Advanced oxidation of bromide-containing drinking water：A balance between bromate and trihalomethane formation control

Addition of H2O2 has been employed to repress bromate formation during ozonation of bromide-containing source water. However, the addition of H2O2 will change the oxidation pathways of organic compounds due to the generation of abundant hydroxyl radicals, which could affect the removal efficacy of trihalomethane precursors via the combination of ozone and biological activated carbon （O3-BAC）. In this study, we evaluated the effects of H2O2 addition on bromate formation and trihalomethane formation potential （THMFP） reduction during treatment of bromide-containing （97.6-129.1 μg/L） source water by the O3-BAC process. At an ozone dose of 4.2 mg/L, an H2O2/O3 （g/g） ratio of over 1.0 was required to maintain the bromate concentration below 10.0 μg/L, while a much lower H2O2/O3 ratio was sufficient for a lower ozone dose. An H2O2/O3 （g/g） ratio below 0.3 should be avoided since the bromate concentration will increase with increasing H2O2 dose below this ratio. However, the addition of H2O2 at an ozone dose of 3.2 mg/L and an H2O2/O3 ratio of 1.0 resulted in a 43% decrease in THMFP removal when compared with the O3-BAC process. The optimum H2O2/O3 （g/g） ratio for balancing bromate and trihalomethane control was about 0.7-1.0. Fractionation of organic materials showed that the addition of H2O2 decreased the removal efficacy of the hydrophilic matter fraction of DOC by ozonation and increased the reactivity of the hydrophobic fractions during formation of trihalomethane, which may be the two main reasons responsible for the decrease in THMFP reduction efficacy. Overall, this study clearly demonstrated that it is necessary to balance bromate reduction and THMFP control when adopting an H2O2 addition strategy.     

含溴水臭氧化过程阴离子对溴酸盐生成的影响

为研究常见无机阴离子对含溴水臭氧化过程溴酸盐(Br O-3)生成的影响,本研究通过小试分别考察了不同质量浓度氯离子(Cl-)、碳酸氢根离子(HCO-3)和硫酸根离子(SO2-4)对Br O-3生成的影响,并结合反应过程臭氧衰减、中间产物次溴酸/次溴酸根离子(HOBr/OBr-)生成及总溴浓度变化情况,进一步分析了这3种无机阴离子对Br O-3生成的影响机制.结果表明,以60 min为例,Cl-质量浓度为3~150 mg·L-1的水样Br O-3生成量相对于未投加Cl-条件降低了8.8%~25.7%;反应20min时,SO2-4质量浓度从0 mg·L-1增至30 mg·L-1时,Br O-3生成量减少了63.9%;而当HCO-3质量浓度由0 mg·L-1上升至30 mg·L-1时,Br O-3生成量增加了6.4倍,其质量浓度超过30 mg·L-1,继续投加HCO-3对Br O-3生成量的促进作用提高不大.研究表明,在相同的臭氧投加量和相同的反应时间下,投加Cl-和SO2-4均能抑制臭氧化过程Br O-3的生成,而投加HCO-3能极大地促进Br O-3的生成.     

改性颗粒活性炭对水中溴酸根的吸附特性研究

采用阳离子表面活性剂氯化十六烷基吡啶(CPC)改性颗粒活性炭以提高活性炭对溴酸根的吸附能力.通过小试研究了改性颗粒活性炭(GAC-CPC)对溴酸根的吸附特性,考察了BrO-3初始浓度、pH、共存阴离子等因素对吸附过程的影响.结果表明,CPC改性能显著提高GAC对BrO-3的吸附能力,吸附量随着初始浓度升高而增大;在碱性条件下GAC-CPC对BrO-3的吸附量减小;共存阴离子与BrO-3在GAC-CPC上存在竞争吸附,其影响顺序为:NO-3SO2-4PO3-4CO2-3.用准一级、准二级和颗粒内扩散动力学模型拟合GAC-CPC吸附BrO-3的动力学过程,结果表明,准二级动力学能更好的描述吸附过程,且孔扩散可能是改性GAC吸附BrO-3初始阶段的主要速率控制因素.用Langmuir和Freundlich等温吸附模型拟合不同温度下BrO-3的吸附平衡过程,结果表明,Langmuir等温吸附模型能很好的描述吸附平衡过程,GAC-CPC吸附BrO-3的过程是自发且放热的,温度升高不利于吸附.     

基于碳捕集的富氧燃煤烟气联合脱硫脱硝试验研究

富氧燃煤烟气压缩液化CO2的高压低温工况为NO氧化为易溶于水的NO2提供了十分有利的条件.基于小型高压吸收试验装置,采用配制的富氧燃煤模拟烟气,在高压常温下进行了NO、SO2、O2与H2O的吸收反应试验.根据反应前后的气液产物分析,测定了不同组分比例与不同压力下混合气体中NO与SO2的转化率.NO氧化与吸收试验表明,NO转化为HNO3的比率随压力升高而增加,在0.5 ～2 MPa之间增加很快,在2 ～3 MPa之间增速趋丁平缓,压力达3 MPa以上时,90％以上的NO均转化为稀硝酸,且初始NO浓度越高,NO的转化率越大.混合气体中同时存在5O2与NO的联合吸收试验发现,只有少量的NO转化成了NO3-,SO2向H2SO4的转化率随压力升高而增加,初始SO2浓度越大,转化率越高.分析表明,SO2与NO同时存在时SO2先行转化为SO3,NO充当了催化剂,但SO2转化为SO3的一次转化率小于35％,反应酸液产物的多次循环能使SO2的转化率达到90％以上.建议的工艺流程中需采用两座吸收反应塔顺序脱除SO2与NO并回收稀酸溶液,有望在富氧燃煤发电捕集CO2系统中降低脱硫脱硝成本,部分地弥补富氧燃烧机组发电成本的增加.     

室内模拟不同因子对岩溶作用与碳循环的影响

为分析岩溶作用及岩溶碳循环的影响因素,设计了6个不同的处理以进行模拟实验.结果表明H2SO4含量、水动力条件以及土壤厚度对岩溶作用及岩溶碳循环具有重要影响.具有相同土壤厚度的3个处理,其Ca2++Mg2+浓度与SO2-4浓度均表现为:B20-2B20-1B20-3,B50-2B50-1B50-3,说明H2SO4的输入导致了岩溶作用增强,并且下渗水水量增加对水化学性质产生了明显的稀释作用.在煤铁残渣输入量及水动力条件相同而土壤厚度不同的条件下,Ca2++Mg2+浓度与SO2-4浓度表现为:B50-1B20-1、B50-2B20-2、B50-3B20-3.这说明较厚的土壤更有利于岩溶作用的进行.另外,由于实验中H2CO3对碳酸盐岩的溶解量贡献较小,岩溶作用对CO2的净消耗量主要取决于H2SO4含量.但B50-2的SO2-4浓度最大,CO2的净消耗量却最高.这可能是由于煤铁残渣向土壤中输入了有机质或其它养分促进了土壤深部CO2的形成,并且B50-2上部较厚的土壤也导致了H2CO3对碳酸盐岩溶解量的贡献增加,因此B50-2的CO2净消耗量也比较高.     

SO2对Ag/Al2O3催化剂上CH3OH还原NO性能的影响

用溶胶-凝胶混合法制备了Ag负载量为5%的Ag/A1₂O₃催化剂.研究了富氧条件下,SO₂对CH₃OH在催化剂上还原NO性能的影响.结果表明,反应气不含SO₂和H₂O时,NO还原活性温度较低,有显著量N₂O生成,这被归因为反应过程中,部分氧化态Ag被还原为金属Ag.添加SO₂或同时添加SO₂和H_{2相似文献}   

吸收液对中空纤维膜接触器回收尿液中氨氮的影响

采用中空纤维膜接触器（Hollow Fiber Membrane Contactor, HFMC）回收尿液中的氨氮,系统研究了吸收液类型（H₃PO₄、H₂SO₄和HNO₃）对氨回收效能、水蒸气的跨膜通量和所获液体肥料的影响.结果表明,使用H₂SO₄作为吸收液时氨氮回收效能最优,其次是H₃PO₄和HNO₃.当采用H₂SO₄为吸收液时,氨氮回收率、氨跨膜通量和传质系数分别为84.49%±0.01%、22.92 g·m^-2·h^-1和2.37×10^-6 m·s^-1.HNO₃的挥发性使其从吸收液侧反向跨膜至料液侧,导致氨跨膜传质驱动力变小;此外,NH₃和HNO₃会在膜孔中反应并生成NH₄NO₃气溶胶,增加氨在膜孔中的传质阻力,导致氨氮的回收效能降低.对采用不同吸收液时膜两侧的水的活度差和理论水通量进行了计算,结果表明,随着氨氮的不断跨膜吸收,膜两侧的活度差和水通量逐渐增大,实验结束时水通量分别为7.44×10^-2 kg·m^-2·h^-1（H₃PO₄）、9.06×10^-2 kg·m^-2·h^-1（H₂SO₄）和2.00×10^-2 kg·m^-2·h^-1（HNO₃）.肥料组分分析表明,以H₂SO₄和HNO₃为吸收液可以获得仅含N素的单一液体肥料,以H₃PO₄作吸收液可获得N-P复合肥,（NH₄）₂HPO₄和NH₄H₂PO₄所占的比例分别为88.33%和11.67%.     

Addition of hydrogen peroxide for the simultaneous control of bromate and odor during advanced drinking water treatment using ozone

Complete removal of the characteristic septic/swampy odor from Huangpu River source water could only be achieved under an ozone dose as high as 4.0 mg/L in an ozone-biological activated carbon （O3- BAC） process, which would lead to the production of high concentrations of carcinogenic bromate due to the high bromide content. This study investigated the possibility of simultaneous control of bromate and the septic/swampy odor by adding H2O2 prior to the O3-BAC process for the treatment of Huangpu River water. H2O2 addition could reduce the bromate concentration effectively at an H2O2/O3 （g/g） ratio of 0.5 or higher. At the same time, the septic/swampy odor removal was enhanced by the addition of H2O2, although optimization of the H2O2/O3 ratio was required for each ozone dose. At an ozone dose of 2.0 mg/L, the odor was removed completely at an H2O2/O3 ratio of 0.5. The results indicated that H2O2 application at a suitable dose could enhance the removal of the septic/swampy odor while suppressing the formation of bromate during ozonation of Huangpu River source water.     

Simultaneous removal of CO2, NOx and SOx using single stage absorption column

Capturing flue gases often require multiple stages of scrubbing, increasing the capital and operating costs. So far, no attempt has been made to study the absorption characteristics of all the three gases (NO, SO₂ and CO₂) in a single stage absorption unit at alkaline pH conditions. We have attempted to capture all the three gases with a single wet scrubbing column. The absorption of all three gases with sodium carbonate solution promoted with oxidizers was investigated in a tall absorption column. The absorbance was found to be 100% for CO₂, 30% for NO and 95% for SO₂ respectively. The capture efficiency of sodium carbonate solution was increased by 40% for CO₂ loading, with the addition of oxidizer. Absorption kinetics and reaction pathways of all the three gases were discussed individually in detail.     

土霉素结晶母液酸化水解过程的研究

土霉素结晶母液是一类含高浓度有机物和氮的废水,反硝化电子供体相对不足,且含有多种生物抑制性物质.为了提高废水的可生化性、增加可利用反硝化电子供体的数量,利用厌氧污泥床对土霉素结晶母液进行了水解处理,并对反应的pH、COD、NH₄⁺、和SO₄^2--浓度等进行了考察.水解过程对COD的去除功能不强,在HRT1.5h～6.0h的条件下,COD去除率也仅从10%提高到16%.由于有机氮氨化和硫酸盐还原作用,酸化后废水的pH值增加.当HRT超过2h以后,SO₄^2-基本上都被还原成S^2-采用经过水解的废水进行批量实验,结果证明硝化速率和反硝化速率分别比未水解时提高90.9%和45.2%.     

Interactions of sulfuric acid with common atmospheric bases and organic acids: Thermodynamics and implications to new particle formation

Interactions of the three common atmospheric bases, dimethylamine ((CH₃)₂NH), methylamine (CH₃NH₂), ammonia (NH₃), all considered to be efficient stabilizers of binary clusters in the Earth's atmosphere, with H₂SO₄, the key atmospheric precursor, and 14 common atmospheric organic acids (COAs) (formic, acetic, oxalic, malonic, succinic, glutaric acid, adipic, benzoic, phenylacetic, pyruvic, maleic acid, malic, tartaric and pinonic acids) have been studied using the density functional theory (DFT) and composite high-accuracy G3MP2 method. The thermodynamic stability of mixed (COA)(H₂SO₄), (COA)(B1), (COA)(B2) and (COA)(B3) dimers and (COA)(H₂SO₄)(B1), (COA)(H₂SO₄)(B2) and (COA)(H₂SO₄)(B3) trimers, where B1, B2 and B3 refer to (CH₃)₂NH, CH₃NH₂ and NH₃, respectively, have been investigated and their impacts on the thermodynamic stability of clusters containing H₂SO₄ have been studied. Our investigation shows that interactions of H₂SO₄ with COA, (CH₃)₂NH, CH₃NH₂ and NH₃ lead to the formation of more stable mixed dimers and trimers than (H₂SO₄)₂ and (H₂SO₄)₂(base), respectively, and emphasize the importance of common organic species for early stages of atmospheric nucleation. We also show that although amines are generally confirmed to be more active than NH₃ as stabilizers of binary clusters, in some cases mixed trimers containing NH₃ are more stable thermodynamically than those containing CH₃NH₂. This study indicates an important role of COA, which coexist and interact with that H₂SO₄ and common atmospheric bases in the Earth atmosphere, in formation of stable pre-nucleation clusters and suggests that the impacts of COA on new particle formation (NPF) should be studied in further details.     

Influence of SO2 in incineration flue gas on the sequestration of CO2 by municipal solid waste incinerator fly ash

The influence of CO2 content and presence of SO2 on the sequestration of CO2 by municipal solid waste incinerator(MSWI) fly ash was studied by investigating the carbonation reaction of MSWI fly ash with different combinations of simulated flue gas.The reaction between fly ash and 100% CO2 was relatively fast;the uptake of CO2 reached 87g CO2/kg ash,and the sequestered CO2 could be entirely released at high temperatures.When CO2 content was reduced to 12%,the reaction rate decreased;the uptake fell to 41g CO2/kg ash,and 70.7% of the sequestered CO2 could be released.With 12% CO2 in the presence of SO2,the reaction rate significantly decreased;the uptake was just 17g CO2/kg ash,and only 52.9% of the sequestered CO2 could be released.SO2 in the simulated gas restricted the ability of fly ash to sequester CO2 because it blocked the pores of the ash.     

辽宁省2000~2030年机动车排放清单及情景分析

机动车排放已经成为城市地区大气污染的主要来源.基于COPERT模型和ArcGIS技术,建立了2000~2030年辽宁省机动车排放清单,分析6类污染物（CO、NMVOC、NO_x、PM₁₀、SO₂和CO₂）排放的总体趋势与空间演变特征,同时以2016年为基准年,基于情景分析法设置8类控制措施情景并评估不同控制措施对污染物的减排效果.结果表明2000~2016年,机动车的CO、NMVOC、NO_x和PM₁₀排放量呈现先增后降的趋势,SO₂排放量呈现波动变化,而CO₂排放量则呈现持续增长态势.轻型载客车和摩托车是CO和NMVOC排放的主要贡献车型,重型载客车和重型载货车是NO_x和PM₁₀的主要排放源,SO₂和CO₂则主要是由轻型载客车排放.辽宁省中部及南部机动车排放量明显高于辽东和辽西.从城市层面来看,排放主要集中在沈阳市和大连市.情景分析表明,实施更加严格的排放标准可以增强减排效果,且升级排放标准的时间越提前减排效果越好.综合情景将实现减排最大化,强化综合情景对CO、NMVOC、NO_x、PM₁₀、CO₂和SO₂的削减率达到了30.7%、14.3%、81.7%、29.4%、12.3%和12.1%.     

Formation of THMs and HANs during bromination of Microcystis aeruginosa

Bromine-contained disinfectants and biocides are widely used in swimming pools, recreational waters and cooling towers. The objective of this study was to evaluate the formation of thrihalomethanes (THMs) and haloacetonitriles (HANs) and their cytotoxicity in algae solutions during free bromine disinfection. Disinfection by-products formation potential experiments were conducted using model solutions containing 7 mg/L (as total organic carbon) Microcystis aeruginosa cells. Effects of free bromine dosage, pH and ammonia were investigated. The results showed that brominated disinfection by-products were the major products when free bromine was applied. The total THMs formed during bromination was much as that formed during chlorination, whereas HANs were elevated by using bromination instead of chlorination. Dibromoacetonitrice (C2H2NBr2 ) and bromoform (CHBr3 ) were the only detected species during free bromine disinfection. The production of C2H2NBr2 and CHBr 3 increased with disinfectant dosage but decreased with dosing ammonia. CHBr3 increased with the pH changing from 5 to 9. However, C2H2NBr2 achieved the highest production at neutral pH, which was due to a joint effect of variation in hydrolysis rate and free bromine reactivity. The hydrolysis of C2H2NBr2 was base-catalytic and nearly unaffected by disinfectant. Finally, estimation of cytotoxicity of the disinfected algae solutions showed that HANs formation was responsible for the majority of toxicity. Considering its highest toxicity among the measured disinfection by-products, the elevated C2H2NBr2 should be considered when using bromine-related algaecide.     

太原市“十四五”规划大气污染防治政策的CO2协同效益评估

为量化评估太原市“十四五”大气污染防治政策的减污降碳协同效益,使用京津冀温室气体-空气污染相互作用与协同模型（GAINS-JJJ）,模拟评估13项大气污染防治措施的减排潜力,CO₂的协同减排效益.2025年政策情景下一次PM_2.5、PM₁₀、SO₂、NO_x、VOCs和NH₃分别减排1.8（5%,相对于基准情景减排比例,下同）、2.5（2%）、3.7（16%）、20.0（27%）、13.6（15%）和0.0 kt（0%）,CO₂减排9.0 Mt（13%）,CH₄排放增加203.3 kt（相对于基准情景增加25%）.SO₂、NO_x与VOCs减排主要发生在电力、工业燃烧与溶剂使用部门,CO₂减排主要发生在工业燃烧部门,CH₄排放量增加是由于煤矿开采活动水平升高.限制“双高”行业的能源消耗,严禁新增产能以及可再生能源发电比例提升措施的CO₂协同减排效益最高.VOCs具有优异协同减碳效益.建议太原市进一步推进终端电气化政策,同时需加大提升电力行业清洁能源比重和可再生能源发电的消纳能力.     

Inhibition of photosynthesis and leaf conductance interactions induced by SO2, NO2 and SO2 + NO2

Effects of 2-h exposures to 0–1 μmol mol⁻¹ SO₂, NO₂ and (1:1) SO₂ + NO₂ on CO₂ uptake by standardized snap bean leaves were studied. Interactions resulting from pollutant-induced changes in leaf conductance were evaluated. Minimum exposure concentrations required to depress CO₂ exchange rates (CER) under the test conditions were:0.17 μmol mol⁻¹ SO₂, 0.38 μmol mol⁻¹ NO₂, and 0.08 μmol mol⁻¹ of each pollutant in the 1:1 mixture. Treatments with 1 μmol mol⁻¹ NO₂ reduced CER 10% without affecting leaf conductance. One μmol mol⁻¹ SO₂ depressed CER by 50%. Leaf conductances increased in SO₂-treated leaves showing 30% inhibition of CER. Greater inhibition led to subsequent stomatal closure. Inhibition caused by the individual pollutants (applied singly) was linear over the range of concentrations investigated. The dual-pollutant mixture produced a synergistic response that was most pronounced at the lower pollutant concentrations. The potentiated effect was correlated with marked stomatal closure.Experimental plants for this study were grown under low moisture stress conditions to enhance stomatal opening in the plant stock material and reduce (damp) the potential for further SO₂-induced stimulation of stomatal opening. The experiments were designed to obtain limiting data for the test conditions.     

Simultaneous removal of selected oxidized contaminants in groundwater using a continuously stirred hydrogen-based membrane biofilm reactor

A laboratory trial was conducted for evaluating the capability of a continuously stirred hydrogen-based membrane biofilm reactor to simultaneously reduce nitrate (NO3--N), sulfate (SO42-), bromate (BrO3-), hexavalent chromium (Cr(VI)) and para- chloronitrobenzene (p-CNB). The reactor contained two bundles of hollow fiber membranes functioning as an autotrophic biofilm carrier and hydrogen pipe as well. On the condition that hydrogen was supplied as electron donor and diffused into water through membrane pores, autohydrogenotrophic bacteria were capable of reducing contaminants to forms with lower toxicity. Reduction occurred within 1 day and removal fluxes for NO3--N, SO4-2 , BrO3-, Cr(VI), and p-CNB reached 0.641, 2.396, 0.008, 0.016 and 0.031 g/(day·m-2 ), respectively after 112 days of continuous operation. Except for the fact that sulfate was 37% removed under high surface loading, the other four contaminants were reduced by over 95%. The removal flux comparison between phases varying in surface loading and H2 pressure showed that decreasing surface loading or increasing H2 pressure would promote removal flux. Competition for electrons occurred among the five contaminants. Electron-equivalent flux analysis showed that the amount of utilized hydrogen was mainly controlled by NO3 -N and SO4-2 reduction, which accounted for over 99% of the electron flux altogether. It also indicated the electron acceptor order, showing that nitrate was the most prior electron acceptor while sulfate was the second of the five contaminants.     

Processes affecting concentrations of aerosol strong acidity at sites in eastern England

Concentrations of aerosol strong acidity and related species have been measured at sites in eastern England using a sampler in which ammonia is pre-separated by a denuder. High concentrations occurred at a coastal site and were associated with air advected over the North Sea. At inland sites, ammonia concentrations were higher and the aerosol was more substantially neutralized. Daytime concentrations of aerosol H⁺ exceeded those measured at night, despite higher daytime levels of ammonia, presumably due to more effective production of H₂SO₄ during daytime hours. Concentrations of acidic aerosols were within the range 0–178 neq m⁻³, well below those observed at many eastern North American sites with lower concentrations of ammonia.     

不同阴离子对水溶性磷酸盐稳定污染土壤中重金属的影响

在重金属污染土壤中加入磷酸盐是稳定重金属的有效方法.本研究的目的是探讨不同阴离子对水溶性磷酸盐稳定污染土壤铅、镉和锌的影响.在重金属复合污染土壤(全铅、镉和锌的含量分别为2337、21.4和391 mg·kg^-1)中按P:Pb=2:1 (mol:mol)加入磷酸二氢钙,之后按P:阴离子=3:1或3:2 (mol:mol)加入盐酸、氯化钠、硫酸、硫酸钠或氟化钠,并设置只加磷酸盐、不加其它试剂的对照,培养55 d,之后测定土壤性质.结果表明,与对照相比,HCl处理、2HCl处理、NaCl处理和2NaCl处理土壤DTPA-Pb含量下降比例依次为5.72%、9.29%、6.38%和8.80%(p<0.05),加入硫酸、硫酸钠的处理土壤DTPA-Pb含量与对照无显著差异(p>0.05),而加入氟化钠的处理升高4.70%(p<0.05).加入盐酸或氯化钠的处理土壤镉有效性显著高于对照(升高5.24%~12.8%)(p<0.05),其它处理对DTPA-Cd含量无显著影响(p>0.05).各处理对土壤DTPA-Zn含量和pH影响较小,但均引起土壤电导率明显升高.以上结果表明,氯离子可促进水溶性磷酸盐对土壤铅的稳定,但可促进镉有效性.氯磷酸铅的生成是加氯情况下磷酸盐稳定铅的重要机制.     

Vaporization reduction characteristics of aqueous ammonia solutions by the addition of ethylene glycol, glycerol and glycine to the CO2 absorption process

Aqueous ammonia (NH₃) solution can be used as an alternative absorption for the control of CO₂ emitted from flue gases due to its high absorption capacity, fast absorption rate and low corrosion problem. The emission of CO₂ from iron and steel plants requires much attention, as they are higher than those emitted from power plants at a single point source. In the present work, low concentration ammonia liquor, 9 wt.%, was used with various additives to obtain the kinetic properties using the blast furnace gas model. Although a solution with a high ammonia concentration enables high CO₂ absorption efficiency, ammonium ions are lost as ammonia vapor, resulting in reduced CO₂ absorption due to the lower concentration of the ammonia absorbent. To decrease the vaporization of ammonia, ethylene glycol, glycerol and glycine, which contain more than one hydroxyl radical, were chosen. The experiments were conducted at 313 K similar to the CO₂ absorption conditions for the blast furnace gas model.