基于稳定碳同位素技术的干旱区绿洲土壤有机碳向无机碳的转移

应用稳定碳同位素技术测定土壤无机碳稳定碳同位素组成(soil inorganic carbonδ13C,SICδ13C),并对干旱区绿洲土壤无机碳进行区分,结合土壤有机碳(soil organic carbon,SOC)与SIC含量关系进一步探讨SOC向SIC转移的碳量.结果表明,4种类型土壤SICδ13C值差异性极显著(P0.01),风沙土SICδ13C值最高且为正,均值为(0.32±0.04)‰,随土层深度增加而增加,说明风沙土原生性碳酸盐占绝对优势;灌漠土、棕漠土和盐碱土SIC的δ13C均值分别(-0.30±0.24)‰、(-1.96±0.66)‰和(-1.24±0.49)‰,随土层变化均呈先降低后逐渐增大的趋势,说明灌漠土原生性碳酸盐占优势,棕漠土和盐碱土发生性碳酸盐相对前者占优势.风沙土、灌漠土、棕漠土和盐碱土的发生性碳酸盐占SIC比例均值分别为1.33%、4.72%、15.01%、35.71%,均小于50%,说明干旱区绿洲土壤发生性碳酸盐比例总体水平较低.风沙土、灌漠土、棕漠土和盐碱土在土壤发生性碳酸盐形成或重结晶过程中固定土壤CO2的量分别为0.30、2.44、4.96、12.40 g·kg~(-1),其中固定来自大气CO2量平均为0.18、0.79、1.45、8.67 g·kg~(-1),来自SOC氧化分解转化为CO2的量分别为0.06、0.83、1.62、1.86g·kg~(-1),说明盐碱土、棕漠土SOC的贡献相对较高,灌漠土、风沙土较低;对土壤固定CO2量的来源比较发现,风沙土、盐碱土固定土壤CO2的量来自大气CO2量较高,SOC的贡献较低,而灌漠土、棕漠土固定来自SOC氧化分解CO2的量较高,大气贡献较低.研究区整体SOC向SIC的碳转移量介于0.03~2.38 g·kg~(-1)之间,平均每千克土壤固定1.09 g的CO2,说明干旱区绿洲土壤发生性碳酸盐所占比例较低,SOC的贡献较少.     

塔里木盆地北缘绿洲不同连作年限棉田土壤有机碳、无机碳含量与环境因子的相关性

农田土壤碳库是土壤碳库的重要组成部分,易受人类活动调节且固碳减排潜力巨大,研究土壤有机碳、无机碳含量特征及其与环境因子的关系有助于深入理解土壤生态过程,为全球碳收支平衡研究提供理论支持.本文以塔里木盆地北缘绿洲为靶区,分析土壤碳库特征,结合冗余分析、通径分析,探究土壤有机碳、无机碳含量及其与环境因子的相关关系.结果表明:(1)同一土层不同连作年限棉田土壤有机碳、无机碳含量存在显著差异(P0.05),随连作年限增加,有机碳含量呈先增加后减少趋势,而无机碳含量呈先减少后增加趋势;同一连作年限棉田不同土层土壤有机碳、无机碳含量存在显著差异(P0.05),有机碳含量均在0~20 cm层达到最大值,而无机碳含量均在20~50 cm层达到最大值.(2)通过冗余分析得出环境因子对土壤碳库特征影响的重要性排序为:磷酸酶活性p H值蔗糖酶活性过氧化氢酶活性全氮速效磷速效钾土壤含水量脲酶活性电导率;磷酸酶活性、p H值、蔗糖酶活性、过氧化氢酶活性、全氮、速效磷、速效钾与土壤有机碳、无机碳含量呈极显著相关关系(P0.01);土壤含水量、脲酶活性与土壤有机碳、无机碳含量表现为显著相关(P0.05).(3)通径分析表明,速效钾对有机碳含量直接作用显著,是影响有机碳含量的主要因素,而脲酶活性对无机碳含量直接作用显著,是影响无机碳含量的主要因素.干旱半干旱区土壤有机碳、无机碳含量研究是评价农田生态系统土壤碳的"源/汇"效应的基础数据,对研究全球碳收支平衡和陆地碳循环机制具有重要意义.     

钙法解吸并固定乙醇胺富液中CO2

针对醇胺类吸收剂富液中CO_2的解吸及后续处置所存在的不足,提出一种新型解吸方案——钙法.通过CO_2负荷试验和Ca(OH)_2投加量试验确定了该法理想处理负荷为0.84 mol·L-1,理想投加比例为C∶Ca=1∶1(摩尔比),此条件下反应15 min和30 min的解吸率达到52.17%和55.02%,这表明钙法矿化解吸乙醇胺富液中CO_2是可行的.在此基础上,进一步研究了pH、温度和搅拌强度对CO_2解吸固定效果的影响.试验结果表明,CO_2解吸率随着pH和搅拌强度的增加而增大,但当pH和搅拌强度增大到一定程度后,解吸率增长放缓甚至出现下降.较高的解吸温度尽管解吸率更大,但高温条件下无法达到矿化固定CO_2的目的.CO_2二次吸收负荷试验表明经钙法解吸后的MEA再生液具有良好的可重复使用性.     

Simultaneous removal of ammonia and N-nitrosamine precursors from high ammonia water by zeolite and powdered activated carbon

When adding sufficient chlorine to achieve breakpoint chlorination to source water containing high concentration of ammonia during drinking water treatment, high concentrations of disinfection by-products(DBPs) may form. If N-nitrosamine precursors are present, highly toxic N-nitrosamines, primarily N-nitrosodimethylamine(NDMA), may also form. Removing their precursors before disinfection should be a more effective way to minimize these DBPs formation. In this study, zeolites and activated carbon were examined for ammonia and N-nitrosamine precursor removal when incorporated into drinking water treatment processes.The test results indicate that Mordenite zeolite can remove ammonia and five of seven N-nitrosamine precursors efficiently by single step adsorption test. The practical applicability was evaluated by simulation of typical drinking water treatment processes using six-gang stirring system. The Mordenite zeolite was applied at the steps of lime softening, alum coagulation, and alum coagulation with powdered activated carbon(PAC) sorption. While the lime softening process resulted in poor zeolite performance, alum coagulation did not impact ammonia and N-nitrosamine precursor removal. During alum coagulation, more than67% ammonia and 70%–100% N-nitrosamine precursors were removed by Mordenite zeolite(except 3-(dimethylaminomethyl)indole(DMAI) and 4-dimethylaminoantipyrine(DMAP)). PAC effectively removed DMAI and DMAP when added during alum coagulation. A combination of the zeolite and PAC selected efficiently removed ammonia and all tested seven N-nitrosamine precursors(dimethylamine(DMA), ethylmethylamine(EMA), diethylamine(DEA), dipropylamine(DPA), trimethylamine(TMA), DMAP, and DMAI) during the alum coagulation process.     

生物质基活性炭负载金属催化还原NOx

为研究生物质材料的脱硝性能,利用木质素与纤维素2种生物质基活性炭作为还原剂,用碱金属与过渡金属作为催化活性相,制备了一系列生物质基活性炭负载金属催化剂用于富氧环境中催化还原NO_x,考察了生物质原料种类、炭化温度以及催化剂组分对脱硝效率的影响.结果表明:①当反应温度低于250℃时,炭表面主要是NO_x的吸附过程;而当反应温度高于250℃时,炭还原NO_x行为占主导,并伴随N₂、CO₂与CO的生成.炭化温度对炭反应活性的影响主要依赖于炭化温度对炭材料表面含氧官能团、比表面积以及炭表面金属还原性的影响.②研究中考察的金属（K、Cu、Fe、Ni）均对还原NO_x与O₂有催化作用,其中,K对C-NO_x反应具有明显促进作用,但对C-O₂反应并无明显促进作用,所有样品中SAC-K的选择性因子为0.56,对还原NO_x的选择性最高,且恒温反应过程NO_x还原量（以C计）达到了1 293 μmol/g.③与传统煤基活性炭催化剂相比,木屑基活性炭负载钾催化剂表现出了优良的NO_x还原选择性;X-射线光电子表征结果显示,木屑基活性炭负载钾催化剂优良的性能与其表面钾活性相的高度分散有关.研究显示,相比于煤基炭材料,生物质基炭材料具有更加优异的选择性还原NO_x性能.      

天津市区夏季碳气溶胶特征及改进的二次有机碳估算方法

为更加准确地估算环境受体PM_2.5中SOC（二次有机碳）的质量浓度,于2015年6-8月利用在线监测仪器同步采集小时分辨率的PM_2.5及OC（有机碳）和EC（元素碳）样品数据,分析碳气溶胶的变化特征,并尝试运用改进的EC示踪法估算ρ（SOC）.结果表明:天津市区夏季ρ（PM_2.5）为（70.9±46.0）μg/m3,ρ（OC）和ρ（EC）分别为（7.6±3.1）（2.2±1.5）μg/m3,占ρ（PM_2.5）的11.8%±4.6%和3.1%±1.4%,OC/EC（质量浓度之比,下同）的平均值为4.0±2.0.ρ（OC）与ρ（EC）之间的Pearson相关系数（R）仅为0.66,说明OC和EC的来源较为复杂,SOC的产生可能是重要影响因素.ρ（NO₂）与OC/EC呈显著负相关（R=-0.47,P < 0.01）,并且OC/EC（4.0）相对较低,说明天津市区机动车可能对碳气溶胶具有重要影响.ρ（SO₂）与ρ（OC）、ρ（EC）的相关性较低（R均为0.33,P均小于0.01）,说明天津市区碳气溶胶可能受燃煤源的影响较低.改进的EC示踪法主要是利用O₃和CO、EC作为光化学反应和一次源排放的指标,并结合ρ（OC）、ρ（EC）和OC/EC的变化特征,逐步筛选一次排放源主导的时间段的ρ（OC）和ρ（EC）数据,然后利用最小二乘法拟合获得ρ（OC）和ρ（EC）的线性方程,最后进行ρ（SOC）和ρ（POC）（POC为一次有机碳）的估算.天津市区夏季ρ（SOC）的平均值为（2.5±2.0）μg/m3,分别占ρ（OC）和ρ（PM_2.5）的28.8%±15.0%和3.7%±3.6%;ρ（POC）的平均值为（5.2±1.7）μg/m3,分别占ρ（OC）和ρ（PM_2.5）的71.2%±15.0%和8.1%±5.2%,说明天津市区夏季有机碳的主要来源是一次排放源.研究显示,相比于EC示踪法,改进的EC示踪法估算的ρ（SOC）明显降低,ρ（POC）明显升高.AT（大气温度）对ρ（SOC）的影响较为显著,而WS（风速）对ρ（POC）的影响较为显著.      

Characterization particulate matter from several Chinese cooking dishes and implications in health effects

Cooking fume produced by oil and food at a high temperature releases large amount of fine particulate matter(PM) which have a potential hazard to human health. This chamber study investigated particle emission characteristics originated from using four types of oil(soybean oil, olive oil, peanut oil and lard) and different kinds of food materials(meat and vegetable). The corresponding emission factors(EFs) of number, mass, surface area and volume for particles were discussed. Temporal variation of size-fractionated particle concentration showed that olive oil produced the highest number PM concentration for the entire cooking process. Multiple path particle dosimetry(MPPD) model was performed to predict deposition in the human respiratory tract. Results showed that the pulmonary airway deposition fraction was the largest. It was also found that particles produced from olive oil led to the highest deposition. We strongly recommend minimizing the moisture content of ingredients before cooking and giving priority to the use of peanut oil instead of olive oil to reduce human exposure to PM.     

Insights into the formation of secondary organic carbon in the summertime in urban Shanghai

To investigate formation mechanisms of secondary organic carbon(SOC) in Eastern China,measurements were conducted in an urban site in Shanghai in the summer of 2015. A period of high O_3 concentrations(daily peak 120 ppb) was observed, during which daily maximum SOC concentrations exceeding 9.0 μg/(C·m~3). Diurnal variations of SOC concentration and SOC/organic carbon(OC) ratio exhibited both daytime and nighttime peaks. The SOC concentrations correlated well with O_x(= O_3+ NO_2) and relative humidity in the daytime and nighttime, respectively, suggesting that secondary organic aerosol formation in Shanghai is driven by both photochemical production and aqueous phase reactions. Single particle mass spectrometry was used to examine the formation pathways of SOC. Along with the daytime increase of SOC, the number fraction of elemental carbon(EC) particles coated with OC quickly increased from 38.1% to 61.9% in the size range of 250–2000 nm, which was likely due to gas-to-particle partitioning of photochemically generated semi-volatile organic compounds onto EC particles. In the nighttime, particles rich in OC components were highly hygroscopic, and number fraction of these particles correlated well with relative humidity and SOC/OC nocturnal peaks. Meanwhile, as an aqueous-phase SOC tracer, particles that contained oxalate-Fe(III) complex also peaked at night. These observations suggested that aqueous-phase processes had an important contribution to the SOC nighttime formation. The influence of aerosol acidity on SOC formation was studied by both bulk and single particle level measurements, suggesting that the aqueous-phase formation of SOC was enhanced by particle acidity.     

Behaviors and kinetics of toluene adsorption‐desorption on activated carbons with varying pore structure

This work was undertaken to investigate the behaviors and kinetics of toluene adsorption and desorption on activated carbons with varying pore structure. Five kinds of activated carbon from different raw materials were selected. Adsorption isotherms and breakthrough curves for toluene were measured. Langmuir and Freundlich equations were fitted to the equilibrium data, and the Freundlich equation was more suitable for simulating toluene adsorption. The process consisted of monolayer, multilayer and partial active site adsorption types. The effect of the pore structure of the activated carbons on toluene adsorption capacity was investigated. The quasi-first-order model was more suitable for describing the process than the quasi-second-order model. The adsorption data was also modeled by the internal particle diffusion model and it was found that the adsorption process could be divided into three stages. In the external surface adsorption process, the rate depended on the specific surface area. During the particle diffusion stage, pore structure and volume were the main factors affecting adsorption rate. In the final equilibrium stage, the rate was determined by the ratio of meso-and macro-pores to total pore volume. The rate over the whole adsorption process was dominated by the toluene concentration. The desorption behavior of toluene on activated carbons was investigated,and the process was divided into heat and mass transfer parts corresponding to emission and diffusion mechanisms, respectively. Physical adsorption played the main role during the adsorption process.     

Impact of density of coating agent on antibacterial activity of silver nanoparticle impregnated plasma treated activated carbon

To use stabilized nanoparticles(NPs) in water as disinfectants over a very long period, the amount of coating agent(for NP stabilization) needs to be optimized. To this end, silver nanoparticles(Ag-NPs) with two different coating densities of tri-sodium citrate(12.05 and46.17 molecules/nm~2, respectively), yet of very similar particle size(29 and 27 nm, respectively)were synthesized. Both sets of citrate capped NPs were then separately impregnated on plasma treated activated carbon(AC), with similar Ag loading of 0.8 and 0.82 wt.%, respectively. On passing contaminated water(containing 10~4 CFU Escherichia coli/m L of water) through a continuous flow-column packed with Ag/AC, zero cell concentration was achieved in 22 and 39 min, with Ag-NPs(impregnated on AC, named as Ag/AC) having lower and higher coating density, respectively. Therefore, even on ensuring similar Ag-NP size and loading, there is a significant difference in antibacterial performance based on citrate coating density in Ag/AC.This is observed in lower coating density case, due to both:(i) higher Ag~+ ion release from Ag-NP and(ii) stronger binding of individual Ag-NPs on AC. The latter ensures that, Ag-NP does not detach from the AC surface for a long duration. TGA-DSC shows that Ag-NPs with a low coating density bind to AC with 4.55 times higher adsorption energy, compared to Ag/AC with a high coating density, implying stronger binding. Therefore, coating density is an important parameter for achieving higher antibacterial efficacy, translating into a faster decontamination rate in experiments, over a long period of flow-column operation.