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Lignocellulosic biomass offers the most abundant renewable resource in replacing traditional fossil resources. However, it is still a major challenge to directly convert the lignin component into value-added materials. The availability of plentiful hydroxyl groups in lignin macromolecules and its unique three-dimensional structure make it an ideal precursor for mesoporous biosorbents. In this work, we reported an environmentally friendly and economically feasible method for the fabrication of mesoporous lignin-based biosorbent (MLBB) from lignocellulosic biomass through a SO3 micro-thermal-explosion process, as a byproduct of microcrystalline cellulose. BET analysis reveal the average pore-size distribution of 5.50 nm, the average pore value of 0.35 cm3/g, and the specific surface area of 186 m2/g. The physicochemical properties of MLBB were studied by fourier transform infrared spectroscopy (FTIR), attenuated-total-reflection fourier transform infrared spectroscopy (ATR-FTIR), X-ray photoelectron spectroscopy (XPS), and element analysis. These results showed that there are large amounts of sulfonic functional groups existing on the surface of this biosorbent. Pb(II) was used as a model heavy-metal-ion to demonstrate the technical feasibility for heavy-metal-ion removal. Considering that lignocellulosic biomass is a naturally abundant and renewable resource and SO3 micro-thermal-explosion is a proven technique, this biosorbent can be easily produced at large scale and become a sustainable and reliable resource for wastewater treatment.  相似文献   

3.
中小燃煤锅炉PM2.5排放特征实测研究   总被引:1,自引:0,他引:1  
楼晟荣 《环境科学学报》2014,34(12):3119-3125
中小燃煤锅炉是我国工业和民用部门最主要的供热方式,掌握其一次颗粒物的排放特征对于研究大气PM2.5的来源和控制途径具有重要意义.本研究通过实测中小燃煤锅炉烟气,获得了中小燃煤锅炉PM2.5及以下粒径段的排放因子和分布,并分析了各粒径段的颗粒密度及除尘装置的去除效率.研究发现,PM2.5质量排放因子平均为(0.123±0.061)kg·t-1,PM2.5粒子数的排放因子平均为(3.17±1.65)×105t-1,烟气中70~120 nm粒径段的积聚模态颗粒在质量和数量上都高于其他粒径段.锅炉燃烧负荷是影响锅炉PM2.5排放的重要因素,锅炉的燃烧负荷越低,PM2.5排放将随之降低.实测锅炉的PM2.5排放因子显著低于物料衡算结果,说明采用物料衡算方法可能极大地高估了现有排放清单中工业燃煤锅炉的一次PM2.5排放量.  相似文献   

4.
For the removal of phosphate (PO43 -) from water, an adsorbent was prepared via carbonization of sewage sludge from a wastewater treatment plant: carbonized sludge adsorbent (CSA). The mechanism of phosphate removal was determined after studying the structure and chemical properties of the CSA and its influence on phosphate removal. The results demonstrate that phosphate adsorption by the CSA can be fitted with the pseudo second-order kinetics and Langmuir isotherm models, indicating that the adsorption is single molecular layer adsorption dominated by chemical reaction. The active sites binding phosphate on the surface are composed of mineral particles containing Si/Ca/Al/Fe. The mineral containing Ca, calcite, is the main factor responsible for phosphate removal. The phosphate removal mechanism is a complex process including crystallization via the interaction between Ca2 + and PO43 -; formation of precipitates of Ca2 +, Al3 +, and PO43 -; and adsorption of PO43 - on some recalcitrant oxides composed of Si/Al/Fe.  相似文献   

5.
杭州市大气超细颗粒数浓度谱季节性特征   总被引:9,自引:5,他引:4  
利用快速迁移率粒径谱仪(fast mobility particle sizer,FMPS)对杭州市大气超细颗粒进行监测,并对杭州市2011~2012年大气超细颗粒物的数浓度、粒径分布的季节变化及其与气象之间的关系进行研究.结果表明,杭州市超细颗粒数浓度呈对数双峰分布,季节变化特征为冬季>夏季>春季>秋季,12月值最高,为3.56×104cm-3,10月最低,为2.51×104cm-3.CMD(count medium diameter)季节变化特征为春>冬>秋>夏,4月最高,为53.51 nm;6月最低,为16.68 nm.气象因素对超细颗粒数浓度有一定影响.  相似文献   

6.
Fe2O3/MIL-53(Al)催化类芬顿氧化性能及其作用机制研究   总被引:1,自引:0,他引:1  
以MIL-53(Al)和铁盐为原料,采用浸渍-焙烧的方法,制备了Fe_2O_3/MIL-53(Al)类芬顿催化剂.通过扫描电子显微镜(SEM)、射透射电子显微镜(TEM)、X射线衍射仪(XRD)、傅里叶变换红外光谱仪(FTIR)及X射线光电子能谱仪(XPS),对Fe_2O_3/MIL-53(Al)、MIL-53(Al)及Fe_2O_3 3种材料的理化性质进行了表征.以亚甲基蓝为相关材料催化类芬顿反应氧化性能的指示剂,考察了Fe_2O_3/MIL-53(Al)、MIL-53(Al)及Fe_2O_3 3种材料催化类芬顿反应的活性.探讨了Fe_2O_3/MIL-53(Al)催化活性强化的相关作用机制.研究结果表明,Fe_2O_3/MIL-53(Al)的物化结构特征是以赤铁矿为主的纳米Fe_2O_3颗粒均匀、离散地分布在MIL-53(Al)之上,纳米Fe_2O_3颗粒尺寸大多集中在1~5 nm.与未负载纳米Fe_2O_3相比,其分散性和颗粒尺寸都展现出潜在优越性.Fe_2O_3/MIL-53(Al)材料催化类芬顿反应降解水溶液中亚甲基蓝的效果是未负载纳米Fe_2O_3的4.8倍(以反应速率常数计),且TOC去除率亦有明显优势.自由基猝灭实验结果表明Fe_2O_3/MIL-53(Al)催化类芬顿降解污染物的主要活性氧类物质为羟基自由基.MIL-53(Al)孔结构发达、孔分布均匀及孔尺寸较小且均一等结构特征,导致负载其中的Fe_2O_3具有孔道负载量大、颗粒分布离散且均匀、颗粒粒径小且均一等特点,从而强化了纳米Fe_2O_3催化类芬顿反应氧化降解水中污染物的性能.  相似文献   

7.
聚合氯化铝中纳米Al13形态的分离纯化及形态表征   总被引:13,自引:2,他引:11  
采用超滤法和层析法分离纯化聚合氯化铝(PAC)中的Al13形态,并采用Al-Ferron逐时络合比色法、27Al-NMR、TEM和粒度测定仪对分离纯化所得的Al13形态进行了分析和表征.研究结果表明,超滤法分离纯化的效果受超滤膜的孔径及PAC浓度的影响,选择合适孔径的膜和PAC溶液浓度即可以获得高纯度的Al13,在层析法中则随着洗脱时间延长按分子的大小依次洗脱下来,因此截取中间组分即可得到Al13;Al-Ferron逐时络合比色法和27Al-NMR的分析结果表明,采用上述2种方法分离提纯得到的样品中Al13的含量分别可达到90%以上和100%.TEM和粒度测定结果表明,在B=2.5的PAC溶液中,Al13极少以Al12AlO4(OH)24(H2O)7+12的单体形态存在,而是呈两维结构的线性和枝状的聚集体,Al12AlO4(OH)24(H2O)7+12的聚集体尺寸通常在几十至几百nm.  相似文献   

8.
Knowledge of particle number size distribution(PND) and new particle formation(NPF)events in Southern China is essential for mitigation strategies related to submicron particles and their effects on regional air quality,haze,and human health.In this study,seven field measurement campaigns were conducted from December 2013 to May 2015 using a scanning mobility particle sizer(SMPS) at four sites in Southern China,including three urban sites and one background site.Particles were measured in the size range of15-515 nm,and the median particle number concentrations(PNCs) were found to vary in the range of 0.3× 10~4-2.2 × 10~4 cn~(-3) at the urban sites and were approximately 0.2 × 10~4 cm~(-3) at the background site.The peak diameters at the different sites varied largely from 22 to 102 nm.The PNCs in the Aitken mode(25-100 nm) at the urban sites were up to 10 times higher than they were at the background site,indicating large primary emissions from traffic at the urban sites.The diurnal variations of PNCs were significantly influenced by both rush hour traffic at the urban sites and NPF events.The frequencies of NPF events at the different sites were0%-30%,with the highest frequency occurring at an urban site during autumn.With higher SO_2 concentrations and higher ambient temperatures being necessary,NPF at the urban site was found to be more influenced by atmospheric oxidizing capability,while NPF at the background site was limited by the condensation sink.This study provides a unique dataset of particle number and size information in various environments in Southern China,which can help understand the sources,formation,and the climate forcing of aerosols in this quickly developing region,as well as help constrain and validate NPF modeling.  相似文献   

9.
There is an increasing world wide demand for energy crops and animal manures for biogas production. To meet these demands, this research project aimed at optimising anaerobic digestion of maize and dairy cattle manures. Methane production was measured for 60 days in 1 l eudiometer batch digesters at 38 °C. Manure received from dairy cows with medium milk yield that were fed a well balanced diet produced the highest specific methane yield of 166.3 Nl CH4 kg VS−1. Thirteen early to late ripening maize varieties were grown on several locations in Austria. Late ripening varieties produced more biomass than medium or early ripening varieties. On fertile locations in Austria more than 30 Mg VS ha−1 can be produced. The methane yield declined as the crop approaches full ripeness. With late ripening maize varieties, yields ranged between 312 and 365 Nl CH4 kg VS−1 (milk ripeness) and 268–286 Nl CH4 kg VS−1 (full ripeness). Silaging increased the methane yield by about 25% compared to green, non-conserved maize. Maize (Zea mays L.) is optimally harvested, when the product from specific methane yield and VS yield per hectare reaches a maximum. With early to medium ripening varieties (FAO 240–390), the optimum harvesting time is at the “end of wax ripeness”. Late ripening varieties (FAO ca. 600) may be harvested later, towards “full ripeness”. Maximum methane yield per hectare from late ripening maize varieties ranged between 7100 and 9000 Nm3 CH4 ha−1. Early and medium ripening varieties yielded 5300–8500 Nm3 CH4 ha−1 when grown in favourable regions. The highest methane yield per hectare was achieved from digestion of whole maize crops. Digestion of corns only or of corn cob mix resulted in a reduction in methane yield per hectare of 70 and 43%, respectively. From the digestion experiments a multiple linear regression equation, the Methane Energy Value Model, was derived that estimates methane production from the composition of maize. It is a helpful tool to optimise biogas production from energy crops. The Methane Energy Value Model requires further validation and refinement.  相似文献   

10.
The aerosol number concentration and size distribution as well as size-resolved particle chemical composition were measured during haze and photochemical smog episodes in Shanghai in 2009. The number of haze days accounted for 43%, of which 30% was severe (visibility 〈 2 km) and moderate (2 km 〈 visibility 〈 3 km) haze, mainly distributed in winter and spring. The mean particle number concentration was about 17,000/cm3 in haze, more than 2 times that in clean days. The greatest increase of particle number concentration was in 0.5-1μm and 1-10 μm size fractions during haze events, about 17.78 times and 8.78 times those of clean days. The largest increase of particle number concentration was within 50-100 nm and 100-200 nm fractions during photochemical smog episodes, about 5.89 times and 4.29 times those of clean days. The particle volume concentration and surface concentration in haze, photochemical smog and clean days were 102, 49, 15 μm3/cm3 and 949, 649, 206 μm2/cm3, respectively. As haze events got more severe, the number concentration of particles smaller than 50 nm decreased, but the particles of 50-200 nm and 0.5-1μm increased. The diurnal variation of particle number concentration showed a bimodal pattern in haze days. All soluble ions were increased during haze events, of which NH4, SO24- and NO3 increased great/y, followed by Na+, IC, Ca2+ and CI-. These ions were very different in size-resolved particles during haze and photochemical smog episodes.  相似文献   

11.
An OH radical measurement instrument based on Fluorescence Assay by Gas Expansion(FAGE)has been developed in our laboratory.Ambient air is introduced into a low-pressure fluorescence cell through a pinhole aperture and irradiated by a dye laser at a high repetition rate of 8.5 k Hz.The OH radical is both excited and detected at 308 nm using A-X(0,0)band.To satisfy the high efficiency needs of fluorescence collection and detection,a 4-lens optical system and a self-designed gated photomultiplier(PMT)is used,and gating is actualized by switching the voltage applied on the PMT dynodes.A micro channel photomultiplier(MCP)is also prepared for fluorescence detection.Then the weak signal is accumulated by a photon counter in a specific timing.The OH radical excitation spectrum range in the wavelength of 307.82–308.2 nm is detected and the excited line for OH detection is determined to be Q_1(2)line.The calibration of the FAGE system is researched by using simultaneous photolysis of H_2O and O_2.The minimum detection limit of the instrument using gated PMT is determined to be 9.4×10~5molecules/cm~3,and the sensitivity is 9.5×10~(-7)cps/(OH·cm~(-3)),with a signal-to-noise ratio of 2 and an integration time of 60 sec,while OH detection limit and the detection sensitivity using MCP is calculated to be 1.6×10~5molecules/cm~3and 2.3×10~(-6)cps/(OH·cm~(-3)).The laboratory OH radical measurement is carried out and results show that the proposed system can be used for atmospheric OH radical measurement.  相似文献   

12.
杭州灰霾天气超细颗粒浓度分布特征   总被引:11,自引:7,他引:4  
陈秋方  孙在  谢小芳 《环境科学》2014,35(8):2851-2856
利用快速迁移率粒径谱仪(FMPS)对杭州2013年12月6~11日连续灰霾天气和灰霾消退过程超细颗粒进行监测,分析颗粒物浓度变化和粒径谱分布特征及其与气象的相关性.结果表明,颗粒物日变化特征为夜晚数浓度较高,凌晨数浓度开始降低,08:00和18:00上下班高峰期出现一个小峰值,体现出明显的交通源峰值,表明交通排放对大气污染影响较大.灰霾天气下颗粒物最高数浓度达到8.0×104cm-3.粒径谱呈双峰分布,峰值粒径分别为15 nm和100 nm,粒径在100 nm附近的粒子占大多数,粒子以爱根核模态和积聚模态为主,平均数量中位径CMD(count medium diameter)为85.89 nm.而在灰霾消退过程,颗粒物数浓度降低,峰值粒径向小粒径演变,粒径在100 nm附近的粒子逐渐减少,核模态粒子增多,大于积聚模态,平均CMD为58.64 nm.气象因素中能见度和风力与数浓度主要呈负相关,相关系数R分别为-0.225和-0.229,相对湿度与数浓度正相关,相关系数R为0.271,冬季大气比较稳定,水平温度与数浓度的相关性较小.研究灰霾天气数浓度分布和气象因素的综合影响对其形成机制及控制有重要意义.  相似文献   

13.
Particles from ambient air and combustion sources including vehicle emission, coal combustion and biomass burning were collected and chemically pretreated with the purpose of obtaining isolated BC (black carbon) samples. TEM (transmission electron microscopy) results indicate that BC from combustion sources shows various patterns, and airborne BC appears spherical and about 50 nm in diameter with a homogeneous surface and turbostratic structure. The BET (Barrett–Emmett–Teller) results suggest that the surface areas of these BC particles fall in the range of 3–23 m2/g, with a total pore volume of 0.03–0.05 cm3/g and a mean pore diameter of 7–53 nm. The nitrogen adsorption–desorption isotherms are indicative of the accumulation mode and uniform pore size. O2-TPO (temperature programmed oxidation) profiles suggest that the airborne BC oxidation could be classified as the oxidation of amorphous carbon, which falls in the range of 406–490°C with peaks at 418, 423 and 475°C, respectively. Generally, the BC characteristics and source analysis suggest that airborne BC most likely comes from diesel vehicle emission at this site.  相似文献   

14.
Highly active mesoporous TiO_2 of about 6 nm crystal size and 280.7 m~2/g specific surface areas has been successfully synthesized via controlled hydrolysis of titanium butoxide at acidic medium. It was characterized by means of XRD(X-ray diffraction), SEM(scanning electron microscopy), TEM(transmission electron microscopy), FT-IR(Fourier transform infrared spectroscopy), TGA(thermogravimetric analysis), DSC(differential scanning calorimetry) and BET(Brunauer–Emmett–Teller) surface area. The degradation of dichlorophenol-indophenol(DCPIP) under ultraviolet(UV) light was studied to evaluate the photocatalytic activity of samples. The effects of different parameters and kinetics were investigated. Accordingly, a complete degradation of DCPIP dye was achieved by applying the optimal operational conditions of 1 g/L of catalyst, 10 mg/L of DCPIP, pH of 3 and the temperature at 25 ± 3°C after 3 min under UV irradiation. Meanwhile, the Langmuir–Hinshelwood kinetic model described the variations in pure photocatalytic branch in consistent with a first order power law model.The results proved that the prepared TiO_2 nanoparticle has a photocatalytic activity significantly better than Degussa P-25.  相似文献   

15.
This study focuses on the effects of pH and fluoride at different molar ratios of fluoride to Al (RF:Al) on the removal of cadmium (Cd2+) and phosphate by Al coagulation. Fluoride at RF:Al ≥ 3:1 inhibits the removal of Cd over wide Al dose ranges from 5 to 10 mg/L as Al. The removal of phosphate decreases significantly at high RF:Al of 10:1 whereas at lowered RF:Al (i.e., ≤ 6:1), an adverse effect is observed only at insufficient Al doses below 2 mg/L. Fluoride shows inhibitive effects towards the removal of Cd at pH 7 and 8 and that of phosphate at pH 6. Fluoride decreases the ζ-potential in both systems, and the decreasing extent is positively correlated to the elevated RF:Al. The Al fluoride interactions include the formation of Al–F complexes and the adsorption of fluoride onto Al(OH)3 precipitates, i.e., the formation of Al(OH)nFm. Al–F complex formation inhibits Al hydrolysis and increases residual Al levels, and a more significant increase was observed at lower pH. Al–F complexes at high RF:Al complicate the coagulation behavior of Al towards both negative and positive ionic species. Moreover, fluoride at low RF:Al shows little effect on Al coagulation behavior towards Cd2 + and phosphate, and the spent defluoridation adsorbent, i.e., aluminum (Al) hydro(oxide) with adsorbed fluoride at RF:Al of below 0.1:1, may be reclaimed as a coagulant after being dissolved.  相似文献   

16.
Impacts of nutrient management on C mineralization and greenhouse gas (GHGs) emission from soils have been of much concern in global change. Using laboratory incubation, the production of CH4 and CO2 were studied from both bulk samples and the particle size fractions (PSF) of topsoil from a paddy under a long-term different fertilization trial (including non (NF), chemical without (CF) and with manure (CFM) fertilization, respectively) in the Tai Lake Region, China. Four PSFs (2000–200, 200–20, 20–2, <2 μm) were separated from undisturbed samples collected after rice harvest by a low-energy ultrasonic dispersion procedure. Both the bulk samples and PSFs were incubated under submerged condition for 72 days. The concentration of CH4 and CO2 evolved during incubation were determined by gas chromatography. C mineralization rates ranged from 0.13 to 0.52 mg C g−1 C day−1, with different fertilizations and size of the PSFs, and were not correlated with C/N ratio. While CO2 production predominated over CH4 from C mineralization from both bulk samples and the size fractions, CH4 production played a predominant role in the total global warming potential (GWP) under all treatments. C mineralization of bulk soil was significantly higher under CF than under CFM and NF. CH4 production, however, was 3 times as under CFM and 27 times as under NF, indicating a tremendous effect of chemical fertilization alone on the total GWP. CO2 production from the PSFs differed from CH4 under a single treatment, which was notably from the coarse PSFs larger than 200 μm. Higher C mineralization and CH4 production with a higher metabolic quotient under CF implicated a vulnerability of soil functioning of GHGs mitigation in the paddy receiving chemical fertilizers only. Thus, rational organic amendments should be undertaken for mitigating the climate change.  相似文献   

17.
Numerous different bioreactor systems are applied for hydrogen production by dark fermentation. Thermophilic fermentations are gaining an increased interest due to the high hydrogen yields associated with them. In order to reach the best thermophilic fermentation system, 2 types of bioreactors, a trickling bed and a fluidized bed system, were constructed and operated under similar conditions. Both systems were designed to meet the requirements of thermophilic fermentations, such as reduction of hydrogen partial pressure, system immanence as its best as well as increasing cell densities. For comparing the 2 systems, the extreme thermophilic organism Caldicellulosiruptor owensensis OLT and a glucose-containing medium were employed. Parameters like hydraulic retention time, glucose concentration and stripping gas amount were varied. Each bioreactor system exhibited certain advantages; the trickling bed system enabled yields close to 3 mol-H2 (mol-glucose)?1 and productivities of 0.2 L L?1 h?1, but the application of stripping gas seemed to be obligatory. The fermentations in the fluidized bed system were characterized by slightly higher productivities (0.25 L L?1 h?1), but generally lower yields. However, operation of this system without stripping gas was possible.  相似文献   

18.
Nano-Al13 was separated and purified by four methods to investigate its characteristic, and was analyzed by Al-Ferron timed complexation spectrophotometer,27 Al-NMR (nuclear magnetic resonance), and transmission electron microscopy (TEM). Coagulation efficiency of nano-Al13, polyaluminum chloride (PAC), and AlCl3 in synthetic water were also investigated by jar test. The dynamic process and aggregation state of kaolin suspensions coagulating with nano-Al13, PAC, and AlCl3 were also investigated. The experimental results indicated that the efficiency of gel column chromatography method was the highest for separating PAC solution with low Al concentration. Ethanol and acetone method was simple and could separated PAC solution with different Al concentrations, while silicon alkylation white block column chromatography method could separate PAC solution only with low Al concentration. The SO42−/Ba2+ displacement method could separate PAC solution with high Al concentration, but extra inorganic cation and anion could be introduced into the solution during the separation. The coagulation efficiency and dynamic experimental results showed that nano- Al13 with a high positive-charged species was the main species of electric neutralization in coagulation process, and it could reduce the turbidity and increase the effective particles collision rate efficiently in coagulation process. Its coagulation speed and the particle size of coagulant formed were of greatest value in this study.  相似文献   

19.
Basic-oxygen furnace slag(BOF-slag) contains 35%CaO,a potential component for CO_2sequestration.In this study,slag-water-CO_2 reaction experiments were conducted with the longest reaction duration extending to 96 hr under high CO_2 pressures of 100-300 kg/cm2 to optimize BOF-slag carbonation conditions,to address carbonation mechanisms,and to evaluate the extents of V and Cr release from slag carbonation.The slag carbonation degree generally reached the maximum values after 24 hr slag-water-CO_2 reaction and was controlled by slag particle size and reaction temperature.The maximum carbonation degree of 71%was produced from the experiment using fine slag of0.5 mm under 100℃and a CO_2 pressure of 250 kg/cm~2 with a water/slag ratio of 5.Vanadium release from the slag to water was significantly enhanced(generally 2 orders) by slag carbonation.In contrast,slag carbonation did not promote chromium release until the reaction duration exceeded 24 hr.However,the water chromium content was generally at least an order lower than the vanadium concentration,which decreased when the reaction duration exceeded 24 hr.Therefore,long reaction durations of 48-96 hr are proposed to reduce environmental impacts while keeping high carbonation degrees.Mineral textures and water compositions indicated that Mg-wustite,in addition to CaO-containing minerals,can also be carbonated.Consequently,the conventional expression that only considered carbonation of the CaO-containing minerals undervalued the CO_2 sequestration capability of the BOF-slag by~20%.Therefore,the BOF-slag is a better CO_2 storage medium than that previously recognized.  相似文献   

20.
刘创创  王逸  周丽华  江峰  袁勇 《环境科学学报》2021,41(10):3956-3968
锆基纳米材料具有很好的物理化学稳定性及较高的比表面积,适用于解决传统过渡金属基催化剂活化过硫酸盐时金属浸出等问题.本研究将氯化锆-尿素络合物通过热解法合成了一种氮掺杂碳/氧化锆复合材料(N-C/ZrO2),用于活化过硫酸盐降解水中苯酚,并采用SEM、XRD、XPS和FTIR技术对N-C/ZrO2进行表征.结果表明,N-C/ZrO2催化材料是直径小于50 nm的纳米颗粒,且氮掺杂量为3.6%~4.9%;在pH=6~7的硼酸缓冲体系中,N-C/ZrO2催化过硫酸盐可在30 min内使水中苯酚(20 mg·L-1)的降解率达99%,且催化剂具有良好的化学稳定性和可重复利用性.淬灭和电子顺磁共振(EPR)结果表明,在N-C/ZrO2/PMS体系中,苯酚的降解是以1O2为主要氧化物质的非自由基氧化过程.本研究为Zr基纳米材料在活化过硫酸盐降解污染物领域的应用提供了理论基础.  相似文献   

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