等离子体与光催化耦合净化空气污染物研究现状

综合探讨了低温等离子体与光催化耦合这一新兴技术净化空气污染物的机理,讨论了影响耦合净化功能的主要因素以及臭氧的去除方法,介绍了该技术在去除挥发性有机物、氮氧化物、除菌等方面的研究现状,提出了其今后的研究方向。     

脉冲电晕低温等离子体提高一氧化氮氧化效率的实验研究

提高一氧化氮（NO）的氧化效率对于提高生物法处理该类废气的净化效率具有重要意义。实验研究了低温等离子体在脉冲电晕条件下氧化废气中NO的过程,考察了不同峰值电压、氧气含量、气体停留时间和添加有机物等因素对提高NO氧化效率的影响。结果表明：低温等离子法可有效地提高NO的氧化效率,主要产物为NO₂;室温条件下,当进气NO浓度590 mg/m³、脉冲频率50 Hz时,增大峰值电压、气体停留时间和进气中的氧气含量可提高NO的氧化效率;在最适峰值电压15 kV,气体停留时间5 s时,NO氧化效率为20%;在进气NO中添加甲苯、乙醇后,NO氧化效率可增加至30%以上,甲苯的效果要好于乙醇。     

Steam reforming of glycerol for syngas generation under cold plasma conditions: A DFT study

Density functional theory (DFT) has been used to investigate the reaction pathways with steam reforming of glycerol under cold plasma conditions. Total energies, energy barriers, and reaction enthalpies at 298.15 K have been calculated at the GGA/PW91/DNP level. The calculation shows that, with the presence of steam, the energy barrier of glycerol conversion is reduced and the conversion from glycerol to H₂ and CO is promoted under cold plasma conditions. The formation of syngas was through a multi-step pathway via the conversion of OHCH₂CHOH, CH₂OH, CH₂O, HCO,·and CH₃, while the recombination of H generated extra H₂. The synthesis of hydrocarbons are from the recombination of·CH₃,·CH₂, and·CH, which could be primarily generated through glycerol dissociation. The structure of glycerol anion was also studied in this work, and it was less stable than the neutral molecule. The route for the formation of OHCH₂CHOH·and CH₂OH·from glycerol anion is thermodynamically favorable.     

氨基化有机-无机杂化整体柱分离富集环境水中五价砷

将四乙氧基硅烷(TEOS)和N-(β-氨乙基)-γ-氨丙基三乙氧基硅烷(AEAPTES)作为共聚前体,采用在毛细管内原位聚合的方式制备得到氨基功能化的有机-无机杂化整体柱,将其作为针式固相微萃取(SPME)介质,建立了现场分离富集环境水中As(V)的SPME方法,优化了有机-无机杂化整体柱富集As(V)的实验条件,并研究了整体柱对As(V)的吸附/洗脱性能和富集能力,实现了环境水样中As(V)的高效、快速、高选择性检测。     

高效液相色谱-电感耦合等离子体质谱法测水中不同形态砷

采用高效液相色谱(HPLC)分离水中两种常见的砷形态As(III)、As(V),电感耦合等离子体质谱系统进行检测鉴定,利用C8色谱柱,探讨了甲醇含量、磷酸二氢钾浓度、四丁基氢氧化铵浓度、p H等测试条件,由此建立了水中砷形态的分析方法。结果表明,以1.5 mmol/L磷酸二氢钾、2 mmol/L四丁基氢氧化铵(TBAOH)、5%甲醇作为流动相,调节流动相为p H 5.5,流速为1.4 m L/min,上述两种不同形态的砷可在5.5 min内得以有效分离,As(III)、As(V)检出限分别为0.001、0.01μg/L,定量下限分别为0.005、0.03μg/L。该方法实现了对水中常见的不同形态砷(As(III)、As(V))的同时分析,具有灵敏度高、选择性好、检测速度快的特点,在水质分析领域具有重要意义与应用价值。     

负载型颗粒活性炭催化过硫酸钠氧化降解橙黄G

通过在颗粒活性炭(GAC)上负载氧化铁,并以此作为催化剂(Fe/GAC)在常温常压下催化过硫酸钠(PS)产生硫酸根自由基降解偶氮染料橙黄G.研究了体系pH、氧化剂浓度、催化剂浓度对橙黄G去除率的影响,并且对催化剂的重复使用性能进行了测试.结果表明,在Fe/GAC/PS体系中,[OG]0=0.2 mmol/L,[GAC] =1 g/L,[PS]0=2 mmol/L,降解2h后OG去除率为99％,且有较高的矿化率;随着氧化剂浓度和催化剂浓度的增加,OG的去除效率提高;催化剂有较好的重复使用性.利用扫描电镜(SEM)对催化剂进行了表征,可以看出在活性炭上成功负载氧化铁.利用化学分子探针竞争实验鉴定催化反应中的活性物种SO4-·和OH·.     

Using multivariate regression modeling for sampling and predicting chemical characteristics of mixed waste in old landfills

Municipal solid waste landfills pose a threat on environment and human health, especially old landfills which lack facilities for collection and treatment of landfill gas and leachate. Consequently, missing information about emission flows prevent site-specific environmental risk assessments. To overcome this gap, the combination of waste sampling and analysis with statistical modeling is one option for estimating present and future emission potentials. Optimizing the tradeoff between investigation costs and reliable results requires knowledge about both: the number of samples to be taken and variables to be analyzed.This article aims to identify the optimized number of waste samples and variables in order to predict a larger set of variables. Therefore, we introduce a multivariate linear regression model and tested the applicability by usage of two case studies. Landfill A was used to set up and calibrate the model based on 50 waste samples and twelve variables. The calibrated model was applied to Landfill B including 36 waste samples and twelve variables with four predictor variables.The case study results are twofold: first, the reliable and accurate prediction of the twelve variables can be achieved with the knowledge of four predictor variables (Loi, EC, pH and Cl). For the second Landfill B, only ten full measurements would be needed for a reliable prediction of most response variables. The four predictor variables would exhibit comparably low analytical costs in comparison to the full set of measurements. This cost reduction could be used to increase the number of samples yielding an improved understanding of the spatial waste heterogeneity in landfills.Concluding, the future application of the developed model potentially improves the reliability of predicted emission potentials. The model could become a standard screening tool for old landfills if its applicability and reliability would be tested in additional case studies.     

镍基催化剂对污泥微波热解制生物气效能的影响

为实现污水污泥减量化、无害化及资源化的目标,在微波热解污水污泥基础上,进行了镍基催化剂对制取生物气效能影响的研究。采用元素分析对污泥元素进行检测,气/质联用分析(GC-MS)和气相色谱(GC)对热解生物气的组成和含量进行测定。实验结果表明,镍基催化剂的添加对微波热解污水污泥制取生物气有较大促进作用。5%添加量与800℃热解终温条件下具有最佳催化效果:生物气中H2、CO产量最大,H2产量由29 g/kg增加到35.8 g/kg,提升23.4%,CO产量由302.7 g/kg增加到383.3 g/kg,提升26.6%;同时催化剂还能提高热能利用效率,降低热解终温,即5%添加量在700℃热解终温时可达到空白800℃时的产气效果;镍基催化剂主要在500~600℃时发挥催化作用,加快了H2和CO的释放。微波热解污泥制取的生物气具有产量大、富含H2与CO等优点,可推动污水污泥的资源化进程。     

反应气耦合等离子体降解沙林模拟剂

采用水蒸气、氨气、过氧化氢气雾和臭氧4种气体对沙林模拟剂氟磷酸二异丙酯(DFP)进行降解研究,发现臭氧对DFP具有较好的降解作用,在流量200 L/h,DFP初始浓度50 mg/m3时,降解率最高可达56.1%。对高浓度DFP(大于80 mg/m3)进行降解研究时,等离子体单独作用最高降解率为89%,而添加臭氧后的降解率都在95%以上。计算得到臭氧作用的能量利用率为0.05 mg/(W·h),等离子体的能量利用率为0.55 mg/(W·h),而添加臭氧后的等离子体能量利用率为0.68 mg/(W·h)明显高于臭氧和等离子体能量利用率之和,因此对高浓度DFP进行处理时,臭氧与等离子体存在耦合作用。对等离子体和臭氧耦合等离子体降解DFP反应进行了产物分析,发现主要的降解产物基本一致,但是臭氧的存在能使降解更加彻底。     

辉光放电等离子体氧化降解水中邻苯二甲酸二丁酯

研究了辉光放电等离子体降解水中典型的环境内分泌干扰物邻苯二甲酸二丁酯(DBP)及降解过程中过氧化氢(H2O2)的生成规律。考察了电解质种类、共存污染物(甲醇、叔丁醇)及催化剂等条件对DBP降解及H2O2生成的影响。结果表明,在硫酸钠溶液中DBP降解效率和H2O2生成速率最高;甲醇、叔丁醇等共存污染物对DBP降解和H2O2生成有抑制作用;Fe2+,Fe3+和Cu2+对DBP的降解有催化作用,其催化效果为Fe2+>Fe3+>Cu2+。用高效液相色谱、离子色谱及气质联用仪等仪器分析了降解中间产物,提出了可能的降解机理。