Cerium dioxide, CeO2, is a potentially superior material in a myriad of areas, and many methods have been proposed to deposit single crystal CeO2 thin films. A novel fabrication technique utilizing dual plasma generat...Cerium dioxide, CeO2, is a potentially superior material in a myriad of areas, and many methods have been proposed to deposit single crystal CeO2 thin films. A novel fabrication technique utilizing dual plasma generated by metal vacuum arc (MEVVA) and radio frequency (RF) is discussed in this paper. We have recently conducted a systematic investigation to determine the optimal process window to deposit CeO2 thin films’on Si(100) substrates. The X-ray diffraction results show the existence of CeO2(100) in the as-deposited sample.展开更多
Cerium dioxide(CeO2) has attracted much attention and has wide applications such as automotive exhaust catalysts,polishing materials for optical glasses and additives for advanced glasses,as well as cosmetic materials...Cerium dioxide(CeO2) has attracted much attention and has wide applications such as automotive exhaust catalysts,polishing materials for optical glasses and additives for advanced glasses,as well as cosmetic materials.The particle size and its distribution are key factors to the performance of the materials in the functional applications.However,control of particle size is still a challenge in materials synthesis.Therefore,continuous precipitation of cerium oxalate(precursor of ceria) was carried out at different operational conditions such as reactant concentration,agitation speed,feeding rate and reaction temperature,and their effect on the particle size distribution,distribution width and morphology of cerium oxalate were investigated.The optimum conditions for preparing cerium oxalate with large particle size were determined based on orthogonal test as follows:[Ce(NO3)]=0.02 mol/L,agitation speed:200 r/min,feeding rate of solutions of cerium nitrate and oxalic acid:10 ml/min,reaction temperature:80 ℃.The results showed that the shape of cerium oxalate was sheet and the phase structure was amorphous.The median particle size of the final product was 27.60 μm,the particle size distribution width was very narrow and the micrograph was still sheet-like.Some attempts were made to explain the experimental phenomena in terms of agglomeration,disrupt,and precipitation kinetics.展开更多
The synthesis of ultrafine cerium dioxide precursor via homogeneous precipitation was studied. Mixed aqueous solution of anhydrous cerium nitrate and urea was first heated to 85℃ for 2 h, and the prepared suspension ...The synthesis of ultrafine cerium dioxide precursor via homogeneous precipitation was studied. Mixed aqueous solution of anhydrous cerium nitrate and urea was first heated to 85℃ for 2 h, and the prepared suspension was then aged at room temperature for various periods of time. White precipitate was finally collected by centrifuging and washed with distilled water and anhydrous ethanol. The obtained cerium dioxide (CeO2) precursor was observed with SEM. It was found that the morphology and size of the precursor were strongly affected by aging time and stirring conditions (with or without stirring).The precipitated fine spherical particles of the precursor changed their shape from ellipse to slice or directly to slice. Fine spherical monodispersed (300 nm) precursor powders could be obtained by controlling the aging time. Stirring the solution also could change the reaction process and thus the morphology and size of the precursor were changed.展开更多
The chlorinating mechanism of cerium dioxide was investigated by chlorinating CeO 2 with NH 4Cl and thermal analysis, which is useful for chlorinating RE minerals such as bastnasite by NH 4 Cl and preparing anhydrous ...The chlorinating mechanism of cerium dioxide was investigated by chlorinating CeO 2 with NH 4Cl and thermal analysis, which is useful for chlorinating RE minerals such as bastnasite by NH 4 Cl and preparing anhydrous RE chloride. The results indicate that NH 4Cl directly takes part in the chlorination of cerium dioxide by forming an intermediate CeOCl rather than by the HCl decomposed from NH 4Cl. Based on the chlorinating ratio of cerium dioxide being about 80% at 300 ℃ and decreasing at higher temperature, it is must be owing to thermal decomposition of CeCl 3·7H 2O. The thermal analysis experiments further prove the existence of CeOCl in the decomposition of CeCl 3·7H 2O, which loses 4H 2O, 5H 2O, 6H 2O and 7H 2O, stepwise and finally CeCl 3 is decomposed to CeOCl. Therefore chlorinating cerium dioxide with NH 4Cl should strictly control the temperature and time, and over dose NH 4Cl should be also applied as well.展开更多
In this work,we prepared a material with magnetic nanoparticles(Fe_(3)O_(4))as core,layered double hydroxides(LDHs)as affinity shell,and cerium dioxide(CeO_(2))as functional molecules(denoted as Fe_(3)O_(4)@LDH-CeO_(2...In this work,we prepared a material with magnetic nanoparticles(Fe_(3)O_(4))as core,layered double hydroxides(LDHs)as affinity shell,and cerium dioxide(CeO_(2))as functional molecules(denoted as Fe_(3)O_(4)@LDH-CeO_(2)).On the basis of combined immobilized metal ion affinity chromatography(IMAC)and metal oxide affinity chromatography(MOAC),Fe_(3)O_(4)@LDH-CeO_(2) was used to enrich phosphopeptides with high efficiency.The material exhibited high selectivity(α-casein:β-casein:BSA=1:1:5000,mass ratio),high recovery(95.87%),and good reusability of 10 times adsorption-desorption experiments.The feasibility of Fe_(3)O_(4)@LDH-CeO_(2) was further investigated by extracting phosphopeptides from biological samples(nonfat milk,serum,saliva,and A549 cell lysate).展开更多
The use of titanium dioxide nanoparticles (nTiO<sub>2</sub>) is gaining interest in agriculture because of their impact on many aspects of plant growth. The present study examines the effects of nTiO<su...The use of titanium dioxide nanoparticles (nTiO<sub>2</sub>) is gaining interest in agriculture because of their impact on many aspects of plant growth. The present study examines the effects of nTiO<sub>2</sub> (5 nm and 10 nm) applied to seeds and the seedlings as a foliar application on various aspects of growth characteristics and biomass accumulation in lettuce (Lactuca sativa, cv. Grand Rapids). Application of 10 nm nTiO<sub>2</sub> to seeds through imbibition resulted in a significant reduction in shoot biomass accumulation while 5 nm nTiO<sub>2</sub> did not affect the biomass accumulation in lettuce. The application of 10 nm nTiO<sub>2</sub> reduced the fresh shoot biomass accumulation by about 18% compared to the control plants. Other growth characteristics such as shoot dry biomass, root fresh and dry biomass, plant height, and leaf area were not affected by the application of both 5 nm and 10 nm nTiO<sub>2</sub>. In addition, foliar application of these nanoparticles to the lettuce seedlings did not have a significant effect on most of the growth parameters examined, and the increasing concentration ranging from 5 nm/L to 400 mg/L did not produce a consistent response in lettuce. Thus, nTiO<sub>2</sub> application to lettuce seeds had a notable negative impact on shoot growth while foliar application did not have a significant effect on many plant growth characteristics. However, foliar applications produced some symptoms of toxicity to the foliage in the form of necrotic or chlorotic patches on the leaves, which were more pronounced with increasing concentrations of both 5 nm and 10 nm nTiO<sub>2</sub>. However, these symptoms were apparent at a concentration as low as 50 mg/L of nTiO<sub>2</sub>. Thus, foliar application of nTiO<sub>2</sub> may not have a significant impact on many of the growth characteristics in lettuce, but it can result in foliar toxicity.展开更多
The reduction of phosphogypsum(PG)to lime slag and SO_(2)using coke can effectively alleviate the environmental problems caused by PG.However,the PG decomposition temperature remains high and the product yield remains...The reduction of phosphogypsum(PG)to lime slag and SO_(2)using coke can effectively alleviate the environmental problems caused by PG.However,the PG decomposition temperature remains high and the product yield remains poor.By adding additives,the decomposition temperature can be further reduced and PG decomposition rate and product yield can be improved.However,the use of current additives such as Fe_(2)O_(3)and SiO_(2)brings the problem of increasing economic cost.Therefore,it is proposed to use solid waste copper slag(CS)as a new additive to reduce PG to prepare SO2,which can reduce the cost and meet the environmental benefits at the same time.The effects of proportion,temperature and thermostatic time on PG decomposition are investigated by experimental and kinetic analysis combined with FactSage thermodynamic calculations to optimize the roasting conditions.Finally,the reaction mechanism is proposed.It is found that adding CS to the coke and PG system can increase the rate of PG decomposition and SO_(2)yield while lowering the PG decomposition temperature.For example,when the CS/PG mass ratio increases from 0 to 1,PG decomposition rate increases from 83.38%to 99.35%,SO_(2)yield increases from 78.62%to 96.81%,and PG decomposition temperature decreases from 992.4℃to 949.6℃.The optimal reaction parameters are CS/PG mass ratio of 1,Coke/PG mass ratio of 0.06 at 1100℃for 20 min with 99.35%PG decomposition rate and 96.81%SO_(2) yield.The process proceeds according to the following reactions:2CaSO_(4)+ 0.7C + 0.8Fe_(2)SiO_(4)→0.8Ca_(2)SiO_(4)+ 0.2Ca_(2)Fe_(2)O_(5)+ 0.4Fe_(3)O_(4)+2SO_(2)+ 0.7CO_(2)Finally,a process for decomposing PG with coke and CS is proposed.展开更多
The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challen...The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO_(2)in synthesizing a wide range of industrial products.Ultimately,the present study provides a unique perspective for achieving the vital goals of“peak shaving”and C-neutrality,contributing significantly to our collective efforts to combat climate change and its associated challenges.展开更多
Objective:To investigate the relationship between ambient sulfur dioxide(SO2)exposure and semen quality parameters.Methods:A systematic literature search was conducted to identify relevant studies investigating the as...Objective:To investigate the relationship between ambient sulfur dioxide(SO2)exposure and semen quality parameters.Methods:A systematic literature search was conducted to identify relevant studies investigating the association between SO2 exposure and semen quality parameters.This search encompassed the timeframe from January 2000 to May 2023 and included electronic databases such as Web of Science,Google Scholar,PubMed,Cochrane,and Scopus.Pooled effect estimates with 95%confidence intervals(CI)were calculated using percent changes(PC).The meta-analysis included seven studies with 6711 participants and 15087 semen samples.Results:The results revealed a significant negative association between ambient SO2 exposure and certain semen quality parameters.In particular,SO2 exposure was associated with a significant decrease in progressive motility(PC=0.032;95%CI:-0.063 to-0.001;P=0.044)and sperm concentration(PC=-0.020;95%CI:-0.036 to-0.005;P=0.012).However,no statistically significant associations were observed for total sperm count(PC=-0.038;95%CI:-0.079 to 0.003;P=0.070),seminal fluid volume(PC=-0.009;95%CI:-0.048 to-0.030;P=0.662)and sperm motility(PC=-0.17;95%CI:-0.363 to 0.022;P=0.830).In addition,the results of the subgroup analysis revealed specific variables that were associated with the decrease in relevant sperm parameters.Conclusions:This systematic review and meta-analysis provides compelling evidence supporting a consistent negative association between exposure to ambient SO2 and semen quality parameters.展开更多
Understanding the response of the Earth system to varying concentrations of carbon dioxide(CO_(2))is critical for projecting possible future climate change and for providing insight into mitigation and adaptation stra...Understanding the response of the Earth system to varying concentrations of carbon dioxide(CO_(2))is critical for projecting possible future climate change and for providing insight into mitigation and adaptation strategies in the near future.In this study,we generate a dataset by conducting an experiment involving carbon dioxide removal(CDR)—a potential way to suppress global warming—using the Chinese Academy of Sciences Earth System Model version 2.0(CASESM2.0).A preliminary evaluation is provided.The model is integrated from 200–340 years as a 1%yr^(−1) CO_(2) concentration increase experiment,and then to~478 years as a carbon dioxide removal experiment until CO_(2) returns to its original value.Finally,another 80 years is integrated in which CO_(2) is kept constant.Changes in the 2-m temperature,precipitation,sea surface temperature,ocean temperature,Atlantic meridional overturning circulation(AMOC),and sea surface height are all analyzed.In the ramp-up period,the global mean 2-m temperature and precipitation both increase while the AMOC weakens.Values of all the above variables change in the opposite direction in the ramp-down period,with a delayed peak relative to the CO_(2) peak.After CO_(2) returns to its original value,the global mean 2-m temperature is still~1 K higher than in the original state,and precipitation is~0.07 mm d^(–1) higher.At the end of the simulation,there is a~0.5°C increase in ocean temperature and a 1 Sv weakening of the AMOC.Our model simulation produces similar results to those of comparable experiments previously reported in the literature.展开更多
Drip irrigation and flood irrigation are major irrigation methods for maize crops in the Hetao Irrigation District,Inner Mongolia Autonomous Region,China.This research delves into the effects of these irrigation metho...Drip irrigation and flood irrigation are major irrigation methods for maize crops in the Hetao Irrigation District,Inner Mongolia Autonomous Region,China.This research delves into the effects of these irrigation methods on carbon dioxide(CO_(2))exchange and crop growth in this region.The experimental site was divided into drip and flood irrigation zones.The irrigation schedules of this study aligned with the local commonly used irrigation schedule.We employed a developed chamber system to measure the diurnal CO_(2)exchange of maize plants during various growth stages under both drip and flood irrigation methods.From May to September in 2020 and 2021,two sets of repeated experiments were conducted.In each experiment,a total of nine measurements of CO_(2)exchange were performed to obtain carbon exchange data at different growth stages of maize crop.During each CO_(2)exchange measurement event,CO_(2)flux data were collected every two hours over a day-long period to capture the diurnal variations in CO_(2)exchange.During each CO_(2)exchange measurement event,the biological parameters(aboveground biomass and crop growth rate)of maize and environmental parameters(including air humidity,air temperature,precipitation,soil water content,and photosynthetically active radiation)were measured.The results indicated a V-shaped trend in net ecosystem CO_(2)exchange in daytime,reducing slowly at night,while the net assimilation rate(net primary productivity)exhibited a contrasting trend.Notably,compared with flood irrigation,drip irrigation demonstrated significantly higher average daily soil CO_(2)emission and greater average daily CO_(2)absorption by maize plants.Consequently,within the maize ecosystem,drip irrigation appeared more conducive to absorbing atmospheric CO_(2).Furthermore,drip irrigation demonstrated a faster crop growth rate and increased aboveground biomass compared with flood irrigation.A strong linear relationship existed between leaf area index and light utilization efficiency,irrespective of the irrigation method.Notably,drip irrigation displayed superior light use efficiency compared with flood irrigation.The final yield results corroborated these findings,indicating that drip irrigation yielded higher harvest index and overall yield than flood irrigation.The results of this study provide a basis for the selection of optimal irrigation methods commonly used in the Hetao Irrigation District.This research also serves as a reference for future irrigation studies that consider measurements of both carbon emissions and yield simultaneously.展开更多
As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates hav...As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates have shown great potential for the preparation of single-atom catalytic materials.In this study,the solubilities of iron(Ⅲ)acetylacetonate(Fe(acac)3)and nickel(Ⅱ)acetylacetonate(Ni(acac)2)were measured at the temperature from 313.15 to 333.15 K and in the pressure range of 9.5–25.2 MPa to accumulate new solubility data.Solubility was measured using a static weight loss method.The semi-empirical models proposed by Chrastil and Sung et al.were used to correlate the solubility data of Fe(acac)3 and Ni(acac)2.The equations obtained can be used to predict the solubility of the same system in the experimental range.展开更多
Ozone(O3)is widely used in drinking water disinfection and wastewater treatment.However,when applied to bromide-containing water,ozone induces the formation of bromate,which is carcinogenic.Our previous study found...Ozone(O3)is widely used in drinking water disinfection and wastewater treatment.However,when applied to bromide-containing water,ozone induces the formation of bromate,which is carcinogenic.Our previous study found±at graphene oxide(GO)can enhance the degradation efficiency of micropollutants during ozonation.However,in this study,GO was found to promote bromate formation during ozonation of bromide-containing waters,with bromate yields from the O3/GO process more than twice those obtained using ozone alone.The promoted bromate formation was attributed to increased hydroxyl radical production,as confirmed by the significant reduction(almost 75%)in bromate yield after adding t-butanol(TBA).Cerium oxide(less tfian 5 mg/L)supported on reduced GO(xCeO2/RGO)significantly inhibited bromate formation during ozonation compared with reduced GO alone,and the optimal Ce atomic percentage(x)was determined to be 0.36%,achieving an inhibition rate of approximately 73%.Fourier transform infrared(FT-IR)spectra indicated the transformation of GO into RGO after hydrothermal treatment,and transmission electron microscope(TEM)results showed that CeO2 nanoparticles were well dispersed on the RGO surface.The X-ray photoelectron spectroscopy(XPS)spectra results demonstrated that the Ce^3+/Ce^4+ratio in xCeO2/RGO was almost 3-4 times higher than that in pure CeO2,which might be attributed to the charge transfer effect from GO to CeO2.Furthermore,Ce+on thexCeO2/RGO surface could quench Br-and BrO-to further inhibit bromate formation.Meanwhile,0.36CeO2/RGO could also enhance the degradation efficiency of N,N-diethyl-zn-toluamide(DEET)in synthetic and reclaimed water during ozonation.展开更多
CeO2 thin film was fabricated by dual ion beam epitaxial technique. The phenomenon of PL violet shift at room temperature was observed, and the distance of shift was about 65 nm. After the analysis of crystal structur...CeO2 thin film was fabricated by dual ion beam epitaxial technique. The phenomenon of PL violet shift at room temperature was observed, and the distance of shift was about 65 nm. After the analysis of crystal structure and valence in the compound were carried out by XRD and XPS technique, it was concluded that the PL shift was related with valence of cerium ion in the oxides. When the valence of cerium ion varied from tetravalence to trivalence, the PL peak position would move from blue region to violet region and the phenomenon of 'violet shift' was observed.展开更多
AIM: To investigate the apoptotic effect of photoexcited titanium dioxide (TiO2) nanoparticles in the presence of visible light on human hepatoma cell line (Bel 7402) and to study the underlying mechanism. METHODS: Ce...AIM: To investigate the apoptotic effect of photoexcited titanium dioxide (TiO2) nanoparticles in the presence of visible light on human hepatoma cell line (Bel 7402) and to study the underlying mechanism. METHODS: Cerium-element-doped titanium dioxide nanoparticles were prepared by impregnation method. Bel 7402 human hepatoma cells were cultured in RPMI 1640 medium in a humidified incubator with 50 mL/L CO2 at 37℃. A 15 W fluorescent lamp with continuous wavelength light was used as light source in the photocatalytic test. Fluorescence morphology and agarose gel eletrophoresis pattern were performed to analyze apoptotic cells. RESULTS: The Ce (Ⅳ)-doped TiO2 nanoparticles displayed their superiority. The adsorption edge shifted to the 400-450 nm region. With visible light illuminated for 10 min, 10 μg/cm3 Ce (Ⅳ)-doped TiO2 induced micronuclei and significant apoptosis in 4 and 24 h, respectively. Hochest 33 258 staining of the fixed cells revealed typical apoptotic structures (apoptotic bodies), agarose gel electrophoresis showed typical DNA ladder pattern in treated cells but not in untreated ones. CONCLUSION: Ce (Ⅳ) doped TiO2 nanoparticles can induce apoptosis of Bel 7402 human hepatoma cells in the presence of visible light.展开更多
Cerium dioxide was used for the first time as reactive sorbent for the degradation of the organophosphate pesticides parathion methyl,chlorpyrifos,dichlofenthion,fenchlorphos,and prothiofos,as well as of some chemical...Cerium dioxide was used for the first time as reactive sorbent for the degradation of the organophosphate pesticides parathion methyl,chlorpyrifos,dichlofenthion,fenchlorphos,and prothiofos,as well as of some chemical warfare agents—nerve gases soman and O-ethyl S-[2-(diisopropylamino) ethyl] methylphosphonothioate(VX).CeO2 specimens were prepared by calcination of basic cerous carbonate obtained by precipitation from an aqueous solution.The CeO2 samples containing certain amounts(1 wt.%–5 wt.%) of the neighboring lanthanides(La,Pr,Nd) were prepared in a similar way from pure lanthanide salts.It was shown that ceria accelerated markedly the decomposition of parathion methyl causing the cleavage of the P-O-aryl bond in the pesticide molecule.A similar reaction mechanism was proposed for the degradation of other organophosphate pesticides and nerve agents.The degradation times(reaction half-times) were in an order of minutes in the presence of CeO2,compared to hours or days under common environmental conditions.The reaction in suitable organic solvents allowed conversions of about 90% for parathion methyl loading of 20 mg pesticide/g CeO2 within 2 h with a reactant half-life in the order of 0.1 min.The key parameter governing the degradation efficiency of CeO2 was the temperature during calcination.At optimum calcination temperature(about 773.15 K),the produced ceria retained a sufficiently high surface area,and attained an optimum degree of crystallinity(related to a number of crystal defects,and thus potential reactive sites).The presence of other lanthanides somewhat decreased the reaction rate,but this effect was not detrimental and permitted the possible use of chemically impure ceria as a reactive sorbent.A fast organophosphate degradation was demonstrated not only in non-polar solvents(such as heptane),but also in polar aprotic solvents(acetonitrile,acetone) that are miscible with water.This opens new possibilities for designing more versatile decontamination strategies.The cleavage of phosphate ester bonds is of a great importance not only for the degradation of dangerous chemicals(chemical weapons,pesticides),but also for interactions of ceria(especially the nano-sized one) in biologically relevant systems.展开更多
Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybde...Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybdenum oxide,tungsten oxide,and cerium oxide were used to reconfigure the redox sites and acid sites of red mud based catalyst.When activated red mud was reconfigured by cerium-tungsten oxide(Ce-W@RM),the NOx conversion kept above 90%at 219-480℃.The existence of Ce^(3+)/Ce^(4+) redox electron pairs provided more surface adsorbed oxygen(O_(α)) and served as a redox cycle.Positive interactions between Ce,W species and Fe oxide in red mud occurred,which led to the formation of unsaturated chemical bond and promoted the activation of adsorbed NH_(3) species.WO_(3) and Ce_(2)(WO_(4))_(3)(formed by solid-state reaction between Ce and W species)could provide more Brønsted acid sites(W-O modes of WO_(3),W=O or W-O-W modes of Ce_(2)(WO_(4))_(3)).CeO_(2) species could provide more Lewis acid sites.The Langmuir-Hinshelwood(L-H)routes and Eley-Rideal(E-R)routes occurred in the low-temperature SCR reaction on the Ce-W@RM surface.NH_(4)^(+) species on Brønsted acid sites,NH_(3) species on Lewis acid sites,bidentate nitrate and bridging nitrate species were key active intermediates species.展开更多
CO_(2) electrolysis with solid oxide electrolytic cells(SOECs)using intermittently available renewable energy has potential applications for carbon neutrality and energy storage.In this study,a pulsed current strategy...CO_(2) electrolysis with solid oxide electrolytic cells(SOECs)using intermittently available renewable energy has potential applications for carbon neutrality and energy storage.In this study,a pulsed current strategy is used to replicate intermittent energy availability,and the stability and conversion rate of the cyclic operation by a large-scale flat-tube SOEC are studied.One hundred cycles under pulsed current ranging from -100 to -300 mA/cm^(2) with a total operating time of about 800 h were carried out.The results show that after 100 cycles,the cell voltage attenuates by 0.041%/cycle in the high current stage of−300 mA/cm^(2),indicating that the lifetime of the cell can reach up to about 500 cycles.The total CO_(2) conversion rate reached 52%,which is close to the theoretical value of 54.3% at -300 mA/cm^(2),and the calculated efficiency approached 98.2%,assuming heat recycling.This study illustrates the significant advantages of SOEC in efficient electrochemical energy conversion,carbon emission mitigation,and seasonal energy storage.展开更多
Perilla frutescens seed (PFS) oil is reported to inhibit skin photoaging;however, its effect on melanogenesis has not yet been investigated. Herein, we tested the anti-melanogenesis activity of an oil-based extract fr...Perilla frutescens seed (PFS) oil is reported to inhibit skin photoaging;however, its effect on melanogenesis has not yet been investigated. Herein, we tested the anti-melanogenesis activity of an oil-based extract from PFS with supercritical carbon dioxide (scCO<sub>2</sub>). In a cell culture system, B16 mouse melanoma cells were treated with the PFS scCO<sub>2</sub> extract and other samples. The PFS scCO<sub>2</sub> extract decreased melanin production by approximately 90% in B16 mouse melanoma cells without cytotoxicity at 100 μg/mL. This effect was greater than that of the well-known melanogenesis inhibitor, kojic acid. Although a hexane-extracted PFS oil and a squeezed PFS oil also decreased melanin production in the B16 cells, the inhibitory effect of the PFS scCO<sub>2</sub> extract was higher than both of these. Chemical analysis of the PFS scCO<sub>2</sub> extract and squeezed PFS oil showed that almost 90% of the components of both oils were α-linolenic acid, linoleic acid, and oleic acid. Furthermore, the ratio of those three fatty acids across both samples was almost the same. When the three fatty acids were mixed in the same ratio as in the PFS scCO<sub>2</sub> extract, the IC<sub>50</sub> of the mixture for melanin production in B16 melanoma cells was identical to that of the PFS scCO<sub>2</sub> extract. However, the IC<sub>50</sub> of the squeezed PFS oil was approximately 6.6 times higher than that of the mixture. Although those fatty acids are the main inhibitory ingredients against melanin production in all of the extracts, some factor(s) in the squeezed PFS reduce their affinity with the cells. These results indicated that the PFS scCO<sub>2</sub> extract could be a superior melanogenesis inhibitor. Although its main ingredients are probably the same as those of the squeezed PFS oil, it is necessary to extract with scCO<sub>2</sub> for stronger anti-melanogenesis activity.展开更多
基金The work was supported by Hong Kong RGC CERG9040344 and 9040412, RGC / Germany Joint Schemes9050084 and 9050150, and CityU S
文摘Cerium dioxide, CeO2, is a potentially superior material in a myriad of areas, and many methods have been proposed to deposit single crystal CeO2 thin films. A novel fabrication technique utilizing dual plasma generated by metal vacuum arc (MEVVA) and radio frequency (RF) is discussed in this paper. We have recently conducted a systematic investigation to determine the optimal process window to deposit CeO2 thin films’on Si(100) substrates. The X-ray diffraction results show the existence of CeO2(100) in the as-deposited sample.
基金supported by the National Natural Science Foundation of China (2056601, 50662002)
文摘Cerium dioxide(CeO2) has attracted much attention and has wide applications such as automotive exhaust catalysts,polishing materials for optical glasses and additives for advanced glasses,as well as cosmetic materials.The particle size and its distribution are key factors to the performance of the materials in the functional applications.However,control of particle size is still a challenge in materials synthesis.Therefore,continuous precipitation of cerium oxalate(precursor of ceria) was carried out at different operational conditions such as reactant concentration,agitation speed,feeding rate and reaction temperature,and their effect on the particle size distribution,distribution width and morphology of cerium oxalate were investigated.The optimum conditions for preparing cerium oxalate with large particle size were determined based on orthogonal test as follows:[Ce(NO3)]=0.02 mol/L,agitation speed:200 r/min,feeding rate of solutions of cerium nitrate and oxalic acid:10 ml/min,reaction temperature:80 ℃.The results showed that the shape of cerium oxalate was sheet and the phase structure was amorphous.The median particle size of the final product was 27.60 μm,the particle size distribution width was very narrow and the micrograph was still sheet-like.Some attempts were made to explain the experimental phenomena in terms of agglomeration,disrupt,and precipitation kinetics.
基金the Natural Science Foundation of Jiangsu Province under pro ject No.BK2002010.
文摘The synthesis of ultrafine cerium dioxide precursor via homogeneous precipitation was studied. Mixed aqueous solution of anhydrous cerium nitrate and urea was first heated to 85℃ for 2 h, and the prepared suspension was then aged at room temperature for various periods of time. White precipitate was finally collected by centrifuging and washed with distilled water and anhydrous ethanol. The obtained cerium dioxide (CeO2) precursor was observed with SEM. It was found that the morphology and size of the precursor were strongly affected by aging time and stirring conditions (with or without stirring).The precipitated fine spherical particles of the precursor changed their shape from ellipse to slice or directly to slice. Fine spherical monodispersed (300 nm) precursor powders could be obtained by controlling the aging time. Stirring the solution also could change the reaction process and thus the morphology and size of the precursor were changed.
文摘The chlorinating mechanism of cerium dioxide was investigated by chlorinating CeO 2 with NH 4Cl and thermal analysis, which is useful for chlorinating RE minerals such as bastnasite by NH 4 Cl and preparing anhydrous RE chloride. The results indicate that NH 4Cl directly takes part in the chlorination of cerium dioxide by forming an intermediate CeOCl rather than by the HCl decomposed from NH 4Cl. Based on the chlorinating ratio of cerium dioxide being about 80% at 300 ℃ and decreasing at higher temperature, it is must be owing to thermal decomposition of CeCl 3·7H 2O. The thermal analysis experiments further prove the existence of CeOCl in the decomposition of CeCl 3·7H 2O, which loses 4H 2O, 5H 2O, 6H 2O and 7H 2O, stepwise and finally CeCl 3 is decomposed to CeOCl. Therefore chlorinating cerium dioxide with NH 4Cl should strictly control the temperature and time, and over dose NH 4Cl should be also applied as well.
基金National Natural Science Foundation of China(Nos.22004073 and 21961024)Natural Science Foundation of Inner Mongolia,China(No.2020BS02010)+2 种基金Talent Research Support Funds from Government-Sponsored Institution of Inner Mongolia,China(No.RCQD19002)Inner Mongolia Minzu University Doctoral Research Startup Fund Project,China(No.BS516)Incentive Funding from Nano Innovation Institute(NII)of Inner Mongolia Minzu University,China.
文摘In this work,we prepared a material with magnetic nanoparticles(Fe_(3)O_(4))as core,layered double hydroxides(LDHs)as affinity shell,and cerium dioxide(CeO_(2))as functional molecules(denoted as Fe_(3)O_(4)@LDH-CeO_(2)).On the basis of combined immobilized metal ion affinity chromatography(IMAC)and metal oxide affinity chromatography(MOAC),Fe_(3)O_(4)@LDH-CeO_(2) was used to enrich phosphopeptides with high efficiency.The material exhibited high selectivity(α-casein:β-casein:BSA=1:1:5000,mass ratio),high recovery(95.87%),and good reusability of 10 times adsorption-desorption experiments.The feasibility of Fe_(3)O_(4)@LDH-CeO_(2) was further investigated by extracting phosphopeptides from biological samples(nonfat milk,serum,saliva,and A549 cell lysate).
文摘The use of titanium dioxide nanoparticles (nTiO<sub>2</sub>) is gaining interest in agriculture because of their impact on many aspects of plant growth. The present study examines the effects of nTiO<sub>2</sub> (5 nm and 10 nm) applied to seeds and the seedlings as a foliar application on various aspects of growth characteristics and biomass accumulation in lettuce (Lactuca sativa, cv. Grand Rapids). Application of 10 nm nTiO<sub>2</sub> to seeds through imbibition resulted in a significant reduction in shoot biomass accumulation while 5 nm nTiO<sub>2</sub> did not affect the biomass accumulation in lettuce. The application of 10 nm nTiO<sub>2</sub> reduced the fresh shoot biomass accumulation by about 18% compared to the control plants. Other growth characteristics such as shoot dry biomass, root fresh and dry biomass, plant height, and leaf area were not affected by the application of both 5 nm and 10 nm nTiO<sub>2</sub>. In addition, foliar application of these nanoparticles to the lettuce seedlings did not have a significant effect on most of the growth parameters examined, and the increasing concentration ranging from 5 nm/L to 400 mg/L did not produce a consistent response in lettuce. Thus, nTiO<sub>2</sub> application to lettuce seeds had a notable negative impact on shoot growth while foliar application did not have a significant effect on many plant growth characteristics. However, foliar applications produced some symptoms of toxicity to the foliage in the form of necrotic or chlorotic patches on the leaves, which were more pronounced with increasing concentrations of both 5 nm and 10 nm nTiO<sub>2</sub>. However, these symptoms were apparent at a concentration as low as 50 mg/L of nTiO<sub>2</sub>. Thus, foliar application of nTiO<sub>2</sub> may not have a significant impact on many of the growth characteristics in lettuce, but it can result in foliar toxicity.
基金financial support from the school-enterprise cooperation projects(2019-KYY-508101-0078).
文摘The reduction of phosphogypsum(PG)to lime slag and SO_(2)using coke can effectively alleviate the environmental problems caused by PG.However,the PG decomposition temperature remains high and the product yield remains poor.By adding additives,the decomposition temperature can be further reduced and PG decomposition rate and product yield can be improved.However,the use of current additives such as Fe_(2)O_(3)and SiO_(2)brings the problem of increasing economic cost.Therefore,it is proposed to use solid waste copper slag(CS)as a new additive to reduce PG to prepare SO2,which can reduce the cost and meet the environmental benefits at the same time.The effects of proportion,temperature and thermostatic time on PG decomposition are investigated by experimental and kinetic analysis combined with FactSage thermodynamic calculations to optimize the roasting conditions.Finally,the reaction mechanism is proposed.It is found that adding CS to the coke and PG system can increase the rate of PG decomposition and SO_(2)yield while lowering the PG decomposition temperature.For example,when the CS/PG mass ratio increases from 0 to 1,PG decomposition rate increases from 83.38%to 99.35%,SO_(2)yield increases from 78.62%to 96.81%,and PG decomposition temperature decreases from 992.4℃to 949.6℃.The optimal reaction parameters are CS/PG mass ratio of 1,Coke/PG mass ratio of 0.06 at 1100℃for 20 min with 99.35%PG decomposition rate and 96.81%SO_(2) yield.The process proceeds according to the following reactions:2CaSO_(4)+ 0.7C + 0.8Fe_(2)SiO_(4)→0.8Ca_(2)SiO_(4)+ 0.2Ca_(2)Fe_(2)O_(5)+ 0.4Fe_(3)O_(4)+2SO_(2)+ 0.7CO_(2)Finally,a process for decomposing PG with coke and CS is proposed.
基金supported by the National Key R&D Program of China(2018YFA0901700)the National Natural Science Foundation of China(31970038,22278241)+1 种基金a grant from the Institute Guo Qiang,Tsinghua University(2021GQG1016)the Department of Chemical Engineering-i BHE Joint Cooperation Fund。
文摘The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO_(2)in synthesizing a wide range of industrial products.Ultimately,the present study provides a unique perspective for achieving the vital goals of“peak shaving”and C-neutrality,contributing significantly to our collective efforts to combat climate change and its associated challenges.
文摘Objective:To investigate the relationship between ambient sulfur dioxide(SO2)exposure and semen quality parameters.Methods:A systematic literature search was conducted to identify relevant studies investigating the association between SO2 exposure and semen quality parameters.This search encompassed the timeframe from January 2000 to May 2023 and included electronic databases such as Web of Science,Google Scholar,PubMed,Cochrane,and Scopus.Pooled effect estimates with 95%confidence intervals(CI)were calculated using percent changes(PC).The meta-analysis included seven studies with 6711 participants and 15087 semen samples.Results:The results revealed a significant negative association between ambient SO2 exposure and certain semen quality parameters.In particular,SO2 exposure was associated with a significant decrease in progressive motility(PC=0.032;95%CI:-0.063 to-0.001;P=0.044)and sperm concentration(PC=-0.020;95%CI:-0.036 to-0.005;P=0.012).However,no statistically significant associations were observed for total sperm count(PC=-0.038;95%CI:-0.079 to 0.003;P=0.070),seminal fluid volume(PC=-0.009;95%CI:-0.048 to-0.030;P=0.662)and sperm motility(PC=-0.17;95%CI:-0.363 to 0.022;P=0.830).In addition,the results of the subgroup analysis revealed specific variables that were associated with the decrease in relevant sperm parameters.Conclusions:This systematic review and meta-analysis provides compelling evidence supporting a consistent negative association between exposure to ambient SO2 and semen quality parameters.
基金jointly supported by the National Key Research and Development Program of China (Grant No. 2022YFC3105000)the Youth Innovation Promotion Association of CAS (2022074)+3 种基金the National Natural Science Foundation of China (Grant Nos. 42005123, 42275173 and 41706028)the National Key Research and Development Program of China(2022YFE0106500)the 7th Youth Talent Support Project of Ningxia Hui Autonomous Region Association for Science and TechnologyNational Key Scientific and Technological Infrastructure project ‘‘Earth System Science Numerical Simulator Facility’’(EarthLab) for supporting the simulations in this study
文摘Understanding the response of the Earth system to varying concentrations of carbon dioxide(CO_(2))is critical for projecting possible future climate change and for providing insight into mitigation and adaptation strategies in the near future.In this study,we generate a dataset by conducting an experiment involving carbon dioxide removal(CDR)—a potential way to suppress global warming—using the Chinese Academy of Sciences Earth System Model version 2.0(CASESM2.0).A preliminary evaluation is provided.The model is integrated from 200–340 years as a 1%yr^(−1) CO_(2) concentration increase experiment,and then to~478 years as a carbon dioxide removal experiment until CO_(2) returns to its original value.Finally,another 80 years is integrated in which CO_(2) is kept constant.Changes in the 2-m temperature,precipitation,sea surface temperature,ocean temperature,Atlantic meridional overturning circulation(AMOC),and sea surface height are all analyzed.In the ramp-up period,the global mean 2-m temperature and precipitation both increase while the AMOC weakens.Values of all the above variables change in the opposite direction in the ramp-down period,with a delayed peak relative to the CO_(2) peak.After CO_(2) returns to its original value,the global mean 2-m temperature is still~1 K higher than in the original state,and precipitation is~0.07 mm d^(–1) higher.At the end of the simulation,there is a~0.5°C increase in ocean temperature and a 1 Sv weakening of the AMOC.Our model simulation produces similar results to those of comparable experiments previously reported in the literature.
基金supported by the Shandong Province Natural Science Foundation Youth Branch(ZR2023QC157)the National Natural Science Foundation of China(51979233)+1 种基金the Key Research and Development Project of Shaanxi Province(2022KW-47,2022NY-220)the Heze University Doctoral Research Fund(XY21BS24,XY22BS17).
文摘Drip irrigation and flood irrigation are major irrigation methods for maize crops in the Hetao Irrigation District,Inner Mongolia Autonomous Region,China.This research delves into the effects of these irrigation methods on carbon dioxide(CO_(2))exchange and crop growth in this region.The experimental site was divided into drip and flood irrigation zones.The irrigation schedules of this study aligned with the local commonly used irrigation schedule.We employed a developed chamber system to measure the diurnal CO_(2)exchange of maize plants during various growth stages under both drip and flood irrigation methods.From May to September in 2020 and 2021,two sets of repeated experiments were conducted.In each experiment,a total of nine measurements of CO_(2)exchange were performed to obtain carbon exchange data at different growth stages of maize crop.During each CO_(2)exchange measurement event,CO_(2)flux data were collected every two hours over a day-long period to capture the diurnal variations in CO_(2)exchange.During each CO_(2)exchange measurement event,the biological parameters(aboveground biomass and crop growth rate)of maize and environmental parameters(including air humidity,air temperature,precipitation,soil water content,and photosynthetically active radiation)were measured.The results indicated a V-shaped trend in net ecosystem CO_(2)exchange in daytime,reducing slowly at night,while the net assimilation rate(net primary productivity)exhibited a contrasting trend.Notably,compared with flood irrigation,drip irrigation demonstrated significantly higher average daily soil CO_(2)emission and greater average daily CO_(2)absorption by maize plants.Consequently,within the maize ecosystem,drip irrigation appeared more conducive to absorbing atmospheric CO_(2).Furthermore,drip irrigation demonstrated a faster crop growth rate and increased aboveground biomass compared with flood irrigation.A strong linear relationship existed between leaf area index and light utilization efficiency,irrespective of the irrigation method.Notably,drip irrigation displayed superior light use efficiency compared with flood irrigation.The final yield results corroborated these findings,indicating that drip irrigation yielded higher harvest index and overall yield than flood irrigation.The results of this study provide a basis for the selection of optimal irrigation methods commonly used in the Hetao Irrigation District.This research also serves as a reference for future irrigation studies that consider measurements of both carbon emissions and yield simultaneously.
基金financial support from the National Key Research and Development Program of China(2020YFA0710202)the National Natural Science Foundation of China(21978043,U1662130)+1 种基金Inner Mongolia University of Technology Scientific Research Initial Funding(DC2300001240)Talent Introduction Support Project of Inner Mongolia(DC2300001426).
文摘As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates have shown great potential for the preparation of single-atom catalytic materials.In this study,the solubilities of iron(Ⅲ)acetylacetonate(Fe(acac)3)and nickel(Ⅱ)acetylacetonate(Ni(acac)2)were measured at the temperature from 313.15 to 333.15 K and in the pressure range of 9.5–25.2 MPa to accumulate new solubility data.Solubility was measured using a static weight loss method.The semi-empirical models proposed by Chrastil and Sung et al.were used to correlate the solubility data of Fe(acac)3 and Ni(acac)2.The equations obtained can be used to predict the solubility of the same system in the experimental range.
文摘Ozone(O3)is widely used in drinking water disinfection and wastewater treatment.However,when applied to bromide-containing water,ozone induces the formation of bromate,which is carcinogenic.Our previous study found±at graphene oxide(GO)can enhance the degradation efficiency of micropollutants during ozonation.However,in this study,GO was found to promote bromate formation during ozonation of bromide-containing waters,with bromate yields from the O3/GO process more than twice those obtained using ozone alone.The promoted bromate formation was attributed to increased hydroxyl radical production,as confirmed by the significant reduction(almost 75%)in bromate yield after adding t-butanol(TBA).Cerium oxide(less tfian 5 mg/L)supported on reduced GO(xCeO2/RGO)significantly inhibited bromate formation during ozonation compared with reduced GO alone,and the optimal Ce atomic percentage(x)was determined to be 0.36%,achieving an inhibition rate of approximately 73%.Fourier transform infrared(FT-IR)spectra indicated the transformation of GO into RGO after hydrothermal treatment,and transmission electron microscope(TEM)results showed that CeO2 nanoparticles were well dispersed on the RGO surface.The X-ray photoelectron spectroscopy(XPS)spectra results demonstrated that the Ce^3+/Ce^4+ratio in xCeO2/RGO was almost 3-4 times higher than that in pure CeO2,which might be attributed to the charge transfer effect from GO to CeO2.Furthermore,Ce+on thexCeO2/RGO surface could quench Br-and BrO-to further inhibit bromate formation.Meanwhile,0.36CeO2/RGO could also enhance the degradation efficiency of N,N-diethyl-zn-toluamide(DEET)in synthetic and reclaimed water during ozonation.
基金This work was supported by the Special Fund for the Major State Basic Research Project (Grant No. G200(X)36505).
文摘CeO2 thin film was fabricated by dual ion beam epitaxial technique. The phenomenon of PL violet shift at room temperature was observed, and the distance of shift was about 65 nm. After the analysis of crystal structure and valence in the compound were carried out by XRD and XPS technique, it was concluded that the PL shift was related with valence of cerium ion in the oxides. When the valence of cerium ion varied from tetravalence to trivalence, the PL peak position would move from blue region to violet region and the phenomenon of 'violet shift' was observed.
文摘AIM: To investigate the apoptotic effect of photoexcited titanium dioxide (TiO2) nanoparticles in the presence of visible light on human hepatoma cell line (Bel 7402) and to study the underlying mechanism. METHODS: Cerium-element-doped titanium dioxide nanoparticles were prepared by impregnation method. Bel 7402 human hepatoma cells were cultured in RPMI 1640 medium in a humidified incubator with 50 mL/L CO2 at 37℃. A 15 W fluorescent lamp with continuous wavelength light was used as light source in the photocatalytic test. Fluorescence morphology and agarose gel eletrophoresis pattern were performed to analyze apoptotic cells. RESULTS: The Ce (Ⅳ)-doped TiO2 nanoparticles displayed their superiority. The adsorption edge shifted to the 400-450 nm region. With visible light illuminated for 10 min, 10 μg/cm3 Ce (Ⅳ)-doped TiO2 induced micronuclei and significant apoptosis in 4 and 24 h, respectively. Hochest 33 258 staining of the fixed cells revealed typical apoptotic structures (apoptotic bodies), agarose gel electrophoresis showed typical DNA ladder pattern in treated cells but not in untreated ones. CONCLUSION: Ce (Ⅳ) doped TiO2 nanoparticles can induce apoptosis of Bel 7402 human hepatoma cells in the presence of visible light.
基金Project supported by Czech Science Foundation(P106/12/1116)
文摘Cerium dioxide was used for the first time as reactive sorbent for the degradation of the organophosphate pesticides parathion methyl,chlorpyrifos,dichlofenthion,fenchlorphos,and prothiofos,as well as of some chemical warfare agents—nerve gases soman and O-ethyl S-[2-(diisopropylamino) ethyl] methylphosphonothioate(VX).CeO2 specimens were prepared by calcination of basic cerous carbonate obtained by precipitation from an aqueous solution.The CeO2 samples containing certain amounts(1 wt.%–5 wt.%) of the neighboring lanthanides(La,Pr,Nd) were prepared in a similar way from pure lanthanide salts.It was shown that ceria accelerated markedly the decomposition of parathion methyl causing the cleavage of the P-O-aryl bond in the pesticide molecule.A similar reaction mechanism was proposed for the degradation of other organophosphate pesticides and nerve agents.The degradation times(reaction half-times) were in an order of minutes in the presence of CeO2,compared to hours or days under common environmental conditions.The reaction in suitable organic solvents allowed conversions of about 90% for parathion methyl loading of 20 mg pesticide/g CeO2 within 2 h with a reactant half-life in the order of 0.1 min.The key parameter governing the degradation efficiency of CeO2 was the temperature during calcination.At optimum calcination temperature(about 773.15 K),the produced ceria retained a sufficiently high surface area,and attained an optimum degree of crystallinity(related to a number of crystal defects,and thus potential reactive sites).The presence of other lanthanides somewhat decreased the reaction rate,but this effect was not detrimental and permitted the possible use of chemically impure ceria as a reactive sorbent.A fast organophosphate degradation was demonstrated not only in non-polar solvents(such as heptane),but also in polar aprotic solvents(acetonitrile,acetone) that are miscible with water.This opens new possibilities for designing more versatile decontamination strategies.The cleavage of phosphate ester bonds is of a great importance not only for the degradation of dangerous chemicals(chemical weapons,pesticides),but also for interactions of ceria(especially the nano-sized one) in biologically relevant systems.
基金supported by the National Natural Science Foundation of China(21906090)the National Key Research and Development Program(2017YFC0210200,2017YFC0212800)Primary Research&Development Project of Shandong Province(2018GSF117034,2019JZZY020305).
文摘Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybdenum oxide,tungsten oxide,and cerium oxide were used to reconfigure the redox sites and acid sites of red mud based catalyst.When activated red mud was reconfigured by cerium-tungsten oxide(Ce-W@RM),the NOx conversion kept above 90%at 219-480℃.The existence of Ce^(3+)/Ce^(4+) redox electron pairs provided more surface adsorbed oxygen(O_(α)) and served as a redox cycle.Positive interactions between Ce,W species and Fe oxide in red mud occurred,which led to the formation of unsaturated chemical bond and promoted the activation of adsorbed NH_(3) species.WO_(3) and Ce_(2)(WO_(4))_(3)(formed by solid-state reaction between Ce and W species)could provide more Brønsted acid sites(W-O modes of WO_(3),W=O or W-O-W modes of Ce_(2)(WO_(4))_(3)).CeO_(2) species could provide more Lewis acid sites.The Langmuir-Hinshelwood(L-H)routes and Eley-Rideal(E-R)routes occurred in the low-temperature SCR reaction on the Ce-W@RM surface.NH_(4)^(+) species on Brønsted acid sites,NH_(3) species on Lewis acid sites,bidentate nitrate and bridging nitrate species were key active intermediates species.
基金National Key Research&Development Project,Grant/Award Number:2017YFE0129300Ningbo Science and Technology Innovation 2025 Major Project,Grant/Award Numbers:2019B10046,2020Z107+2 种基金Zhejiang Provincial Key R&D Program,Grant/Award Number:2021C01101National Natural Science Foundation of China,Grant/Award Numbers:U20A20251,11932005The from 0 to 1 Innovative Program of CAS,Grant/Award Number:ZDBS-LY-JSC021。
文摘CO_(2) electrolysis with solid oxide electrolytic cells(SOECs)using intermittently available renewable energy has potential applications for carbon neutrality and energy storage.In this study,a pulsed current strategy is used to replicate intermittent energy availability,and the stability and conversion rate of the cyclic operation by a large-scale flat-tube SOEC are studied.One hundred cycles under pulsed current ranging from -100 to -300 mA/cm^(2) with a total operating time of about 800 h were carried out.The results show that after 100 cycles,the cell voltage attenuates by 0.041%/cycle in the high current stage of−300 mA/cm^(2),indicating that the lifetime of the cell can reach up to about 500 cycles.The total CO_(2) conversion rate reached 52%,which is close to the theoretical value of 54.3% at -300 mA/cm^(2),and the calculated efficiency approached 98.2%,assuming heat recycling.This study illustrates the significant advantages of SOEC in efficient electrochemical energy conversion,carbon emission mitigation,and seasonal energy storage.
文摘Perilla frutescens seed (PFS) oil is reported to inhibit skin photoaging;however, its effect on melanogenesis has not yet been investigated. Herein, we tested the anti-melanogenesis activity of an oil-based extract from PFS with supercritical carbon dioxide (scCO<sub>2</sub>). In a cell culture system, B16 mouse melanoma cells were treated with the PFS scCO<sub>2</sub> extract and other samples. The PFS scCO<sub>2</sub> extract decreased melanin production by approximately 90% in B16 mouse melanoma cells without cytotoxicity at 100 μg/mL. This effect was greater than that of the well-known melanogenesis inhibitor, kojic acid. Although a hexane-extracted PFS oil and a squeezed PFS oil also decreased melanin production in the B16 cells, the inhibitory effect of the PFS scCO<sub>2</sub> extract was higher than both of these. Chemical analysis of the PFS scCO<sub>2</sub> extract and squeezed PFS oil showed that almost 90% of the components of both oils were α-linolenic acid, linoleic acid, and oleic acid. Furthermore, the ratio of those three fatty acids across both samples was almost the same. When the three fatty acids were mixed in the same ratio as in the PFS scCO<sub>2</sub> extract, the IC<sub>50</sub> of the mixture for melanin production in B16 melanoma cells was identical to that of the PFS scCO<sub>2</sub> extract. However, the IC<sub>50</sub> of the squeezed PFS oil was approximately 6.6 times higher than that of the mixture. Although those fatty acids are the main inhibitory ingredients against melanin production in all of the extracts, some factor(s) in the squeezed PFS reduce their affinity with the cells. These results indicated that the PFS scCO<sub>2</sub> extract could be a superior melanogenesis inhibitor. Although its main ingredients are probably the same as those of the squeezed PFS oil, it is necessary to extract with scCO<sub>2</sub> for stronger anti-melanogenesis activity.
