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221.
《环境科学学报(英文版)》2023,35(4):423-433
Decomposition of the polycation Al13O4(OH)24(H2O)127+ (Al13) promoted by ligand is a vital subject to advance our understanding of natural and artificial occurrence and evolution of aluminum ions, especially in the case of acidic condition that dissolved Al3+ species can be released from the Al-bearing substances. However, the microscopic pathway of synchronous proton-promoted and ligand-promoted decomposition process for Al13 is still in the status of ambiguity. Herein, we applied differential mass spectrometry method and DFT calculation to study the initial detailed process of Al13 decomposition under the presence of proton and salicylic acid (H2Sal). Mass results showed that the mononuclear Al3+-H2Sal complexes dominated the resulting Al species, whereas the monodentate complex Al13HSal6+ was not observed in the spectra. The difference of decomposition levels between the ligand/Al ratio 0.2 and 0.5 cases revealed that proton and ligand performed synergistic effect in initial Al13 decomposition process, and the proton transfer determined the ring closure efficiency. The ring closure reaction is the prerequisite for the collapse of Al13 structure and detachment of the mononuclear complex. DFT calculations reveal that hydrogen bond plays an important role in inducing the formation of chelated complex accompanying proton transfer. Attachment of protons at the bridging OH− can elongate and weaken the critical bond between targeted Al3+ and µ4-O2- resulting from delocalization of electron pairs in the oxygen atom. These results demonstrate the detailed mechanism of Al13 composition promoted by ligand and proton, and provide significant understanding for further application and control of Al13. 相似文献
222.
浑河-大辽河水系水体与沉积物中典型全氟化合物的污染水平及生态风险评价 总被引:2,自引:0,他引:2
采用超高效液相色谱串联质谱(UPLC-ESI-MS/MS)分析了水体和沉积物中全氟化合物(PFCs)浓度水平,结果表明,浑河-大辽河的干流水中,PFCs总浓度范围为1.80~13.0 ng·L-1,其中,PFHx A、PFHp A、PFOA、PFOS和PFDA是主要污染物;沈阳细河中PFCs的总浓度为27.0~50.0 ng·L-1,其主要污染物为PFPA、PFOA、PFOS和PFDA.在浑河-大辽河沉积物中,PFHx A是唯一的检出物,其含量为0.130~0.490 ng·g-1干重;除了PFHx A,PFOS也是细河中的主要污染物,其浓度水平分别为0.070~0.220 ng·g-1和0.180~0.830 ng·g-1干重.采用实测的水和沉积物中PFOA和PFOS的暴露浓度以及预测的无效应浓度(PNEC),运用商值法对浑河-大辽河干流及沈阳细河水体和沉积物中PFOA和PFOS的生态风险进行评价.结果表明水体和沉积物中PFOA和PFOS的浓度均未达到对生态环境具有风险的水平. 相似文献
223.
养猪废水和污泥中11种兽用抗生素的同时分析技术及其在生物降解过程的应用 总被引:7,自引:2,他引:5
优化了固相萃取与高效液相色谱串联质谱联用的分析条件,使之适用于检测长三角地区养猪废水和污泥中常见的11种兽用抗生素(包括4种四环素类、2种磺胺类、3种喹诺酮类和2种大环内酯类).该分析方法对养猪废水的平均加标回收率(n=3)为73.0%~105.2%,相对标准偏差为3.1%~10.2%;对污泥的平均加标回收率(n=3)为57.4%~104.6%,相对标准偏差为1.9%~10.9%.研究膜生物反应器中抗生素的浓度变化,发现废水中抗生素以四环素类和磺胺类为主,而污泥中以四环素类为主.反应器对废水中四环素类抗生素的去除率为85.2%,其中最主要的去除途径是生物分解(51.9%),其次是污泥吸附(33.2%);而磺胺类抗生素去除率为95.8%,几乎全部是依靠生物分解,污泥吸附很少.摇瓶实验结果显示,污泥中积累的抗生素未对活性污泥的有机物降解活性和硝化活性产生明显影响. 相似文献
224.
高分辨率气相色谱/高分辨率质谱同位素内标法测定烟气样品中的多氯萘 总被引:1,自引:0,他引:1
多氯萘(PCNs)同二噁英(PCDD/Fs)和类二噁英多氯联苯(PCBs)类似,在烟气中的含量处于痕量水平,一般都在pg·m-3以下,因此分析方法要求有较高的灵敏度和选择性.以国内外的研究方法和参考文献为基础,建立了同位素内标稀释高分辨气相色谱/高分辨率质谱联用对垃圾焚烧发电厂的烟气样品中的PCNs进行分析.结果表明,该方法对17种氯取代位的PCNs单体的空白干扰在N.D.—2.1 pg之间;方法检出限范围为2.8—9.1 pg·nm-3,线性范围为0.40—240 pg·μL-1;空白加标实验中目标化合物的回收率为84.62%—116.21%,提取内标回收率为40.41%—75.79%,采样内标的回收率为88.92%—89.89%.实际烟气样品测得17种PCNs的同系物浓度分布在8.79—509 pg·nm-3之间,PCN-6的含量最高,PCNs-31S含量最低,相对标准偏差在4.43%—14.44%.该分析方法具有较高的准确性和可靠性,适用于烟气样品中多氯萘物质的测定. 相似文献
225.
In order to search the degradability of kraft lignin, the potential bacterial strains Bacillus subtilis (GU193980) and Klebsiella pneumoniae (GU193981) were isolated, screened and applied in axenic and co-culture conditions. Results revealed that mixed culture showed better decolorization efficiency (80%) and reduction of pollution parameters (COD 73% and BOD 62%) than axenic culture. This indicated syntrophic growth of these two bacteria rather than any antagonistic effect. The HPLC analysis of degraded samples of kraft lignin has shown the reduction in peak area compared to control, suggesting that decrease in color intensity might be largely attributed to the degradation of lignin by isolated bacteria. Further, the GC–MS analysis showed that most of the compounds detected in control were diminished after bacterial treatment. Further, the seed germination test using Phaseolus aureus has supported the detoxification of bacterial decolorized kraft lignin for environmental safety. All these observations have revealed that the developed bacterial co-culture was capable for the effective degradation and decolorization of lignin containing rayon grade pulp mill wastewater for environmental safety. 相似文献
226.
Experimental and geochemical modelling studies were carried out to identify mineral and solid phases containing major, minor, and trace elements and the mechanism of the retention of these elements in Flue Gas Desulphurisation (FGD)-gypsum samples from a coal-fired power plant under filtered water recirculation to the scrubber and forced oxidation conditions. The role of the pH and related environmental factors on the mobility of Li, Ni, Zn, As, Se, Mo, and U from FGD-gypsums for a comprehensive assessment of element leaching behaviour were also carried out. Results show that the extraction rate of the studied elements generally increases with decreasing the pH value of the FGD-gypsum leachates. The increase of the mobility of elements such as U, Se, and As in the FGD-gypsum entails the modification of their aqueous speciation in the leachates; UO2SO4, H2Se, and HAsO2 are the aqueous complexes with the highest activities under acidic conditions. The speciation of Zn, Li, and Ni is not affected in spite of pH changes; these elements occur as free cations and associated to SO42 in the FGD-gypsum leachates. The mobility of Cu and Mo decreases by decreasing the pH of the FGD-gypsum leachates, which might be associated to the precipitation of CuSe2 and MoSe2, respectively. Time-of-Flight mass spectrometry of the solid phase combined with geochemical modelling of the aqueous phase has proved useful in understanding the mobility and geochemical behaviour of elements and their partitioning into FGD-gypsum samples. 相似文献
227.
Experimental and geochemical modelling studies were carried out to identify mineral and solid phases containing major, minor, and trace elements and the mechanism of the retention of these elements in Flue Gas Desulphurisation (FGD)-gypsum samples from a coal-fired power plant under filtered water recirculation to the scrubber and forced oxidation conditions. The role of the pH and related environmental factors on the mobility of Li, Ni, Zn, As, Se, Mo, and U from FGD-gypsums for a comprehensive assessment of element leaching behaviour were also carried out. Results show that the extraction rate of the studied elements generally increases with decreasing the pH value of the FGD-gypsum leachates. The increase of the mobility of elements such as U, Se, and As in the FGD-gypsum entails the modification of their aqueous speciation in the leachates; UO2SO4, H2Se, and HAsO2 are the aqueous complexes with the highest activities under acidic conditions. The speciation of Zn, Li, and Ni is not affected in spite of pH changes; these elements occur as free cations and associated to SO4 2 in the FGD-gypsum leachates. The mobility of Cu and Mo decreases by decreasing the pH of the FGD-gypsum leachates, which might be associated to the precipitation of CuSe2 and MoSe2, respectively. Time-of-Flight mass spectrometry of the solid phase combined with geochemical modelling of the aqueous phase has proved useful in understanding the mobility and geochemical behaviour of elements and their partitioning into FGD-gypsum samples. 相似文献
228.
建立了微波消解土壤、石墨炉原子吸收法测定土壤中痕量铋的方法。采用磷酸二氢铵作为基体改进剂,热解涂层石墨管,塞曼扣背景。此方法对测定土壤中铋的灵敏度、准确度都有很大的提高。方法的最低检出浓度为0.02μg/g,加标回收率为94.5%~103.8%,能够满足环境监测分析的要求。 相似文献
229.
230.