负载镍锌氧体木质素基活性炭吸附磺胺噻唑

以碱木素为原料热解制备碱木素基活性炭（LAC）,在此基础上添加硝酸镍、硝酸锌等,用水热合成法成功制备出负载镍锌氧体的木质素基活性炭（NiZn-DO/LAC）.通过SEM、BET、XRD等仪器对木质素基活性炭性能结构进行表征,并研究其在水溶液中对于磺胺噻唑（ST）的吸附.结果表明,所制得的木质素基活性炭具有明显的三维多孔结构与稳定的晶体结构,其具备较大的比表面积（759.1m²/g）.在吸附ST的过程中,NiZn-DO/LAC表现出较好的吸附性能,最大吸附容量可达328.2mg/g,优于其他报道的吸附剂.在NaOH溶液中,ST易从活性炭材料中脱附,在循环利用4次后,解吸率仍可达79.43%.NiZn-DO/LAC对ST的吸附主要通过静电作用、π-π堆积作用、络合作用、氢键作用及疏水性作用的协同,从而使吸附性能得到很大提高.     

施加Fe3O4/桑树杆生物炭对土壤砷形态和水稻砷含量的影响

以桑树杆为生物炭原料,制备Fe₃ O₄/桑树杆生物炭(Fe-MBC).通过土壤培养试验,研究不同炭化温度下制备的Fe-MBC对土壤有效态As含量的钝化效果,筛选出钝化效果好的Fe-MBC-800(800℃下炭化制备)并对其进行表征.通过盆栽试验,研究Fe-MBC-800添加比例为1%~7%(质量分数)时,其对种植水稻后土壤pH值、土壤电导率(EC)、土壤As形态、水稻生物量和水稻总As含量的影响.结果表明:①Fe-MBC-800成功负载了Fe₃ O₄,其主要官能团有C=O双键、O-H键、C-O键和Fe-O键; Fe-MBC-800、MBC-800和Fe₃ O₄的比表面积分别为209.659、517.714和68.025 m² ·g^-1.②添加Fe-MBC-800可提高土壤pH值,降低土壤EC值,提高土壤残渣态As含量,降低土壤水溶态As含量和土壤有效态As含量; 土壤中添加7%的Fe-MBC-800后,水溶态As含量和土壤有效态As含量分别降低了81.6%和56.33%.③土壤中Fe-MBC-800的添加比例为5%~7%时,能促进水稻植株的生长,提高水稻生物量,使水稻植株As的累积降低了62.5%~68.75%.     

MON-3超声辅助化学电位法制备氧化石墨烯

目的得到关于氧化石墨烯制备的最佳工艺条件。方法以绿色四氧化二氮推进剂和石墨为原料,开展基于化学电位法和超声法制备氧化石墨烯的实验研究,结合对氧化石墨烯产物进行扫描电子显微镜(SEM)和X-射线衍射仪(XRD)表征。结果对于氧化石墨的制备,最佳初始ORP区间为1700～1800 mV。石墨与N2O4配料比为1︰10、低温预处理工艺H2O2用量为18 mL、KMnO4用量为1.5 g、氧化温度为30℃、氧化时间为120 min是最佳工艺条件。对于氧化石墨烯的制备,分散溶剂pH为11,分散功率为150 W,分散时间为40 min是超声分散的最佳工艺条件。结论采用该工艺条件制备氧化石墨烯,既有利于解决大批量报废硝基氧化剂的转化处理难题,也制备得到了氧化石墨烯这种高附加值的民用工业产品。     

以淀粉为模板多孔纳米氧化铈的制备及其催化性能研究

为获得多孔纳米CeO₂（氧化铈）,以淀粉为生物模板,以Ce（NO₃）₃·6H₂O为铈源,在温和条件下制备出海绵状的多孔纳米CeO₂,同时考察了焙烧温度、碱液、铈源投加量对样品形貌的影响.利用XRD（X射线衍射光谱）、SEM（扫描电镜）、N₂吸附-脱附等表征手段对合成的多孔纳米CeO₂进行物相组成、微观形貌及孔径大小分布的分析.通过湿式催化过氧化试验,探究其对腈纶废水中有机物COD_Cr的催化降解性能.结果表明:①所制备的多孔纳米CeO₂具有多孔结构,孔径分布范围为2~4 nm,孔容为0.225 cm3/g,BET比表面积为256.426 m2/g;②多孔纳米CeO₂的最佳制备条件为1 g淀粉溶解于20 mL水中,加入0.02 mol Ce（NO₃）₃·6H₂O,以5%的氨水调节前驱体混合液pH,以1℃/min升至400℃,焙烧4 h,得到海绵状的多孔纳米CeO₂.③以不同形貌的CeO₂作为湿式催化反应中的催化剂,催化降解腈纶废水中有机物,其中以制备的多孔纳米CeO₂催化性能最佳,COD_Cr去除率可达82.5%.研究显示,焙烧温度、碱液、铈源投加量均可影响样品的形貌,在湿式催化过氧化处理腈纶废水试验中,多孔纳米CeO₂能显著提高废水COD_Cr的去除率.      

Facile synthesis of graphitic carbon-nitride supported antimony-doped tin oxide nanocomposite and its application for the adsorption of volatile organic compounds

Antimony-doped tin oxide(ATO) nanoparticles with an average size of ～ 6 nm were prepared by co-precipitation and subsequent heat treatment. Graphitic carbon nitride(g-CN)/ATO hybrid nanocomposite was designed by the combination of thermally synthesized g-CN and ATO nanoparticles by ultrasonication. The materials were characterized using N2 adsorption/desorption(BET), X-ray diffraction(XRD), scanning electron microscopy(SEM), energy dispersive spectroscopy(EDS), transmission electron microscopy(TEM) and Fourier transform infrared spectroscopy(FTIR). A mixture of five volatile organic compounds(VOCs, chloroform, benzene, toluene, xylene and styrene) was used to compare the adsorption capacity of the samples. The adsorption capacity of ATO nanoparticles was improved by the addition of g-CN. Experimental data showed that, among the five VOCs,chloroform was the least adsorbed, regardless of the samples. The g-CN/ATO showed nearly three times greater adsorption capacity for the VOC mixture than pure ATO. The unchanged efficiency of VOC adsorption during cyclic use demonstrated the completely reversible adsorption and desorption behavior of the nanocomposite at room conditions. This economically and environmentally friendly material can be a practical solution for outdoor and indoor VOC removal.     

A novel graphene oxide-carbon nanotubes anchored α-FeOOH hybrid activated persulfate system for enhanced degradation of Orange II

Persulfate activation has been applied as one of the efficient advanced oxidation processes(AOPs) to remediate polluted environments. In this study, a novel α-FeOOH anchored by graphene oxide(GO)-carbon nanotubes(CNTs) aerogel(α-FeOOH@GCA) nanocomposite activated persulfate system(α-FeOOH@GCA + K_2S_2O_8) was applied for decolorization of Orange Ⅱ(OⅡ). The decolorization of OⅡ was remarkably enhanced to a level of ～ 99% in this system compared with that of pristine α-FeOOH(～ 44%) or GO-CNTs(～18%). The enhanced catalytic activity of α-FeOOH@GCA was due to the formation of a heterojunction byα-FeOOH and GO-CNTs as confirmed by the presence of Fe–O–C chemical bonds. The degradation intermediates of OⅡ were comprehensively identified. The proposed degradation pathway of OⅡ begins with the destruction of the conjugated structures of OⅡ by the dominant reactive oxygen species, surface-bound SO_4~(·-). The decolorization efficiency of OⅡ by the α-FeOOH@GCA activated persulfate system decreased from the first to third cycle of recycling. Ultraviolet(UV) irradiation or introduction of a small amount of Fe~(2+) could restore the activation of this system. The results show that the α-FeOOH@GCA persulfate activation system promises to be a highly efficient environmental remediation method for organic pollutants.     

TiO2复合催化剂弱光催化降解模拟海水中苯酚及其催化活性的影响

为了获得适用于海水中有机污染物光降解催化剂,分别选用纳米SiO_2粒子和氧化石墨烯GO为载体,利用吸附相反应技术并结合热处理过程制备了基于TiO_2的复合催化剂,研究了弱光(光强小于1mW·cm~(-3))激发下复合催化剂光催化降解模拟海水中苯酚.结果表明,吸附相反应技术结合焙烧得到的La~(3+)掺杂TiO_2-SiO_2,表面亲水性较强和对苯酚吸附能力较弱,难以克服盐离子的干扰并有效降解模拟海水中高浓度苯酚.而吸附相反应技术结合醇溶剂热还原处理后,La~(3+)掺杂TiO_2-SiO_2催化剂表面亲水性显著减弱,但该催化剂在模拟海水中不能形成稳定的悬浮体系.吸附相反应技术得到的TiO_2-GO和La~(3+)掺杂TiO_2-GO中,TiO_2粒子粒径小于10nm且均匀负载于GO的表面.醇溶剂热还原处理可使TiO_2形成晶型结构,从而提高其催化活性,同时还能将GO表面的含氧基团还原,降低催化剂表面亲水性.从而提升催化剂对苯酚的吸附能力和对盐离子的抗干扰能力.另外,还原GO与小粒径TiO_2粒子紧密结合,使光生电子能很快转移至还原GO表面,增大光生电荷分离率,进一步提升催化剂的光降解性能.     

Bioaccumulation and effects of sediment-associated gold- and graphene oxide nanoparticles on Tubifex tubifex

With the development of nanotechnology,gold(Au) and graphene oxide(GO) nanoparticles have been widely used in various fields,resulting in an increased release of these particles into the environment.The released nanoparticles may eventually accumulate in sediment,causing possible ecotoxicological effects to benthic invertebrates.However,the impact of Au-NPs and GO-NPs on the cosmopolitan oligochaete,Tubifex tubifex,in sediment exposure is not known.Mortality,behavioral impact(GO-NP and Au-NP) and uptake(only Au-NP) of sediment-associated Au-NPs(4.9±0.14 nm) and GO-NPs(116±0.05 nm) to T.tubifex were assessed in a number of 5-day exposure experiments.The results showed that the applied Au-NP concentrations(10 and 60 μg Au/g dry weight sediment) had no adverse effect on T.tubifex survival,while Au bioaccumulation increased with exposure concentration.In the case of GO-NPs,no mortality of T.tubifex was observed at a concentration range of 20 and180 μg GO/g dry weight sediment,whereas burrowing activity was significantly reduced at 20 and 180 μg GO/g dry weight sediment.Our results suggest that Au-NPs at 60 μg Au/g or GO-NPs at 20 and 180 μg GO/g were detected by T.tubifex as toxicants during short-term exposures.     

Dissolved nitrous oxide and emission relating to denitrification across the Poyang Lake aquatic continuum

Most aquatic ecosystems contribute elevated N_2 O to atmosphere due to increasing anthropogenic nitrogen loading. To further understand the spatial heterogeneity along an aquatic continuum from the upriver to wetland to lake to downriver, the study was conducted on spatial variations in N_2 O emission along Poyang Lake aquatic continuum during the flood season from 15 July 2013 to 10 August 2013. The results showed the N_2 O concentrations, the ratio of N_2O/dinitrogen(N_2) gases production, N_2 O emission and denitrification rates ranged from 0.10 to 1.11 μg N/L,- 0.007% to 0.051%,- 9.73 to 127 μg N/m2/hr and 1.33 × 104to31.9 × 104μg N_2/m2/hr, respectively, across the continuum. The average N_2 O concentrations,the ratio of N_2O/N_2 and N_2O emission was significantly lower in wetlands as compared to the rivers and lake(p 0.01). The significantly high denitrification rate and low N_2 O emission together highlighted that most N_2 O can be converted into N_2 via near complete denitrification in the Poyang Lake wetlands. Our study suggests that the wetlands might impact N_2 O budget in an integrated aquatic ecosystems. Moreover, N_2 O emission from different aquatic ecosystem should be considered separately when quantifying the regional budget in aquatic ecosystem.     

铁锰双金属材料在不同pH条件下对土壤As和重金属的稳定化作用

pH是影响土壤As和重金属赋存形态及稳定化过程的重要因素,本文以人工合成的铁锰双金属材料(FMBO)为研究对象,研究了其在不同pH条件下对3种As和重金属复合污染土壤的稳定化作用,同时探讨了材料添加对土壤pH和酸碱缓冲性的影响.结果表明,As、Pb元素分别在土壤pH 3~9的中性偏酸性条件、pH 5~10的中性偏碱性条件下较为稳定,Cd、Zn、Cu在pH为7~11的碱性条件下浸出浓度较低.在碱性条件下,FMBO材料自身稳定性及稳定化作用均优于酸性条件,在As和重金属稳定的最适pH范围内,随着材料添加量增加,稳定化效率逐渐升高,其对As、Pb、Cd、Zn、Cu的稳定化效率最高分别能达到92.7%、100%、97.0%、88.7%、82.7%.添加FMBO材料可使土壤pH值升高,并能够提高土壤的酸缓冲能力,对As和重金属的长期稳定性有促进作用,而对土壤碱缓冲作用影响较小.从浸出元素的相关关系可以看出,Fe元素对土壤中As的稳定性有重要作用,Pb、Cd、Zn、Cu的稳定性受土壤pH影响较大.