years, supported metal nanoparticle catalysts have been researched due to their high metal utilization. Low-temperature catalysts have shown promising results, including high selectivity, high shift rates, and higher activity potential. Additionally, significant progress has been made in removing trace CO through the redox reaction in electrolytic cell. This paper reviews the development of WGS reaction catalysts, including the reaction mechanism, catalyst design, and innovative research methods. The catalyst plays a crucial role in the WGS reaction, and this paper provides an instant of catalyst design under different conditions. The progress of catalysts is closely related to the development of advanced characterization techniques.Furthermore, modifying the catalyst surface to enhance activity and significantly increase reaction kinetics is a current research direction. This review goals to stimulate a better understanding of catalyst design, performance optimization, and driving mechanisms, leading to further progress in this field.
基金National Natural Science Foundation of China(Nos.52041001,21808024)Natural Science Foundation of Liaoning Province(No.2020-MS-126)Special Foundation for Key Fields of Colleges and Universities in Guangdong Province(No.2021ZDZX4094)。
文摘Efficient sterilization by a plasma photocatalytic system(PPS)requires strong synergy between plasma and photocatalyst to inactivate microorganisms while suppressing the formation of secondary pollutants.Here,we report that a PPS constructed from a needle array corona discharge and Au/TiO2plasmonic nanocatalyst could remarkably improve the sterilization of Escherichia coli(E.coli)and alleviate formation of the discharge pollutant O3.At 6 kV,the combination of corona discharge and Au/TiO2achieves sterilization efficiency of 100%within an exposure time of 5 min.At 5 kV and an exposure time of 8 min,the presence of Au/TiO2improves sterilization efficiency of the corona discharge from 73%to 91%and reduces the O3concentration from 0.38 to 0.04 ppm,whereas the presence of TiO2reduces the sterilization efficiency and O3concentration to 66%and 0.17 ppm,respectively.The Au/TiO2in the PPS enables a uniform corona discharge,enhances the interaction between plasma,E.coli and nanocatalysts,and suppresses the formation of O3.Further,the Au/TiO2can be excited by ultraviolet-visible light emitted from the plasma to generate electron-hole pairs,and thus contributes to the formation of reactive radicals and the oxidative inactivation of E.coli.The PPS constructed from a needle array corona discharge and Au-based plasmonic nanocatalyst provides a promising approach for developing high-efficiency sterilization techniques.
基金The National Natural Science Foundation of China(22078317)。
文摘Efficient use of energy is a pressing issue.Improvement of chemical processes is currently an important target for energy efficiency.Although chemical processes are independent of pathways with respect to the final energy output or consumption,the application of catalysts can reduce involved activation energies considerably and therefore save large amounts of energy.
基金supported by the Grant-in-Aid for Scientific Research(KAKENHI,20226016)from the Japan Society for the Promotion of Science(JSPS)
文摘Currently,under huge pressure from energy demands and environmental problems,much attention is being paid to biomass conversion,which will play an important role in meeting the requirements for a sustainable society.As the most abundant biomass on earth, cellulose is usually used as the first research target for biomass conversion.In this review,the recalcitrant structure of cellulose is discussed and non-catalytic hydrolysis by hot-compressed water and catalytic hydrolysis using solid acids are then considered.We also review the catalytic conversion of cellulose into valuable chemicals including hexitols(sorbitol and mannitol),ethylene glycol,and related compounds using various heterogeneous catalysts.
基金EPSRC CDT in Metamaterials at University of Exeter and Leverhulme Trust(RPG-2018-320) for financial support。
文摘Surface-functionalized nitrogen/carbon co-doped polymorphic TiO_(2) phase junction nanoparticles uniformly distributed in porous carbon matrix were synthesized by a simple one-step pyrolysis of titanium based metal-organic framework(MOF),NH_(2)-MIL^(-1)25(Ti) at 700℃ under water vapour atmosphere.Introducing water vapour during the pyrolysis of NH_(2)-MIL^(-1)25(Ti) not only functionalizes the derived porous carbon matrix with carboxyl groups but also forms additional oxygen-rich N like interstitial/intraband states lying above the valence band of TiO2 along with the self-doped carbo n,which further narrows the energy band gaps of polymorphic TiO2 nanoparticles that enhance photocatalytic charge transfer efficiency.Without co-catalyst,sample N-C-TiO2/CArW demonstrates H_(2) evolution activity of 426 μmol gcat-1h^(-1),which remarkably outperforms commercial TiO_(2)(P-25) and N-C-TiO_(2)/CAr with a 5-fold and 3-fold H_(2) generation,respectively.This study clearly shows that water vapour atmosphere during the pyrolysis increases the hydrophilicity of the Ti-MOF derived composites by functionalizing porous carbon matrix with carboxylic groups,as well as enhancing the electrical conductivity and charge transfer efficiency due to the formation of additional localized oxygen-rich N like interstitial/intraband states.This work also demonstrates that by optimizing the anatase-rutile phase composition of the TiO2 polymorphs,tuning the energy band gaps by N/C co-doping and functionalizing the porous carbon matrix in the N-C-TiO2/C nanocomposites,the photocatalytic H_(2) generation activity can be further enhanced.
文摘Cellulose is a renewable biomass material and natural polymer which is abundantly available on Earth,and includes agricultural wastes,forestry residues,and woody materials.The excellent and smart characteristics of cellulose materials,such as lightweight,biocompatibility,biodegradability,high mechanical strength/stiffness and low thermal expansibility,have made cellulose a highpotential material for various industry applications.Cellulose has recently been discovered as a smart material in the electroactive polymers family which carries the name of cellulose-based electroactive paper(EAPap).The shear piezoelectricity in cellulose polymers is able to induce large displacement output,low actuation voltage,and low power consumption in the application of biomimetic sensors/actuators and electromechanical system.The present study provides an overview of biomass pretreatment from various lignocellulosic cellulose(LC)resources and nanocellulose production via TEMPO-mediated oxidation reaction,followed by the production of different types of EAPap versus its performance,and lastly the applications of EAPap in different areas and industries.Specifically,LC biomass consists mainly of cellulose having a small content of hemicelluloses and lignins which form a defensive inner structure against the degradation of plant cell wall.Thus,selective approaches are discussed to ensure proper extraction of cellulosic fibers from complex biomass for further minimization to nano-dimensions.In addition,a comprehensive review of the development of cellulose-based EAPap as well as fabrication,characterization,performance enhancement and applications of EAPap devices are discussed herein.
基金supported by Liaoning Revitalization Talents Program (XLYC1807121)National Natural Science Foundation of China (20673054)~~
文摘The interfacial perimeter of gold nanocatalysts is popularly viewed as the active sites for a number of chemical reactions,while the geometrical structure of the interface at atomic scale is less known.Here,TiO2-nanosheets and nanospindles were adapted to accommodate Au particles(~2.2 nm),forming Au-TiO2{001}and Au-TiO2{101}interfaces.Upon calcination at 623 K in air,HAADF-STEM images evidenced that the Au particles on TiO2{101}enlarged to 3.1 nm and these on TiO2{001}remained unchanged,suggesting the stronger metal-support interaction on TiO2{001}.Au/TiO2{001}was more active for CO oxidation than Au/TiO2{101}system.
基金supported by the National Natural Science Foundation of China(21971082)the Jilin Province Science and Technology Development Plan(20200201096JC and 20190201229JC)+1 种基金the China Postdoctoral Science Foundation(2019T120235 and 2018M640280)for supporting this workthe 111 Project(B17020)。
文摘With the increasingly stringent standards for limiting sulfide content in liquid fuels,oxidative desulfurization(ODS)has become a promising ultra-deep desulfurization process in fuel desulfurization.TS-1 zeolites show great potential as catalysts for ODS reactions,due to its remarkable oxidation activity at low temperatures and pressure.However,the inherent microporous structure of conventional TS-1 zeolites restricts the mass transportation and renders the active sites in the microporous space of TS-1 zeolites inaccessible for bulky aromatic organosulfur compounds.Fabrication of hierarchical TS-1 zeolites by incorporating meso-/macropores into microporous TS-1 zeolites is an effective strategy to improve mass transportability.In recent years,abundant efforts have been dedicated to developing synthetic strategies of hierarchical TS-1 zeolite,thereby improving its catalytic performance in the ODS process.This mini-review addresses the synthetic methods of hierarchical TS-1 catalysts and their catalytic performance in the ODS reactions.In addition,some current problems and prospects of synthesis routes for constructing hierarchical TS-1 catalysts have also been revised.We expect this mini-review to shed light on the more efficient preparation strategies of hierarchical TS-1 zeolites for the ODS process.
文摘We used a dielectric barrier discharge(DBD)plasma technique to eliminate the protective ligand of ZnAl-hydrotalcite-supported gold nanoclusters.We used X-ray powder diffraction,ultraviolet-visible spectrophotometry,thermogravimetric analysis,and high angle annular dark-field-scanning transmission electron microscopy characterization to show that the samples pretreated with/without DBD-plasma displayed different performances in CO oxidation.The enhanced activity was obtained on the plasma-treated samples,implying that the protective ligand was effectively removed via the plasma technique.The crystal structure of the plasma-treated samples changed markedly,suggesting that the plasma treatment could not only break the chemical bond between the gold and the protective agent but could also decompose the interlayer ions over the hydrotalcite support.The particle sizes of the gold after DBD-plasma treatment implied that it was a good way to control the size of the gold nanoparticles under mild conditions.
基金Supported by two grants(No.-09-148 RG/BIO/AS_G and No.-10-087 RG/ITC/AS_C)from the Academy of Science for the developing World(TWAS)
文摘Objective:To investigate the prevalence of Cryptosporidium spp.in goat kids in selected areas of Bangladesh and to elucidate the potential zoonotic hazards.Methods:In the present study,we have used Ziehl-Neelsen staining and nested PCR approach to identify and characterize the Cryptosporidium sp.from diarrhoeic feces of goat kids.A total of 100 diarrhoeic feces samples were collected from Chittagong region in Southern Bangladesh.For nested PCR analysis,specific primers for amplification of 581 base pair fragments of 18 S rRNA gene were used.Results:A total of 15%and 3%samples were found positive in microscopic study and in nested PCR analysis respectively.Phylogenetic analysis of sequence data showed similarity with that of Cryptosporidium xiaoi recorded from sheep and goat.Conclusions:To our knowledge,this is the first report of Cryptosporidium xiaoi responsible for diarrhoea in goat kids in Bangladesh.Further study can highlight their zoonotic significance along with genetic diversity in other host species inside the country.
基金supported by the German Research Council(DFG)within the priority program(Schwerpunktprogramm),“Poröse Medien mit definierter Porenstruktur in der Verfahrenstechnik–Modellierung,Anwendngen,Synthese”(SPP 1570)under the projects LE 1187/10 and SP 648/4the framework of the DFG Excellence Initiative the Cluster of Excellence“Engineering of Advanced Materials”(DFG EXC 415)funding via the DFG research training group GRK 1896
文摘Macroscopic SiO2 spheres with a homogeneous amine distribution were synthesized by a one-step emulsion based synthesis approach in a flow column reactor. The CO2 adsorption capacity of the nanostructured amine-functionalized silica spheres was studied in absence and presence of H2O. The structural properties were adjusted by varying solvents and surfactants during the synthesis and, at constant amine loadings, were found to be the main factor for influencing the CO2 sorption capacities. Under water-free conditions CO2 is bound to the amino groups via the formation of carbamates, which require two neighboring amino groups to adsorb one CO2 molecule. At constant amine concentrations sorbents with lower surface area allow to establish a higher amine density on the surface, which enhances the CO2 uptake capacities under dry conditions. In presence of H2O the CO2 adsorption changes to 1：1 stoichiometry due to stabilization of carbamates by protonation of H2O and formation of further species such as bicarbonates, which should in principle double the adsorption capacities. Low concentrations of physisorbed H2O（0.3 mmol/g） did not impair the adsorption capacity of the adsorbents for CO2, while at higher water uptakes（0.6 and 1.1 mmol/g） the CO2 uptake is reduced, which could be attributed to capillary condensation of H2O or formation of bulky reaction products blocking inner pores and access to active sites.
文摘The influence of adding Fe, Cr, Co, and Ga into 3%Mo/HZSM-5 catalyst on methane aromatization, and the influence of additives ratio on methane conversion, selectivity to hydrocarbons and coke, as well as distribution of aromatics were investigated. The experimental results showed that the addition of Fe, Cr, Co and Ga promoted the dehydrogenation and dissociation of methane. The results of NH3-TPD indicated that the acidity of HZSM-5 was changed by adding Fe and Co components, consequently the catalytic properties of Mo/HZSM-5 were changed. It was also revealed that strong acid sites were the center of methane aromatization. The results of XRD characterization showed that the crystallinity of Mo on ZSM-5 zeolite was increased after adding Fe, Co additives.
基金High Energy Accelerator Organization under Proposal Number 2012G680
文摘We have directly investigated the chemical state of the Pd species in a real l-gas sensor device by examining the l-fluorescence X-ray absorption fine structure. The l-gas sensor device was heavily damaged by a heating process in which the temperature was ill-controlled, resulting in decrease of methane selectivity. We found that the Pd O in the fresh l-gas sensor was reduced to Pd metal particles as the methane selectivity decreased. Based on the investigation results, we modified the device structure so as to heat up homogeneously. The lifetime of the sensor was then successfully increased by more than 5 years.
基金supported by the National Natural Science Foundation of China(Nos.21171119 and 81573822)the Beijing Municipal Natural Science Foundation(No.2172017)
文摘Three new copper（Ⅰ） complexes, namely [Cu（DPEphos）（Biq）]CF3SO3（1） and [Cu（PPh3）2（Biq）]CF3SO3（2） and [Cu（PPh3）2（Biq）]ClO4（3）（DPEphos = bis[2-（diphenylphosp hino）phenyl]ether, PPh3 = triphenylphosphine and Biq = 2,2A-biquinoline）, are synthesized and characterized by IR, ~1H NMR, ^（31） P NMR, fluorescence spectra and terahertz time-domain spectroscopy（THz-TDS）. Complex 1 crystallizes in triclinic, space group P1 with a = 12.6997（5）, b = 13.2813（5）, c = 15.3593（6） A, α = 80.211（3）°, β = 88.752（3）°, γ = 70.113（3）°, V = 2398.85（15） A^3, C（55）H（41.2）CuF3N2O（4.6）P2S, Mr = 1018.27, Z = 2, Dc = 1.410 g/cm3, F（000） = 1048, μ = 0.628 mm-1, the final R = 0.0450 and w R = 0.1105 for 9419 observed reflections（I 〉 2σ（I））. Complex 2 crystallizes in monoclinic, space group C2/c with a = 19.9961（7）, b = 15.9774（5）, c = 17.7908（6） A, β = 119.758（4）°, V = 4982.8（3） A^3, C（56.47）H（47.88）CuF3N2O（4.47）P2S, Mr = 1040.54, Z = 4, Dc = 1.387 g/cm^3, F（000） = 2154, μ = 0.606 mm-1, the final R = 0.0430 and w R = 0.1218 for 4897 observed reflections（I 〉 2σ（I））. Complex 3 crystallizes in monoclinic, space group C2/c with a = 19.7534（8）, b = 15.0797（5）, c = 17.8097（7） A, β = 116.400（5）°, V = 4751.8（3） A^3, C（56）H（45）ClCuN3O4P2, Mr = 984.88, Z = 4, Dc = 1.377 g/cm^3, F（000） = 2040, μ = 0.635 mm-1, the final R = 0.0731 and w R = 0.2180 for 4670 observed reflections（I 〉 2σ（I））. In the emission spectra, shifts of emission peak are derived from ligand-centered（π-π＊） transition.
文摘Date palm fiber(DPF)derived from agrowaste was utilized as a new precursor for the optimized synthesis of a costeffective,nanostructured,powderactivated carbon(nPAC)for aluminum(Al3+)removal from aqueous solutions using carbonization,KOH activation,response surface methodology(RSM)and central composite design(CCD).The optimum synthesis condition,activation temperature,time and impregnation ratio were found to be 650℃,1.09 hour and 1:1,respectively.Furthermore,the optimum conditions for removal were 99.5%and 9.958 mgg 1 in regard to uptake capacity.The optimum conditions of nPAC was analyzed and characterized using XRD,FTIR,FESEM,BET,TGA and Zeta potential.Moreover,the adsorption of the Al3+conditions was optimized with an integrated RSMCCD experimental design.Regression results revealed that the adsorption kinetics data was well fitted by the pseudosecond order model,whereas the adsorption isotherm data was best represented by the Freundlich isotherm model.Optimum activated carbon indicated that DPF can serve as a costeffective precursor adsorbent for Al^(3+)removal.
基金BASF SE(Germany)for their fundingfunding from the German Federal Ministry of Education and Research(BMBF)within the projects ExZellTUMⅡ(grant number 03XP0081)and ExZellTUMⅢ(grant number 03XP0255)and of BMW AG。
文摘Interfacial reactions in lithium-ion batteries often involve gaseous reaction products.Mechanistic investigation of material degradation processes requires a technique to identify and quantify these gases in battery cells.Online electrochemical mass spectrometry(OEMS)is an operando gas analysis method that continuously samples the headspace of a custom battery cell.Real-time gas analysis by quantitative OEMS was used to create mechanistic understanding of battery degradation reactions,some of which will be highlight in this article.
基金supported by the Natural Science Foundation of Jiangsu Province (BK20151380)NSF of China (21103087 and 21872067)supported by the Fundamental Research Funds for the Central Universities (020514380116)。
文摘To study the effect of adjacent hydroxyl to the active sites, several acid catalysts, i.e. substituted benzoic acids with adjacent carboxyl are employed in the fructose dehydration to 5-hydroxymethylfurfural(HMF).Experimental results reveal that Br?nsted acid sites with adjacent carboxyl present higher catalytic ability than isolated ones. Computational results suggest that the adjacent sites lead to co-interaction on fructose, corresponding more stable transition state and faster HMF formation rate. Based on the enhancement from the adjacent sites, a novel ordered mesoporous carbon(OMC) full of carboxyls in surface is prepared and turns out to be an effective solid catalyst for HMF production from fructose derived from biomass.
文摘In this work, the magnesium aluminum spinel (MgAl2O4) was prepared by Mg and Al as precursors through a method of sol-gel subsequent with high temperature calcination. The wide range of synthetic conditions, including organic alcohols, ammonia content, dispersant, alkoxide concentration, hydrolysis time, hydrolysis temperature and calcination temperature were screened over as-prepared samples. This work provides a necessary experimental basis for the synthesis of MgAl2O4 with uniform particle size of spherical structure, which has a potential to be used in many industrial and military applications.
基金supported by JSPS KAKENHI Grant Numbers JP26810098 and JP16K17943~~
文摘Gold clusters and small nanoparticles supported on metal oxides could be prepared by deposition‐precipitation followed by microwave irradiation as a drying method and then calcination.The drying method influenced the size of the Au particles.Au(III)was partly reduced during conventional oven drying,resulting in Au aggregates.In contrast,Au(III)was preserved during microwave drying owing to rapid and uniform heating,and the Au diameter was minimized to1.4nm on Al2O3.This method can be applied to several metal oxide supports having different microwave absorption efficiencies,such as MnO2,Al2O3,and TiO2.These catalysts exhibited higher catalytic activities for CO oxidation at low temperature and for selective aerobic oxidation of sulfide than those prepared by conventional methods.
文摘In this study, the effects of pre-carburization of catalyst, hydrogen addition to methane feed and the space velocity of methane on the catalytic performance in methane to benzene （MTB） reaction were discussed in detail over Mo/HZSM-5 catalyst at 1023 K and 0.3 MPa. Compared with the non-precarburized catalyst, the Mo catalyst pre-carburized under the flow of CHa＋4H2 at 973 K was found to have the higher activity and better stability. Further 6% H2 addition to the methane feed suppressed the aromatic type of coke formation effectively, and improved the stability of catalyst markedly, moreover gave a much longer reaction life of catalyst （53 h at 1023 K and 5400 ml/（g-h）） and much more formation amounts of benzene and hydrogen. With increase of methane space velocity, both the naphthalene formation selectivity and the coke formation selectivity were decreased by the shortened contact time; the benzene formation selectivity and total formation amount before the complete deactivation of catalyst were increased markedly, while the total naphthalene and coke formation amounts did not change much. At high methane space velocity （≥5400 ml/（g·h））, a new middle temperature coke derived from the high temperature aromatic coke was formed on the catalyst; all the coke formed could be burnt off at lower temperature in oxygen, compared with those obtained at low space velocity. Considering the benzene formation amount and catalyst stability together, 5400 ml/（g·h） was proved to be the most efficient methane space velocity for benzene production.
