This work describes the discharge characteristics and acetone degradation with plasma under different electric fields based on a coaxial cylindrical dielectric barrier discharge(DBD)device energized by pulsed power.It...This work describes the discharge characteristics and acetone degradation with plasma under different electric fields based on a coaxial cylindrical dielectric barrier discharge(DBD)device energized by pulsed power.It is found that the segmented electrodes with appropriate spacing in coaxial cylindrical DBD are beneficial to the plasma ionization.In this work,the plasma distribution,discharge thermal effect,ionization of reactive species,and acetone degradation performance in coaxial cylindrical DBD with different segmented electrodes are systematically investigated.The experimental results show that segmented electrodes with a certain distance can cause additional ionization in the non-electrode-covered region between adjacent electrodes,thus enlarging the plasma region compared with a single electrode with equivalent total electrode length.The additional ionization involved the inner volume discharge between the quartz tubes and the outer surface discharge along the surface of the external quartz tube.The spatial distributions of the inner volume discharge and external surface discharge were predominantly governed by the radial and axial components of the inter-electrode electric field,respectively.The external surface discharge exhibited significant suppression when the electrode spacing was<1.5 mm,and it reached its maximum length at 3 mm spacing.When the electrode distance increased to 7-9 mm,a weak ionizing region appeared in the middle of the adjacent electrodes,which could be attributed to the gradual attenuation of the radial component with the increasing electrode spacing.A higher thermal effect and better oxidation of acetone to CO_(x)(CO and CO_(2))were achieved with the segmented electrode;the dual-segment configuration(3 mm per electrode)achieved a reactor temperature of 63.4℃,representing a 10℃enhancement over comparable single-electrode systems.Similarly,the CO_(2)and CO concentration reached 328.8 mg/m3and 105.7 mg/m3,respectively,in two 3 mm long segmented electrodes,which was an increase of 12.2%and 25.6%,respectively,compared with the single electrode.Notably,considering the equivalent ionization of the inner discharge with different electrodes,the enhanced thermal effects and CO_(x)conversion efficiency directly correlate with the expanded plasma zone induced by electrode segmentation.This work provides critical insights into optimizing electrode configurations for efficient plasma-assisted volatile organic compound degradation systems.展开更多
Acetone is a common volatile organic compound that can cause harm to human health when inhaled in small amounts.Therefore,the development of fast response and low detection limit acetone sensors becomes crucial.In thi...Acetone is a common volatile organic compound that can cause harm to human health when inhaled in small amounts.Therefore,the development of fast response and low detection limit acetone sensors becomes crucial.In this study,a core-shell spherical TiO_(2) sensor with a rich pore structure was designed.This sensor exhibited excellent sensing properties,including higher responsiveness(100 ppm acetone,R_(a)/R_(g)=80),lower detection limit(10 ppb)and short response time(8 s).The problem is that the sensing mechanism between TiO_(2) and acetone is not thoroughly analyzed.To gain further insight,the interaction process of TiO_(2) core-shell spheres and acetone under varying oxygen content environments was investigated by dynamic testing,X-ray photoelectron spectroscopy,in-situ Fourier transform infrared spectroscopy and gas chromatography-mass spectrometry.The research results show that acetone not only adsorbs on the surface of the material and reacts with adsorbed oxygen,but also undergoes catalytic oxidation reaction with TiO_(2) core-shell spheres.Significantly,in high oxygen content environments,acetone undergoes oxidation to form intermediates such as acids and anhydrides that are difficult to desorpt on the surface of the material,thus prolonging the recovery time of the sensor.The discovery of this sensing process will provide some guidance for the design of acetone sensing materials in the future.Meanwhile,this also imparts valuable references and insights for the investigation of the mechanism and application of other sensitive metal oxide materials.展开更多
In practical applications,noble metal doping is often used to prepare high performance gas sensors,but more noble metal doping will lead to higher preparation costs.In this study,CeO_(2)/ZnO-Pd with low palladium cont...In practical applications,noble metal doping is often used to prepare high performance gas sensors,but more noble metal doping will lead to higher preparation costs.In this study,CeO_(2)/ZnO-Pd with low palladium content was prepared by ultrasonic method with fast response and high selectivity for acetone sensing.With the same amount of palladium added,the selectivity coefficient of CeO_(2)/ZnO-Pd is 1.88 times higher than that of the stirred sensor.Compared with the pure PdO-doped CeO_(2)/ZnO-PdO material,the content of Pd in CeO_(2)/ZnO-PdO is about 30%of that in CeO_(2)/ZnO-PdO,but the selectivity coefficient for acetone is 2.56 times higher.The CeO_(2)/ZnO-Pd sensor has a higher response(22.54)to 50×10^(−6) acetone at 300℃and the selectivity coefficient is 2.57 times that of the CeO_(2)/ZnO sensor.The sensor has a sub-second response time(0.6 s)and still has a 2.36 response to 330×10^(−9) of acetone.Ultrasonic doping makes Pd particles smaller and increases the contact area with gas.Meanwhile,the composition of n-p-n heterojunction and the synergistic effect of Pd/PdO improve the sensor performance.It shows that ultrasonic Pd doping provides a way to improve the utilization rate of doped metals and prepare highly selective gas sensors.展开更多
Zeolitic imidazolate frameworks(ZIFs)are a series of materials composited by metal ions and organic ligands with high specific surface area,which might be great precursors to produce metal oxides by calcination for ga...Zeolitic imidazolate frameworks(ZIFs)are a series of materials composited by metal ions and organic ligands with high specific surface area,which might be great precursors to produce metal oxides by calcination for gas sensor application.However,Zn-ZIF(ZIF-8)is hard to transform as ZnO in air and keeping the unique framework simultaneously.In this work,Fe^(2+)was introduced into the metal node to replace a part of Zn^(2+)ions,and it could be oxidized as Fe^(3+)in the calcination to facilitate the oxidation process of the 2-methylimdazole ligands to give Fe-ZnO complex shell with high specific surface area(108 m~2/g)and abundant oxygen vacancies(48%).The micro electro mechanical systems(MEMS)sensor based on the6%-Fe-ZnO complex shell performed outstanding gas sensing properties to the low-concentration acetone vapor,including high response(ΔR/R_g=11.2 to 5 ppm acetone),superior selectivity(S_(acetone)/S_(ethanol)=5.6)and fast response speed(τ_(res)=2.6 s).This work not only provided the research of an exceptional acetone MEMS sensor,but also induced a strategy to produce metal oxide derived from ZIFs with complex structures for the universal synthesis methodology.展开更多
As a key biomarker for noninvasive diagnosis of diabetes,the selective detection of trace acetone in exhaled gas using a portable and low-cost device remains a great challenge.Semiconductor metal oxide(SMO)based gas s...As a key biomarker for noninvasive diagnosis of diabetes,the selective detection of trace acetone in exhaled gas using a portable and low-cost device remains a great challenge.Semiconductor metal oxide(SMO)based gas sensors have drawn signification attention due to their potential in miniaturization,user-friendliness,high cost-effectiveness and selective real-time detection for noninvasive clinical diagnosis.Herein,we propose a one-pot solvent evaporation induced tricomponent co-assembly strategy to design a novel ordered mesoporous SMO of silica-implanted WO_(3)(Si O_(2)/WO_(3))as sensing materials for trace acetone detection.The controlled co-assembly of silicon and tungsten precursors and amphiphilic diblock copolymer poly(ethylene oxide)-block-polystyrene(PEO-b-PS),and the subsequent thermal treatment enable the local lattice disorder of WO_(3)induced by the amorphous silica and the formation of ordered mesoporous Si O_(2)/WO_(3)hybrid walls with a unique metastableε-phase WO_(3)framework.The obtained mesoporous SiO_(2)/WO_(3)composites possess highly crystalline framework with large uniform pore size(12.0-13.3 nm),high surface area(99-113 m^(2)/g)and pore volume(0.17-0.23 cm^(3)/g).Typically,the asfabricated gas sensor based on mesoporous 2.5%Si O_(2)/WO_(3)exhibits rapid response/recovery rate(5/17 s),superior sensitivity(R_(air)/R_(gas)=105 for 50 ppm acetone),as well as high selectivity towards acetone.The limit of detection is as low as 0.25 ppm,which is considerably lower than the thresh value of acetone concentration(>1.1 ppm)in the exhaled breath of diabetic patients,demonstrating its great prospect in real-time monitoring in diabetes diagnosis.Moreover,the mesoporous 2.5%Si O_(2)/WO_(3)sensor is integrated into a wireless sensing module connected to a smart phone,providing a convenient real-time detection of acetone.展开更多
The conversion of acetone derived from biomass to isobutene has attracted extensive attentions.In comparison with Brønsted acidic catalyst,Lewis acidic catalyst could exhibit a better catalytic performance with a...The conversion of acetone derived from biomass to isobutene has attracted extensive attentions.In comparison with Brønsted acidic catalyst,Lewis acidic catalyst could exhibit a better catalytic performance with a higher isobutene selectivity.However,the catalyst stability remains a key problem for the long-running acetone conversion and the reasons for catalyst deactivation are poorly understood up to now.Herein,the deactivation mechanism of Lewis acidic Y/Beta catalyst during the acetone to isobutene conversion was investigated by various characterization techniques,including acetone-temperature-programmed surface reaction,gas chromatography-mass spectrometry,in situ ultraviolet-visible,and ^(13)C cross polarization magic angle spinning nuclear magnetic resonance spectroscopy.A successive aldol condensation and cyclization were observed as the main side-reactions during the acetone conversion at Lewis acidic Y sites.In comparison with the low reaction temperature,a rapid formation and accumulation of the larger cyclic unsaturated aldehydes/ketones and aromatics could be observed,and which could strongly adsorb on the Lewis acidic sites,and thus cause the catalyst deactivation eventually.After a simple calcination,the coke deposits could be easily removed and the catalytic activity could be well restored.展开更多
The exploitation of the highly reliable gassensing device for exhaled acetone detection possesses momentous and capacious development prospects in the field of an early noninvasive diabetes diagnosis.Considering that ...The exploitation of the highly reliable gassensing device for exhaled acetone detection possesses momentous and capacious development prospects in the field of an early noninvasive diabetes diagnosis.Considering that the characteristics of crystal facets will impact the gas-sensitive performance,herein three different resistive gas sensors were successfully developed by utilizing the stable α-Fe_(2)O_(3)with different crystal facets as the sensitive materials.The gas-sensitive performance testing results reveal that the(110)crystal faceted α-Fe_(2)O_(3)sensor exhibits relatively superior comprehensive gas sensitivity toward acetone.Particularly,it is worth mentioning that the sensor demonstrates reliable sensitivity,rapid response(25 s)/recovery(3 s)speed,and strong anti-interference capability in detecting 2×10^(-6)acetone for the concentration threshold of diabetes,even when exposed to prolonged periods in variable environments.Furthermore,by simply validating the feasibility of the exhalation diagnosis using the as-prepared gas sensor,the(110)faceted α-Fe_(2)O_(3)gas sensor can effectively discriminate the states of healthy human exhalation and the simulated diabetic exhalation.Through integrating the experimental and theoretical analyses,the superior acetone-sensitive performance of the(110)facetedα-Fe_(2)O_(3)gas sensor can principally be interpreted in correlation with crystal facet-dependent gas adsorption capacity and defect-forming ability.These results not only imply a tremendous application perspective in monitoring acetone gas at sub-ppm concentration,but also open up an effective throughway to develop reliable gas-sensing devices for early non-invasive diabetes screening.展开更多
Nickel ferrite nano-powders were prepared by microwave radiating low-temperature solid-state reaction method, and then modified with Ag by dipping method. The crystal structure and morphology of the samples were chara...Nickel ferrite nano-powders were prepared by microwave radiating low-temperature solid-state reaction method, and then modified with Ag by dipping method. The crystal structure and morphology of the samples were characterized by means of X-ray diffraction(XRD), scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). The gas sensing properties of the samples were also investigated. The results reveal that the Ag, as amorphous structure, can efficiently prevent the reuniting and growing-up of nanosized NiFe2O4 grains, and 1.5% Ag modified NiFe2O4 sensor has a better sensitivity, up to 43, for acetone gas than 1.5%Ag mixed NiFe2O4 sensor prepared by low-temperature solid-state reaction, at an optimal working voltage of 4.5 V. The quick response time (1 s) and fast recovery time (~10 s) are the main characteristics of this sensor.展开更多
A synthetic method of dialkylideneacetones has been developed. Compared with known protocols, the method employed catalytic Ca(OH)_2 as the cheap, mild base catalyst and dilute aqueous EtOH(20%, v/v)as the green and s...A synthetic method of dialkylideneacetones has been developed. Compared with known protocols, the method employed catalytic Ca(OH)_2 as the cheap, mild base catalyst and dilute aqueous EtOH(20%, v/v)as the green and safe solvent. The procedure was easily operated: In most cases, the product could be isolated by a simple filtration, and purified by washing with water. This paper provided experimental details of the reactions, which could be applied in gram-scale synthesis and should be a very reliable and practical protocol to prepare these useful compounds in laboratory and at the industrial level.展开更多
The morphologic changes and growth status of PC12 cells were observed after intervened by different concentrations of methanol, ethanol, acetone, glycerol and the toxic concentrations were ascertained. Four kinds of o...The morphologic changes and growth status of PC12 cells were observed after intervened by different concentrations of methanol, ethanol, acetone, glycerol and the toxic concentrations were ascertained. Four kinds of organic solvents al showed certain cytotoxicity to PC12 cells. Compared with other three kinds of or-ganic solvents, ethanol showed the most obvious cytotoxicity to PC12 cells and the cellviability would be reduced to 60% if the concentration of ethanol was 20 ml/L and the intervention lasted for 24 h. Under the same condition, the reduced per-centages of cellviability for acetone and ethanol were 20% and 15% respectively. Glycerol also showed cytotoxicity to PC12 cells, especial y as the concentration was raised gradual y, but the toxicity was relatively mild. This study would provide refer-ence material for subsequent pharmacological studies.展开更多
Mesoporous semiconducting metal oxides(SMOs)heterojunctions are appealing sensors for gas detecting.However,due to the different hydrolysis and condensation mechanism of every metal precursor and the contradiction bet...Mesoporous semiconducting metal oxides(SMOs)heterojunctions are appealing sensors for gas detecting.However,due to the different hydrolysis and condensation mechanism of every metal precursor and the contradiction between high crystallinity and high surface area,the synthesis of mesoporous SMOs heterojunctions with highly o rdered mesostructures,highly crystallized frameworks,and high surface area remains a huge challenge.In this work,we develop a novel"acid-base pair"adjusted solvent evaporation induced self-assembly(EISA)strategy to prepare highly crystallized ordered mesoporous TiO2/WO3(OM-TiO2/WO3)heterojunctions.The WCl6 and titanium isopropoxide(TIPO)are used as the precursors,respectively,which function as the"acid-base pair",enabling the coassembly with the structure directing agent(PEO-b-PS)into highly ordered meso structures.In addition,PEO-b-PS can be converted to rigid carbon which can protect the meso structures from collapse during the crystallization process.The resultant OM-TiO2/WO3 heterojunctions possess primitive cubic mesostructures,large pore size(~21.1 nm),highly crystalline frameworks and surface area(~98 m2/g).As a sensor for acetone,the obtained OM-TiO2/WO3 show excellent re sponse/recovery perfo rmance(3 s/5 s),good linear dependence,repeatability,selectivity,and long-term stability(35 days).展开更多
Acetone,as widely used reagents in industry and laboratories,are extremely harmful to the human.So the detection of acetone gas concentrations and leaks in special environments at room temperature is essential.Herein,...Acetone,as widely used reagents in industry and laboratories,are extremely harmful to the human.So the detection of acetone gas concentrations and leaks in special environments at room temperature is essential.Herein,the nanocomposite combining SnO-SnO_(2)(p-n junction)and Ti_(3)C_(2)T_(x) MXene was successfully synthesized by a one-step hydrothermal method.Because of the existence of a small amount of oxygen during the hydrothermal conditions,part of the p-type SnO was oxidized to n-type SnO_(2),forming in-situ p-n junctions on the surface of Sn O.The hamburger-like SnO-SnO_(2)/Ti_(3)C_(2)T_(x) sensor exhibited improved acetone gas sensing response of 12.1(R_(g)/R_(a))at room temperature,which were nearly 11 and 4 times higher than those of pristine Ti_(3)C_(2)T_(x) and pristine SnO-SnO_(2),respectively.Moreover,it expressed a short recovery time(9 s)and outstanding reproducibility.Because of the different work functions,the Schottky barrier was formed between the SnO and the Ti_(3)C_(2)T_(x) nanosheets,acting as a hole accumulation layer(HALs)between Ti_(3)C_(2)T_(x) and tin oxides.Herein,the sensing mechanism based on the formation of hetero-junctions and high conductivity of the metallic phase of Ti_(3)C_(2)T_(x) MXene in SnO-SnO_(2)/Ti_(3)C_(2)T_(x) sensors was discussed in detail.展开更多
Currently,SmFeO_(3)-based sensors are an effective platform for detecting acetone gas.However,they require high operating temperatures,which increases energy consumption and safety hazards,and their response is low wh...Currently,SmFeO_(3)-based sensors are an effective platform for detecting acetone gas.However,they require high operating temperatures,which increases energy consumption and safety hazards,and their response is low when the gas concentration is at 10^(-9)(PPB),which cannot meet the requirements of using exhaled breath to pre-diagnose diabetes.Herein,Pd-SmFeO_(3)hollow nanotubes with an extremely high specific surface area and porosity were synthesized by electrospinning.After Pd doping,the specific surface area improved by more than two times,and the acetone response improved by more than three times.In addition,the response further improved by more than 1.5 times,and the optimum operating temperature reduced by 100℃under light irradiation.Moreover,the relative humidity adaptability,long-term stability,and selectivity of the material were significantly improved after Pd doping or light irradiation.Finally,the acetone concentration in a person’s exhaled breath was detected by a Pd-SmFeO_(3)-based gas sensor,and the error was less than 10%compared to that obtained by gas chromatography-mass spectrometry method.展开更多
Ternary Au/Fe2O3-ZnO gas-sensing materials were synthesized by combining co-precipitation and microwave irradiation process.The as-prepared Au/Fe2O3-ZnO was characterized with X-ray diffractometer and scanning electro...Ternary Au/Fe2O3-ZnO gas-sensing materials were synthesized by combining co-precipitation and microwave irradiation process.The as-prepared Au/Fe2O3-ZnO was characterized with X-ray diffractometer and scanning electron microscope,and its gas-sensing performance was measured using a gas-sensor analysis system.The results show that the as-prepared products consist of hexagonal wurtzite ZnO,face-centered cubic gold nanoparticles and orthorhombic Fe2O3crystallines.The Au/Fe2O3-ZnO based sensor has a very high selectivity to ethanol and acetone,and also has high sensitivity(154)at a low working temperature(270°C)and an extremely fast response(1s)against acetone.It is found that the selectivity can be adjusted by Fe2O3content added in the ternary materials.It possesses a worth looking forward prospect to practical applications in acetone detecting and administrating field.展开更多
In recent years, clinical studies have found that acetone concentration in exhaled breath can be taken as a characteristic marker of diabetes. Metal-oxide-semiconductor (MOS) materials are widely used in acetone gas s...In recent years, clinical studies have found that acetone concentration in exhaled breath can be taken as a characteristic marker of diabetes. Metal-oxide-semiconductor (MOS) materials are widely used in acetone gas sensors due to their low cost, high sensitivity, fast response/recovery time, and easy integration. This paper reviews recent progress in acetone sensors based on MOS materials for diabetes diagnosis. The methods of improving the performance of acetone sensor have been explored for comparison, especially in high humidity conditions. We summarize the current excellent methods of preparations of sensors based on MOSs and hope to provide some help for the progress of acetone sensors in the diagnosis of diabetes.展开更多
The PdC12 was mixed with nanocrystalline powders LaFeO3 and subsequently followed by an annealing of 800 ℃. PdO phase was formed and almost distributed uniformly on the surface of LaFeO3 nano-particles. With an incre...The PdC12 was mixed with nanocrystalline powders LaFeO3 and subsequently followed by an annealing of 800 ℃. PdO phase was formed and almost distributed uniformly on the surface of LaFeO3 nano-particles. With an increase of PdO amounts in composite powders, sensing sensitivity Rg/Ra to low concentration acetone or ethanol for Pd doped LaFeO3 sensors increased at first, underwent the maximum with 2 wt.% PdC12 dopant, and then doped again. Interestingly, appropriate Pd doping in LaFeO3 changed the selectivity behavior of gas sensing. LaFeO3 sensor showed good selectivity to ethanol, but 2 wt.% Pd doped LaFeO3 sensor showed good selectivity to acetone. The sensitivity for LaFeO3 at 200 ℃was 1.32 to 1 ppm ethanol, and 1.19 to 1 ppm acetone. Whereas the sensitivity for 2 wt.% Pd doped LaFeO3 at 200 ℃ was 1.53 to 1 ppm ethanol, and 1.9 to 1 ppm acetone. The 2 wt.% Pd doped LaFeO3 sensor at 200 ℃ showed very short response time (4 s) and recovery time (2 s) to 1 ppm acetone gas, respectively. Such results showed that 2 wt.% Pd doped LaFeO3 sensor is a new promising sensing candidate for detecting low concentration acetone.展开更多
Three-dimensionally ordered mesoporous Fe2O3(meso-Fe2O3) and its supported Au, Pd,and Au-Pd alloy(xA uP dy/meso-Fe2O3; x = 0.08–0.72 wt.%; Pd/Au molar ratio(y) = 1.48–1.85)photocatalysts have been prepared via...Three-dimensionally ordered mesoporous Fe2O3(meso-Fe2O3) and its supported Au, Pd,and Au-Pd alloy(xA uP dy/meso-Fe2O3; x = 0.08–0.72 wt.%; Pd/Au molar ratio(y) = 1.48–1.85)photocatalysts have been prepared via the KIT-6-templating and polyvinyl alcohol-protected reduction routes, respectively. Physical properties of the samples were characterized, and their photocatalytic activities were evaluated for the photocatalytic oxidation of acetone in the presence of a small amount of H2O2 under visible-light illumination. It was found that the meso-Fe2O3 was rhombohedral in crystal structure. The as-obtained samples displayed a high surface area of 111.0–140.8 m^2/g and a bandgap energy of 1.98–2.12 eV. The Au, Pd and/or Au–Pd alloy nanoparticles(NPs) with a size of 3–4 nm were uniformly dispersed on the surface of the meso-Fe2O3 support. The 0.72 wt.% AuP d1.48/meso-Fe2O3 sample performed the best in the presence of 0.06 mol/L H2O2 aqueous solution, showing a 100% acetone conversion within4 hr of visible-light illumination. It was concluded that the good performance of 0.72 wt.%AuPd(1.48)/meso-Fe2O3 for photocatalytic acetone oxidation was associated with its ordered mesoporous structure, high adsorbed oxygen species concentration, plasmonic resonance effect between AuPd(1.48) NPs and meso-Fe2O3, and effective separation of the photogenerated charge carriers. In addition, the introduction of H2O2 and the involvement of the photo-Fenton process also played important roles in enhancing the photocatalytic activity of 0.72 wt.%AuPd(1.48)/meso-Fe2O3.展开更多
In the present work, we synthesized Sm2O3 doped SnO2 in order to prepare a selective acetone sensor with fast response, quick recovery and good repeatability. Pure as well as 2 mol.%, 4 mol.%, 6 mol.% and 8 mol.% Sm2O...In the present work, we synthesized Sm2O3 doped SnO2 in order to prepare a selective acetone sensor with fast response, quick recovery and good repeatability. Pure as well as 2 mol.%, 4 mol.%, 6 mol.% and 8 mol.% Sm2O3 doped SnO2 nanostructured samples were synthesized by using a co-precipitation method. The characterization of the samples was done by thermogravimetric and differential thermo-gravimetric analysis(TG-DTA), X-ray diffraction(XRD), field emission gun-scanning electron microscopy(FEG-SEM), energy dispersive analysis by X-rays(EDAX), high resolution scanning electron microscopy(HR-TEM), selected area X-ray diffraction(SAED), Brunauer-Emmet-Teller(BET) and ultraviolet-visible-near infrared(UV-Vis-NIR) spectroscopy techniques. The gas response studies of liquid petroleum gas, ammonia, ethanol and acetone vapor were carried out. The results showed that Sm doping systematically lowered operating temperature and enhanced the gas response and selectivity for acetone. The response and recovery time for 6 mol.% Sm2O3 doped SnO2 thick film at the operating temperature of 250 °C were 15 and 24 s, respectively.展开更多
TiO2hollow microspheres(TiO2‐HMSs)have attracted much attention because of their high photoreactivity,low density,and good permeability.However,anatase TiO2‐HMSs have poor thermal stability.In this study,surface‐fl...TiO2hollow microspheres(TiO2‐HMSs)have attracted much attention because of their high photoreactivity,low density,and good permeability.However,anatase TiO2‐HMSs have poor thermal stability.In this study,surface‐fluorinated TiO2‐HMSs were assembled from hollow nanoparticles by the hydrothermal reaction of the mixed Ti(SO4)2–NH4HF–H2O2solution at180°C.The effect of the calcination temperature on the structure and photoreactivity of the TiO2‐HMSs was systematically investigated,which was evaluated by photocatalytic oxidation of acetone in air under ultraviolet irradiation.We found that after calcination at300°C,the photoreactivity of the TiO2‐HMSs decreases from1.39×10?3min?1(TiO2‐HMS precursor)to0.82×10?3min?1because of removal of surface‐adsorbed fluoride ions.With increasing calcination temperature from300to900°C,the building blocks of the TiO2‐HMSs evolve from truncated bipyramidal shaped hollow nanoparticles to round solid nanoparticles,and the photoreactivity of the TiO2‐HMSs steady increases from0.82×10?3to2.09×10?3min?1because of enhanced crystallization.Further increasing the calcination temperature to1000and1100°C results in a decrease of the photoreactivity,which is ascribed to a sharp decrease of the Brunauer–Emmett–Teller surface area and the beginning of the anatase–rutile phase transformation at1100°C.The effect of surface‐adsorbed fluoride ions on the thermal stability of the TiO2‐HMSs is also discussed.展开更多
The heterostructured NiWO_(4)/WO_(3) nanotubes(Ni/W NTs)were synthesized by using a facile self-assembly method on the sacrificial polystyrene(PS)nanofibers templates.Then,the Pt-decorated NiWO_(4)/WO_(3)(Pt@Ni/W)comp...The heterostructured NiWO_(4)/WO_(3) nanotubes(Ni/W NTs)were synthesized by using a facile self-assembly method on the sacrificial polystyrene(PS)nanofibers templates.Then,the Pt-decorated NiWO_(4)/WO_(3)(Pt@Ni/W)composite NTs were obtained through using an ultrasonic mixing method.The experimental results display that the order of gas-sensing performance is Pt@Ni/W>Ni/W>WO_(3).The 2wt.%Pt@Ni/W-5 NTs indicate the supreme acetone-sensing response(R_(air)/R_(gas)=58.4 at 100×10^(−6))at 375℃,which is 10.6 and 1.53 times that of the WO_(3) and NiWO_(4)/WO_(3) NTs,respectively.Additionally,the 2wt.%Pt@Ni/W-5 NTs also exhibit the dramatically high selectivity toward acetone against ethanol,methanal,methanol,NH_(3) and toluene.The Pt-decorated Ni/W NTs show the excellent responsivity and stability toward acetone,which is ascribed to the construction of heterostructured NiWO_(4)/WO_(3) and the spill-over effect of Pt nanoparticles.展开更多
文摘This work describes the discharge characteristics and acetone degradation with plasma under different electric fields based on a coaxial cylindrical dielectric barrier discharge(DBD)device energized by pulsed power.It is found that the segmented electrodes with appropriate spacing in coaxial cylindrical DBD are beneficial to the plasma ionization.In this work,the plasma distribution,discharge thermal effect,ionization of reactive species,and acetone degradation performance in coaxial cylindrical DBD with different segmented electrodes are systematically investigated.The experimental results show that segmented electrodes with a certain distance can cause additional ionization in the non-electrode-covered region between adjacent electrodes,thus enlarging the plasma region compared with a single electrode with equivalent total electrode length.The additional ionization involved the inner volume discharge between the quartz tubes and the outer surface discharge along the surface of the external quartz tube.The spatial distributions of the inner volume discharge and external surface discharge were predominantly governed by the radial and axial components of the inter-electrode electric field,respectively.The external surface discharge exhibited significant suppression when the electrode spacing was<1.5 mm,and it reached its maximum length at 3 mm spacing.When the electrode distance increased to 7-9 mm,a weak ionizing region appeared in the middle of the adjacent electrodes,which could be attributed to the gradual attenuation of the radial component with the increasing electrode spacing.A higher thermal effect and better oxidation of acetone to CO_(x)(CO and CO_(2))were achieved with the segmented electrode;the dual-segment configuration(3 mm per electrode)achieved a reactor temperature of 63.4℃,representing a 10℃enhancement over comparable single-electrode systems.Similarly,the CO_(2)and CO concentration reached 328.8 mg/m3and 105.7 mg/m3,respectively,in two 3 mm long segmented electrodes,which was an increase of 12.2%and 25.6%,respectively,compared with the single electrode.Notably,considering the equivalent ionization of the inner discharge with different electrodes,the enhanced thermal effects and CO_(x)conversion efficiency directly correlate with the expanded plasma zone induced by electrode segmentation.This work provides critical insights into optimizing electrode configurations for efficient plasma-assisted volatile organic compound degradation systems.
基金supported by the National Natural Science Foundation of China(Nos.21771060 and 61271126)the International Science&Technology Cooperation Program of China(No.2016YFE0115100)+2 种基金Heilongjiang Provincial Natural Science Foundation of China(No.LH_(2)023B021)Reform and Development Fund Project of Local University supported by the Central Government,Heilongjiang Touyan Innovation Team Program,New Era Excellent Master’s and Doctoral Dissertations of Heilongjiang Province(No.LJYXL2023-020)Basic Scientific Research Project for Heilongjiang Provincial Colleges and Universities(No.2023-KYYWF-1482).
文摘Acetone is a common volatile organic compound that can cause harm to human health when inhaled in small amounts.Therefore,the development of fast response and low detection limit acetone sensors becomes crucial.In this study,a core-shell spherical TiO_(2) sensor with a rich pore structure was designed.This sensor exhibited excellent sensing properties,including higher responsiveness(100 ppm acetone,R_(a)/R_(g)=80),lower detection limit(10 ppb)and short response time(8 s).The problem is that the sensing mechanism between TiO_(2) and acetone is not thoroughly analyzed.To gain further insight,the interaction process of TiO_(2) core-shell spheres and acetone under varying oxygen content environments was investigated by dynamic testing,X-ray photoelectron spectroscopy,in-situ Fourier transform infrared spectroscopy and gas chromatography-mass spectrometry.The research results show that acetone not only adsorbs on the surface of the material and reacts with adsorbed oxygen,but also undergoes catalytic oxidation reaction with TiO_(2) core-shell spheres.Significantly,in high oxygen content environments,acetone undergoes oxidation to form intermediates such as acids and anhydrides that are difficult to desorpt on the surface of the material,thus prolonging the recovery time of the sensor.The discovery of this sensing process will provide some guidance for the design of acetone sensing materials in the future.Meanwhile,this also imparts valuable references and insights for the investigation of the mechanism and application of other sensitive metal oxide materials.
基金Project(2023JJ10005)supported by the Natural Science Foundation of Hunan Province,ChinaProjects(51772082,51804106)supported by the National Natural Science Foundation of China。
文摘In practical applications,noble metal doping is often used to prepare high performance gas sensors,but more noble metal doping will lead to higher preparation costs.In this study,CeO_(2)/ZnO-Pd with low palladium content was prepared by ultrasonic method with fast response and high selectivity for acetone sensing.With the same amount of palladium added,the selectivity coefficient of CeO_(2)/ZnO-Pd is 1.88 times higher than that of the stirred sensor.Compared with the pure PdO-doped CeO_(2)/ZnO-PdO material,the content of Pd in CeO_(2)/ZnO-PdO is about 30%of that in CeO_(2)/ZnO-PdO,but the selectivity coefficient for acetone is 2.56 times higher.The CeO_(2)/ZnO-Pd sensor has a higher response(22.54)to 50×10^(−6) acetone at 300℃and the selectivity coefficient is 2.57 times that of the CeO_(2)/ZnO sensor.The sensor has a sub-second response time(0.6 s)and still has a 2.36 response to 330×10^(−9) of acetone.Ultrasonic doping makes Pd particles smaller and increases the contact area with gas.Meanwhile,the composition of n-p-n heterojunction and the synergistic effect of Pd/PdO improve the sensor performance.It shows that ultrasonic Pd doping provides a way to improve the utilization rate of doped metals and prepare highly selective gas sensors.
基金supported by the National Natural Science Foundation of China(No.62271299)Shanghai Engineering Research Center for Integrated Circuits and Advanced Display Materials。
文摘Zeolitic imidazolate frameworks(ZIFs)are a series of materials composited by metal ions and organic ligands with high specific surface area,which might be great precursors to produce metal oxides by calcination for gas sensor application.However,Zn-ZIF(ZIF-8)is hard to transform as ZnO in air and keeping the unique framework simultaneously.In this work,Fe^(2+)was introduced into the metal node to replace a part of Zn^(2+)ions,and it could be oxidized as Fe^(3+)in the calcination to facilitate the oxidation process of the 2-methylimdazole ligands to give Fe-ZnO complex shell with high specific surface area(108 m~2/g)and abundant oxygen vacancies(48%).The micro electro mechanical systems(MEMS)sensor based on the6%-Fe-ZnO complex shell performed outstanding gas sensing properties to the low-concentration acetone vapor,including high response(ΔR/R_g=11.2 to 5 ppm acetone),superior selectivity(S_(acetone)/S_(ethanol)=5.6)and fast response speed(τ_(res)=2.6 s).This work not only provided the research of an exceptional acetone MEMS sensor,but also induced a strategy to produce metal oxide derived from ZIFs with complex structures for the universal synthesis methodology.
基金financially supported by National Natural Science Foundation of China(Nos.62104045,22125501,U22A20152)State Key Laboratory of Transducer Technology of China(No.SKT2207)+1 种基金Medical Engineering Jiont Fund of Fudan University(No.yg2023-10)Fundamental Research Funds for the Central Universities(No.20720220010)。
文摘As a key biomarker for noninvasive diagnosis of diabetes,the selective detection of trace acetone in exhaled gas using a portable and low-cost device remains a great challenge.Semiconductor metal oxide(SMO)based gas sensors have drawn signification attention due to their potential in miniaturization,user-friendliness,high cost-effectiveness and selective real-time detection for noninvasive clinical diagnosis.Herein,we propose a one-pot solvent evaporation induced tricomponent co-assembly strategy to design a novel ordered mesoporous SMO of silica-implanted WO_(3)(Si O_(2)/WO_(3))as sensing materials for trace acetone detection.The controlled co-assembly of silicon and tungsten precursors and amphiphilic diblock copolymer poly(ethylene oxide)-block-polystyrene(PEO-b-PS),and the subsequent thermal treatment enable the local lattice disorder of WO_(3)induced by the amorphous silica and the formation of ordered mesoporous Si O_(2)/WO_(3)hybrid walls with a unique metastableε-phase WO_(3)framework.The obtained mesoporous SiO_(2)/WO_(3)composites possess highly crystalline framework with large uniform pore size(12.0-13.3 nm),high surface area(99-113 m^(2)/g)and pore volume(0.17-0.23 cm^(3)/g).Typically,the asfabricated gas sensor based on mesoporous 2.5%Si O_(2)/WO_(3)exhibits rapid response/recovery rate(5/17 s),superior sensitivity(R_(air)/R_(gas)=105 for 50 ppm acetone),as well as high selectivity towards acetone.The limit of detection is as low as 0.25 ppm,which is considerably lower than the thresh value of acetone concentration(>1.1 ppm)in the exhaled breath of diabetic patients,demonstrating its great prospect in real-time monitoring in diabetes diagnosis.Moreover,the mesoporous 2.5%Si O_(2)/WO_(3)sensor is integrated into a wireless sensing module connected to a smart phone,providing a convenient real-time detection of acetone.
文摘The conversion of acetone derived from biomass to isobutene has attracted extensive attentions.In comparison with Brønsted acidic catalyst,Lewis acidic catalyst could exhibit a better catalytic performance with a higher isobutene selectivity.However,the catalyst stability remains a key problem for the long-running acetone conversion and the reasons for catalyst deactivation are poorly understood up to now.Herein,the deactivation mechanism of Lewis acidic Y/Beta catalyst during the acetone to isobutene conversion was investigated by various characterization techniques,including acetone-temperature-programmed surface reaction,gas chromatography-mass spectrometry,in situ ultraviolet-visible,and ^(13)C cross polarization magic angle spinning nuclear magnetic resonance spectroscopy.A successive aldol condensation and cyclization were observed as the main side-reactions during the acetone conversion at Lewis acidic Y sites.In comparison with the low reaction temperature,a rapid formation and accumulation of the larger cyclic unsaturated aldehydes/ketones and aromatics could be observed,and which could strongly adsorb on the Lewis acidic sites,and thus cause the catalyst deactivation eventually.After a simple calcination,the coke deposits could be easily removed and the catalytic activity could be well restored.
基金financially supported by the National Natural Science Foundation of China(Nos.62101477,62071410 and 21802114)the Science and Technology Innovation Program of Hunan Province(No.2023RC3133)the Excellent Youth Scholars of Hunan Provincial Department of Education(No.21B0141)。
文摘The exploitation of the highly reliable gassensing device for exhaled acetone detection possesses momentous and capacious development prospects in the field of an early noninvasive diabetes diagnosis.Considering that the characteristics of crystal facets will impact the gas-sensitive performance,herein three different resistive gas sensors were successfully developed by utilizing the stable α-Fe_(2)O_(3)with different crystal facets as the sensitive materials.The gas-sensitive performance testing results reveal that the(110)crystal faceted α-Fe_(2)O_(3)sensor exhibits relatively superior comprehensive gas sensitivity toward acetone.Particularly,it is worth mentioning that the sensor demonstrates reliable sensitivity,rapid response(25 s)/recovery(3 s)speed,and strong anti-interference capability in detecting 2×10^(-6)acetone for the concentration threshold of diabetes,even when exposed to prolonged periods in variable environments.Furthermore,by simply validating the feasibility of the exhalation diagnosis using the as-prepared gas sensor,the(110)faceted α-Fe_(2)O_(3)gas sensor can effectively discriminate the states of healthy human exhalation and the simulated diabetic exhalation.Through integrating the experimental and theoretical analyses,the superior acetone-sensitive performance of the(110)facetedα-Fe_(2)O_(3)gas sensor can principally be interpreted in correlation with crystal facet-dependent gas adsorption capacity and defect-forming ability.These results not only imply a tremendous application perspective in monitoring acetone gas at sub-ppm concentration,but also open up an effective throughway to develop reliable gas-sensing devices for early non-invasive diabetes screening.
基金Project (2006BS04035) supported by the Youth Scientific Research Foundation of Shandong Province, China
文摘Nickel ferrite nano-powders were prepared by microwave radiating low-temperature solid-state reaction method, and then modified with Ag by dipping method. The crystal structure and morphology of the samples were characterized by means of X-ray diffraction(XRD), scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). The gas sensing properties of the samples were also investigated. The results reveal that the Ag, as amorphous structure, can efficiently prevent the reuniting and growing-up of nanosized NiFe2O4 grains, and 1.5% Ag modified NiFe2O4 sensor has a better sensitivity, up to 43, for acetone gas than 1.5%Ag mixed NiFe2O4 sensor prepared by low-temperature solid-state reaction, at an optimal working voltage of 4.5 V. The quick response time (1 s) and fast recovery time (~10 s) are the main characteristics of this sensor.
基金the National Natural Science Foundation of China (Nos. 21202141, 21672163)Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)+3 种基金Top-notch Academic Programs Project of Jiangsu Higher Education Institutions (TAPP)the high level talent support project of Yangzhou University (top-notch talent, L. Yu)Yangzhou Natural Science Foundation (No. YZ2014040)the Natural Science Foundation of Guangling College (No. ZKZD17005) for financial support
文摘A synthetic method of dialkylideneacetones has been developed. Compared with known protocols, the method employed catalytic Ca(OH)_2 as the cheap, mild base catalyst and dilute aqueous EtOH(20%, v/v)as the green and safe solvent. The procedure was easily operated: In most cases, the product could be isolated by a simple filtration, and purified by washing with water. This paper provided experimental details of the reactions, which could be applied in gram-scale synthesis and should be a very reliable and practical protocol to prepare these useful compounds in laboratory and at the industrial level.
文摘The morphologic changes and growth status of PC12 cells were observed after intervened by different concentrations of methanol, ethanol, acetone, glycerol and the toxic concentrations were ascertained. Four kinds of organic solvents al showed certain cytotoxicity to PC12 cells. Compared with other three kinds of or-ganic solvents, ethanol showed the most obvious cytotoxicity to PC12 cells and the cellviability would be reduced to 60% if the concentration of ethanol was 20 ml/L and the intervention lasted for 24 h. Under the same condition, the reduced per-centages of cellviability for acetone and ethanol were 20% and 15% respectively. Glycerol also showed cytotoxicity to PC12 cells, especial y as the concentration was raised gradual y, but the toxicity was relatively mild. This study would provide refer-ence material for subsequent pharmacological studies.
基金supported by the National Natural Science Foundation of China(Nos.51822202 and 51772050)China Postdoctoral Science Foundation(No.2019M651342)+2 种基金Shanghai Rising-Star Program(No.18QA1400100)Youth Top-notch Talent Support Program of Shanghai,the Shanghai Committee of Science and Technology,China(No.19520713200)DHU Distinguished Young Professor Program and Fundamental Research Funds for the Central Universities。
文摘Mesoporous semiconducting metal oxides(SMOs)heterojunctions are appealing sensors for gas detecting.However,due to the different hydrolysis and condensation mechanism of every metal precursor and the contradiction between high crystallinity and high surface area,the synthesis of mesoporous SMOs heterojunctions with highly o rdered mesostructures,highly crystallized frameworks,and high surface area remains a huge challenge.In this work,we develop a novel"acid-base pair"adjusted solvent evaporation induced self-assembly(EISA)strategy to prepare highly crystallized ordered mesoporous TiO2/WO3(OM-TiO2/WO3)heterojunctions.The WCl6 and titanium isopropoxide(TIPO)are used as the precursors,respectively,which function as the"acid-base pair",enabling the coassembly with the structure directing agent(PEO-b-PS)into highly ordered meso structures.In addition,PEO-b-PS can be converted to rigid carbon which can protect the meso structures from collapse during the crystallization process.The resultant OM-TiO2/WO3 heterojunctions possess primitive cubic mesostructures,large pore size(~21.1 nm),highly crystalline frameworks and surface area(~98 m2/g).As a sensor for acetone,the obtained OM-TiO2/WO3 show excellent re sponse/recovery perfo rmance(3 s/5 s),good linear dependence,repeatability,selectivity,and long-term stability(35 days).
基金supported financially by the National Natural Science Foundation of China(Nos.,51572158 and 51972200)the Graduate Innovation Fund of Shaanxi University of Science&Technology+2 种基金funded by the Japan Society for the Promotion of Science(JSPS)Grant-in-Aid for the Scientific Research(KAKENHI Nos.20H00297 and Innovative Area“Mixed Anion”(No.16H06439))the Nippon Sheet Glass Foundation for Materials Science and Engineeringby the Dynamic Alliance for Open Innovations Bridging Human,Environment and Materials,the Cooperative Research Program of“Network Joint Research Center for Materials and Devices”。
文摘Acetone,as widely used reagents in industry and laboratories,are extremely harmful to the human.So the detection of acetone gas concentrations and leaks in special environments at room temperature is essential.Herein,the nanocomposite combining SnO-SnO_(2)(p-n junction)and Ti_(3)C_(2)T_(x) MXene was successfully synthesized by a one-step hydrothermal method.Because of the existence of a small amount of oxygen during the hydrothermal conditions,part of the p-type SnO was oxidized to n-type SnO_(2),forming in-situ p-n junctions on the surface of Sn O.The hamburger-like SnO-SnO_(2)/Ti_(3)C_(2)T_(x) sensor exhibited improved acetone gas sensing response of 12.1(R_(g)/R_(a))at room temperature,which were nearly 11 and 4 times higher than those of pristine Ti_(3)C_(2)T_(x) and pristine SnO-SnO_(2),respectively.Moreover,it expressed a short recovery time(9 s)and outstanding reproducibility.Because of the different work functions,the Schottky barrier was formed between the SnO and the Ti_(3)C_(2)T_(x) nanosheets,acting as a hole accumulation layer(HALs)between Ti_(3)C_(2)T_(x) and tin oxides.Herein,the sensing mechanism based on the formation of hetero-junctions and high conductivity of the metallic phase of Ti_(3)C_(2)T_(x) MXene in SnO-SnO_(2)/Ti_(3)C_(2)T_(x) sensors was discussed in detail.
基金financially supported by Shandong Natural Science Foundation(No.ZR2021QE265)the Fundamental Research Funds of Taishan University(No.Y01-2020015)+1 种基金the National Natural Science Foundation of China(Nos.61574098,61204051)Shandong Province Key Research and Development Program(No.2019GGX101016)。
文摘Currently,SmFeO_(3)-based sensors are an effective platform for detecting acetone gas.However,they require high operating temperatures,which increases energy consumption and safety hazards,and their response is low when the gas concentration is at 10^(-9)(PPB),which cannot meet the requirements of using exhaled breath to pre-diagnose diabetes.Herein,Pd-SmFeO_(3)hollow nanotubes with an extremely high specific surface area and porosity were synthesized by electrospinning.After Pd doping,the specific surface area improved by more than two times,and the acetone response improved by more than three times.In addition,the response further improved by more than 1.5 times,and the optimum operating temperature reduced by 100℃under light irradiation.Moreover,the relative humidity adaptability,long-term stability,and selectivity of the material were significantly improved after Pd doping or light irradiation.Finally,the acetone concentration in a person’s exhaled breath was detected by a Pd-SmFeO_(3)-based gas sensor,and the error was less than 10%compared to that obtained by gas chromatography-mass spectrometry method.
基金Project(30916014103) supported by the Fundamental Research Funds for the Central Universities,China
文摘Ternary Au/Fe2O3-ZnO gas-sensing materials were synthesized by combining co-precipitation and microwave irradiation process.The as-prepared Au/Fe2O3-ZnO was characterized with X-ray diffractometer and scanning electron microscope,and its gas-sensing performance was measured using a gas-sensor analysis system.The results show that the as-prepared products consist of hexagonal wurtzite ZnO,face-centered cubic gold nanoparticles and orthorhombic Fe2O3crystallines.The Au/Fe2O3-ZnO based sensor has a very high selectivity to ethanol and acetone,and also has high sensitivity(154)at a low working temperature(270°C)and an extremely fast response(1s)against acetone.It is found that the selectivity can be adjusted by Fe2O3content added in the ternary materials.It possesses a worth looking forward prospect to practical applications in acetone detecting and administrating field.
文摘In recent years, clinical studies have found that acetone concentration in exhaled breath can be taken as a characteristic marker of diabetes. Metal-oxide-semiconductor (MOS) materials are widely used in acetone gas sensors due to their low cost, high sensitivity, fast response/recovery time, and easy integration. This paper reviews recent progress in acetone sensors based on MOS materials for diabetes diagnosis. The methods of improving the performance of acetone sensor have been explored for comparison, especially in high humidity conditions. We summarize the current excellent methods of preparations of sensors based on MOSs and hope to provide some help for the progress of acetone sensors in the diagnosis of diabetes.
基金Project supported by Shandong Natural Science Foundation(ZR2013EMM016)National Natural Science Foundation of China(51472145,51272133,51472150,J1103212)the Fundamental Research Funds for the Central Universities(DUT16RC(4)69)
文摘The PdC12 was mixed with nanocrystalline powders LaFeO3 and subsequently followed by an annealing of 800 ℃. PdO phase was formed and almost distributed uniformly on the surface of LaFeO3 nano-particles. With an increase of PdO amounts in composite powders, sensing sensitivity Rg/Ra to low concentration acetone or ethanol for Pd doped LaFeO3 sensors increased at first, underwent the maximum with 2 wt.% PdC12 dopant, and then doped again. Interestingly, appropriate Pd doping in LaFeO3 changed the selectivity behavior of gas sensing. LaFeO3 sensor showed good selectivity to ethanol, but 2 wt.% Pd doped LaFeO3 sensor showed good selectivity to acetone. The sensitivity for LaFeO3 at 200 ℃was 1.32 to 1 ppm ethanol, and 1.19 to 1 ppm acetone. Whereas the sensitivity for 2 wt.% Pd doped LaFeO3 at 200 ℃ was 1.53 to 1 ppm ethanol, and 1.9 to 1 ppm acetone. The 2 wt.% Pd doped LaFeO3 sensor at 200 ℃ showed very short response time (4 s) and recovery time (2 s) to 1 ppm acetone gas, respectively. Such results showed that 2 wt.% Pd doped LaFeO3 sensor is a new promising sensing candidate for detecting low concentration acetone.
基金supported by the National Natural Science Foundation of China (No. 21377008)the National High Technology Research and Development Program of China ("863"Program)(No. 2015AA034603)the Foundation of the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions
文摘Three-dimensionally ordered mesoporous Fe2O3(meso-Fe2O3) and its supported Au, Pd,and Au-Pd alloy(xA uP dy/meso-Fe2O3; x = 0.08–0.72 wt.%; Pd/Au molar ratio(y) = 1.48–1.85)photocatalysts have been prepared via the KIT-6-templating and polyvinyl alcohol-protected reduction routes, respectively. Physical properties of the samples were characterized, and their photocatalytic activities were evaluated for the photocatalytic oxidation of acetone in the presence of a small amount of H2O2 under visible-light illumination. It was found that the meso-Fe2O3 was rhombohedral in crystal structure. The as-obtained samples displayed a high surface area of 111.0–140.8 m^2/g and a bandgap energy of 1.98–2.12 eV. The Au, Pd and/or Au–Pd alloy nanoparticles(NPs) with a size of 3–4 nm were uniformly dispersed on the surface of the meso-Fe2O3 support. The 0.72 wt.% AuP d1.48/meso-Fe2O3 sample performed the best in the presence of 0.06 mol/L H2O2 aqueous solution, showing a 100% acetone conversion within4 hr of visible-light illumination. It was concluded that the good performance of 0.72 wt.%AuPd(1.48)/meso-Fe2O3 for photocatalytic acetone oxidation was associated with its ordered mesoporous structure, high adsorbed oxygen species concentration, plasmonic resonance effect between AuPd(1.48) NPs and meso-Fe2O3, and effective separation of the photogenerated charge carriers. In addition, the introduction of H2O2 and the involvement of the photo-Fenton process also played important roles in enhancing the photocatalytic activity of 0.72 wt.%AuPd(1.48)/meso-Fe2O3.
文摘In the present work, we synthesized Sm2O3 doped SnO2 in order to prepare a selective acetone sensor with fast response, quick recovery and good repeatability. Pure as well as 2 mol.%, 4 mol.%, 6 mol.% and 8 mol.% Sm2O3 doped SnO2 nanostructured samples were synthesized by using a co-precipitation method. The characterization of the samples was done by thermogravimetric and differential thermo-gravimetric analysis(TG-DTA), X-ray diffraction(XRD), field emission gun-scanning electron microscopy(FEG-SEM), energy dispersive analysis by X-rays(EDAX), high resolution scanning electron microscopy(HR-TEM), selected area X-ray diffraction(SAED), Brunauer-Emmet-Teller(BET) and ultraviolet-visible-near infrared(UV-Vis-NIR) spectroscopy techniques. The gas response studies of liquid petroleum gas, ammonia, ethanol and acetone vapor were carried out. The results showed that Sm doping systematically lowered operating temperature and enhanced the gas response and selectivity for acetone. The response and recovery time for 6 mol.% Sm2O3 doped SnO2 thick film at the operating temperature of 250 °C were 15 and 24 s, respectively.
基金supported by the National Natural Science Foundation of China(51672312,21373275)the Science and Technology Program of Wuhan,China(2016010101010018,2015070504020220)the Dean’s Research Fund–04257 from the Education University of Hong Kong~~
文摘TiO2hollow microspheres(TiO2‐HMSs)have attracted much attention because of their high photoreactivity,low density,and good permeability.However,anatase TiO2‐HMSs have poor thermal stability.In this study,surface‐fluorinated TiO2‐HMSs were assembled from hollow nanoparticles by the hydrothermal reaction of the mixed Ti(SO4)2–NH4HF–H2O2solution at180°C.The effect of the calcination temperature on the structure and photoreactivity of the TiO2‐HMSs was systematically investigated,which was evaluated by photocatalytic oxidation of acetone in air under ultraviolet irradiation.We found that after calcination at300°C,the photoreactivity of the TiO2‐HMSs decreases from1.39×10?3min?1(TiO2‐HMS precursor)to0.82×10?3min?1because of removal of surface‐adsorbed fluoride ions.With increasing calcination temperature from300to900°C,the building blocks of the TiO2‐HMSs evolve from truncated bipyramidal shaped hollow nanoparticles to round solid nanoparticles,and the photoreactivity of the TiO2‐HMSs steady increases from0.82×10?3to2.09×10?3min?1because of enhanced crystallization.Further increasing the calcination temperature to1000and1100°C results in a decrease of the photoreactivity,which is ascribed to a sharp decrease of the Brunauer–Emmett–Teller surface area and the beginning of the anatase–rutile phase transformation at1100°C.The effect of surface‐adsorbed fluoride ions on the thermal stability of the TiO2‐HMSs is also discussed.
基金supported by the National Natural Science Foundation of China (Nos. 51772130, 51972145)。
文摘The heterostructured NiWO_(4)/WO_(3) nanotubes(Ni/W NTs)were synthesized by using a facile self-assembly method on the sacrificial polystyrene(PS)nanofibers templates.Then,the Pt-decorated NiWO_(4)/WO_(3)(Pt@Ni/W)composite NTs were obtained through using an ultrasonic mixing method.The experimental results display that the order of gas-sensing performance is Pt@Ni/W>Ni/W>WO_(3).The 2wt.%Pt@Ni/W-5 NTs indicate the supreme acetone-sensing response(R_(air)/R_(gas)=58.4 at 100×10^(−6))at 375℃,which is 10.6 and 1.53 times that of the WO_(3) and NiWO_(4)/WO_(3) NTs,respectively.Additionally,the 2wt.%Pt@Ni/W-5 NTs also exhibit the dramatically high selectivity toward acetone against ethanol,methanal,methanol,NH_(3) and toluene.The Pt-decorated Ni/W NTs show the excellent responsivity and stability toward acetone,which is ascribed to the construction of heterostructured NiWO_(4)/WO_(3) and the spill-over effect of Pt nanoparticles.