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51.
Glycine(Gly) is ubiquitous in the atmosphere and plays a vital role in new particle formation(NPF).However,the potential mechanism of its on sulfuric acid(SA)-ammonia(A)clusters formation under various atmospheric conditions is still ambiguous.Herein,a(Gly)_x·(SA)_y·(A)_z(z≤x+y≤3) multicomponent system was investigated by using density functional theory(DFT) combined with Atmospheric Cluster Dynamics Code(ACDC) at different temperatures and precursor concentrations.The results show that Gly,with one carboxyl(-COOH) and one amine(-NH_2) group,can interact strongly with SA and A in two directions through hydrogen bonds or proton transfer.Within the relevant range of atmospheric concentrations,Gly can enhance the formation rate of SA-A-based clusters,especially at low temperature,low [SA],and median [A].The enhancement(R) of Gly on NPF can be up to 340 at T=218.15 K,[SA]=10~4,[A]=10~9,and [Gly]=10~7 molecules/cm~3.In addition,the main growth paths of clusters show that Gly molecules participate into cluster formation in the initial stage and eventually leave the cluster by evaporation in subsequent cluster growth at low [Gly],it acts as an important "transporter" to connect the smaller and larger cluster.With the increase of [Gly],it acts as a "participator" directly participating in NPF. 相似文献
52.
Ni Liu Yunguo Liu Guangming Zeng Jilai Gong Xiaofei Tan Shaobo Liu Luhua Jiang Meifang Li Zhihong Yin 《环境科学学报(英文版)》2020,32(1):10-23
Five biochars derived from lotus seedpod(LSP) were applied to examine and compare the adsorption capacity of 17β-estradiol(E2) from aqueous solution.The effect of KOH activation and the order of activation steps on material properties were discussed.The effect of contact time,initial concentration,p H,ionic strength and humic acid on E2 adsorption were investigated in a batch adsorption process.Experimental results demonstrated that the pseudo second-order model fitted the experimental data best and that adsorption equilibrium was reached within 20 hr.The efficiency of E2 removal increased with increasing E2 concentration and decreased with the increase of ionic strength.E2 adsorption on LSP-derived biochar(BCs) was influenced little by humic acid,and slightly affected by the solution p H when its value ranged from 4.0 to 9.0,but considerably affected at p H 10.0.Low environmental temperature is favorable for E2 adsorption.Chemisorption,π–π interactions,monolayer adsorption and electrostatic interaction are the possible adsorption mechanisms.Comparative studies indicated that KOH activation and the order of activation steps had significant impacts on the material.Post-treated biochar exhibited better adsorption capacity for E2 than direct treated,pretreated,and raw LSP biochar.Pyrolyzed biochar at higher temperature improved E2 removal.The excellent performance of BCs in removing E2 suggested that BCs have potential in E2 treatment and that the biochar directly treated by KOH would be a good choice for the treatment of E2 in aqueous solution,with its advantages of good efficiency and simple technology. 相似文献
53.
F-V_2 O_5-WO3/Ti02 catalysts were prepared by the impregnation method.As the content of F ions increased from 0.00 to 0.35 wt.%,the NO conversion of F-V_2 O_5-WO_3/TiO_2 catalysts initially increased and then decreased.The 0.2 F-V_2 O_5-WO_3/TiO_2 catalyst(0.2 wt.% F ion)exhibited the best denitration(De-NOx) performance,with more than 95% NO conversion in the temperature range 160-360℃,and 99.0% N2 selectivity between 110 and 280℃.The addition of an appropriate amount of F ions eroded the surface morphology of the catalyst and reduced its grain size,thus enhancing the NO conversion at low temperature as well as the sulfur and water resistance of the V_2 O_5-WO3/Ti02 catalyst.After selective catalytic reduction(SCR) reaction in a gas flow containing SO_2 and H_2 O,the number of NH3 adsorption sites,active component content,specific surface area and pore volume decreased to different degrees.Ammonium sulfate species deposited on the catalyst surface,which blocked part of the active sites and reduced the NO conversion performance of the catalyst.On-line thermal regeneration could not completely recover the catalyst activity,although it prolonged the cumulative life of the catalyst.In addition,a mechanism for the effects of S02 and H_2 O on catalyst NO conversion was proposed. 相似文献
54.
Peng Du Jianguo Liu Huaqiao Gui Jiaoshi Zhang Tongzhu Yu Jie Wang Yin Cheng Yihuai Lu Yawei Yao Qiang Fu ChihChieh Chen 《环境科学学报(英文版)》2020,32(1):238-249
PM_(2.5) separator directly affects the accuracy of PM_(2.5) sampling.The specification testing and evaluation for PM_(2.5) separator is particularly important,especially under China's wide variation of terrain and climate.In this study,first a static test apparatus based on polydisperse aerosol was established and calibrated to evaluate the performance of the PM_(2.5) separators.A uniform mixing chamber was developed to make particles mix completely.The aerosol concentration relative standard deviations of three test points at the same horizontal chamber position were less than 0.57%,and the particle size distribution obeyed logarithmic normal distribution with an R~2 of 0.996.The flow rate deviation between the measurement and the set point flow rate agreed to within ± 1.0% in the range of -40 to 50℃.Secondly,the separation,flow and loading characteristics of three cyclone separators(VSCC-A,SCC-A and SCC112) were evaluated using this system.The results showed that the 50% cutoff sizes(D_(50)) of the three cyclones were 2.48,2.47 and 2.44 μm when worked at the manufacturer's recommended flow rates,respectively.The geometric standard deviation(GSD) of the capture efficiency of VSCCA was 1.23,showed a slightly sharper than SCC-A(GSD = 1.27),while the SCC112 did not meet the relevant indicator(GSD = 1.2 ± 0.1) with a GSD = 1.44.The flow rate and loading test had a great effect on D_(50),while the GSD remained almost the same as before.In addition,the maintenance frequency under different air pollution conditions of the cyclones was summarized according to the loading test. 相似文献
55.
Because of its significant toxicological effects on the environment and human health,arsenic(As) is a major global issue.In this study,an Fe-based metal-organic framework(MOF)(Materials of Institut Lavoisier:MIL-100(Fe)) which was impregnated with reduced graphene oxide(rGO) by using a simple hydrothermal method and coated with birnessitetype manganese oxide(δ-MnO_2) using the one-pot reaction process(MIL-100(Fe)/rGO/δ-MnO_2 nanocomposites) was synthesized and applied successfully in As removal.The removal efficiency was rapid,the equilibrium was achieved in 40 min and 120 min for As(Ⅲ) and As(Ⅴ),respectively,at a level of 5 mg/L.The maximum adsorption capacities of As(Ⅲ) and As(Ⅴ) at pH 2 were 192.67 mg/g and 162.07 mg/g,respectively.The adsorbent revealed high stability in pH range 2-9 and saturated adsorbent can be fully regenerated at least five runs.The adsorption process can be described by the pseudo-second-order kinetic model and Langmuir monolayer adsorption.The adsorption mechanisms consisted of electrostatic interaction,oxidation and inner sphere surface complexation. 相似文献
56.
Ling Liu Qiuhua Zhou Xuezhi Yang Gang Li Jingzhu Zhang Xuehua Zhou Wei Jiang 《环境科学学报(英文版)》2020,32(5):105-116
Inhaled atmospheric fine particulate matter(PM_(2.5)) includes soluble and insoluble fractions,and each fraction can interact with cells and cause adverse effects.PM_(2.5) samples were collected in Jinan,China,and the soluble and insoluble fractions were separated.According to physiochemical characterization,the soluble fraction mainly contains watersoluble ions and organic acids,and the insoluble fraction mainly contains kaolinite,calcium carbonate and some organic carbon.The interaction between PM_(2.5) and model cell membranes was examined with a quartz crystal microbalance with dissipation(QCM-D) to quantify PM_(2.5) attachment on membranes and membrane disruption.The cytotoxicity of the total PM_(2.5) and the soluble and insoluble fractions,was investigated.Negatively charged PM_(2.5) can adhere to the positively charged membranes and disrupt them.PM_(2.5)also adheres to negatively charged membranes but does not cause membrane rupture.Therefore,electrostatic repulsion does not prevent PM_(2.5) attachment,but electrostatic attraction induces remarkable membrane rupture.The human lung epithelial cell line A549 was used for cytotoxicity assessment.The detected membrane leakage,cellular swelling and blebbing indicated a cell necrosis process.Moreover,the insoluble PM_(2.5) fraction caused a higher cell mortality and more serious cell membrane damage than the soluble fraction.The levels of reactive oxygen species(ROS) enhanced by the two fractions were not significantly different.The findings provide more information to better understand the mechanism of PM_(2.5) cytotoxicity and the effect of PM_(2.5) solubility on cytotoxicity. 相似文献
57.
Electrotrophs are microbes that can receive electrons directly from cathode in a microbial electrolysis cell (MEC). They not only participate in organic biosynthesis, but also be crucial in cathode-based bioremediation. However, little is known about the electrotrophic community in paddy soils. Here, the putative electrotrophs were enriched by cathodes of MECs constructed from five paddy soils with various properties using bicarbonate as an electron acceptor, and identified by 16S rRNA-gene based Illumina sequencing. The electrons were gradually consumed on the cathodes, and 25%–45% of which were recovered to reduce bicarbonate to acetic acid during MEC operation. Firmicutes was the dominant bacterial phylum on the cathodes, and Bacillus genus within this phylum was greatly enriched and was the most abundant population among the detected putative electrotrophs for almost all soils. Furthermore, several other members of Firmicutes and Proteobacteria may also participate in electrotrophic process in different soils. Soil pH, amorphous iron and electrical conductivity significantly influenced the putative electrotrophic bacterial community, which explained about 33.5% of the community structural variation. This study provides a basis for understanding the microbial diversity of putative electrotrophs in paddy soils, and highlights the importance of soil properties in shaping the community of putative electrotrophs. 相似文献
58.
Based on density functional theory (DFT) and basic structure models, the chemical reactions on the surface of vanadium-titanium based selective catalytic reduction (SCR) denitrification catalysts were summarized. Reasonable structural models (non-periodic and periodic structural models) are the basis of density functional calculations. A periodic structure model was more appropriate to represent the catalyst surface, and its theoretical calculation results were more comparable with the experimental results than a non-periodic model. It is generally believed that the SCR mechanism where NH3 and NO react to produce N2 and H2O follows an Eley-Rideal type mechanism. NH2NO was found to be an important intermediate in the SCR reaction, with multiple production routes. Simultaneously, the effects of H2O, SO2 and metal on SCR catalysts were also summarized. 相似文献
59.
60.
Shuyan Wang Lin Du Narcisse T. Tson Xiaotong Jiang Bo You Li Xu Zhaomin Yang Wenxing Wang 《环境科学学报(英文版)》2020,32(6):151-162
Methylglyoxal(CH_3COCHO,MG),which is one of the most abundant α-dicarbonyl compounds in the atmosphere,has been reported as a major source of secondary organic aerosol(SOA).In this work,the reaction of MG with hydroxyl radicals was studied in a 500 L smog chamber at(293±3) K,atmospheric pressure,(18±2)% relative humidity,and under different NOx and SO_2.Particle size distribution was measured by using a scanning mobility particle sizer(SMPS) and the results showed that the addition of SO_2 can promote SOA formation,while different NOx concentrations have different influences on SOA production.High NOx suppressed the SOA formation,whereas the particle mass concentration,particle number concentration and particle geometric mean diameter increased with the increasing NOx concentration at low NOx concentration in the presence of SO_2.In addition,the products of the OH-initiated oxidation of MG and the functional groups of the particle phase in the MG/OH/SO_2 and MG/OH/NOx/SO_2 reaction systems were detected by gas chromatography mass spectrometry(GC-MS) and attenuated total reflection fourier transformed infrared spectroscopy(ATR-FTIR) analysis.Two products,glyoxylic acid and oxalic acid,were detected by GC-MS.The mechanism of the reaction of MG and OH radicals that follows two main pathways,H atom abstraction and hydration,is proposed.Evidence is provided for the formation of organic nitrates and organic sulfate in particle phase from IR spectra.Incorporation of NOx and SO_2 influence suggested that SOA formation from anthropogenic hydrocarbons may be more efficient in polluted environment. 相似文献