柱状V2O5/AC中V2O5的分布特征对烟气脱硫活性的影响

采用过量浸溃(XS)、等体积浸渍(PV)和半等体积浸渍(HPV)方法,分别制得3种柱状V2O5/AC催化剂,并对其脱硫能力进行评价.结果表明:尽管这3种方法制取的催化剂总w(V2O5)相同(均为0.5%),但V2O3在柱状颗粒中的分布差异却很大;其中半等体积浸渍法制备的催化剂外层w(V2O5)最高,等体积浸渍法的w(V2O5)居中,过量浸渍法的w(V2O5)最低.脱硫前期,催化剂外层的w(V2O5)对脱硫活性的影响很大,外层w(V2O5)高的催化剂脱硫活性较高;脱硫后期,催化剂外层w(V2O5)对脱硫活性的影响变小,而内层w(V2O5)的影响变大,内层w(V2O5)高的催化剂脱硫活性较高.     

三峡库区及其下游溶解氧化亚氮(N2O)分布和释放

氧化亚氮(N_2O)是一种重要温室气体,对全球变暖具有重要影响.河流和水库是释放N_2O的活跃区域,但是目前对于温带和亚热带水库及其下游河道释放N_2O的研究相对较少.分别于2009年9～10月和2016年10月对长江三峡水库及其下游干流进行了调查,对库区水体溶解N_2O的浓度分布、释放通量及其影响因素进行了研究,探讨了筑坝和水库运行对长江N_2O分布和释放的可能影响.结果表明秋季三峡库区表层(～0 m)、底层(6～103 m)水体溶解N_2O平均值为(12. 49±1. 75)nmol·L-1和(11. 21±0. 91) nmol·L-1.秋季库区水体N_2O浓度变化较小,和三峡坝下干流站位无显著差异(P 0. 05).三峡库区水体N_2O与氨氮(NH4+)、亚硝态氮(NO2-)呈显著负相关(P 0. 05; P 0. 01),与硝态氮(NO3-)呈正相关(P 0. 01). 2016年和2009年10月三峡水库表层N_2O均处于过饱和状态,饱和度范围分别为114%～187%和122%～170%,库区N_2O平均释放通量分别为(4. 6±2. 4)μmol·(m2·d)-1和(16. 6±4. 9)μmol·(m2·d)-1.两次调查中大坝下游N_2O平均释放通量(6. 0±7. 0)μmol·(m2·d)-1,虽然三峡库区水面释放N_2O通量低于全球水库的平均水平,但是三峡库区仍是大气N_2O不可忽视的源.大坝下泄水和发电未造成库区和大坝下游N_2O浓度出现显著差异.运行多年以来三峡库区已进入平稳期,2009年和2016年秋季N_2O浓度无明显变化.     

酸性条件下Ti（Ⅳ）催化O3/H2O2降解邻苯二甲酸二甲酯

研究了酸性条件下O3、O3/H2O2、Ti(Ⅳ)/O3和Ti(Ⅳ)/O3/H2O2氧化邻苯二甲酸二甲酯(DMP)的效能.结果表明,在初始pH为2.8条件下,Ti(Ⅳ)/O3/H2O2体系对DMP的降解效率,矿化程度和臭氧的利用率都明显优于其他3种氧化体系.相同条件下O3、O3/H2O2、Ti(Ⅳ)/O3和Ti(Ⅳ)/O3/H2O2降解DMP的一级表观速率常数分别为3.96×10-4s-1、9.54×10-4s-1、1.07×10-3s-1和6.41×10-3s-1.与单独臭氧化相比,Ti(Ⅳ)/O3/H2O2体系臭氧的利用率约可提升6.51%.优化实验表明,本实验条件下Ti(Ⅳ)的最佳浓度为1.4 mg·L-1,H2O2最佳投加量为10 mg·L-1.结合气质联用(GC/MS)与离子色谱(IC)的分析结果,对Ti(Ⅳ)/O3/H2O2降解DMP的可能反应途径进行了初步的解析.     

N2:O emissions from a cultivated Andisol after application of nitrogen fertilizers with or without nitrification inhibitor under soil moisture regime

IntroductionNitrousoxide (N2 O)isoneoftheenvironmentallyimportanttracegases ,currentlyaccountingfor 2 %—4 %oftotalGreenhouseWarmingPotential (GWP ) .Itisalsoinvolvedinthedepletionofstratosphericozone .SoilhasbeenknownasthemajorsourceofN2 O ,accountingfor 6 5 %oftotalglobalemissions(Prather,1995 ) .Thus,reducingN2 Oemissionsfromsoilsisamaintaskfortheprotectionoftheglobalatmosphere .N2 Oisproducedastheresultofsoilmicrobialprocesses ,primarillybynitrification ,whentheoxidationhappensofNH+…     

高盐高碱环境下硝化反硝化过程及N2O产生特征

采用稳定运行在高盐高碱环境厌氧/好氧/缺氧(A_n/O/A)模式下的序批式生物膜反应器(SBBR),考察在不同碳氮比(C/N)条件下,硝化反硝化过程及N_2O产生特征.结果表明,在C/N为5、2和对照组(C/N=0)时,总氮去除率分别为(98. 17±0. 42)%、(65. 78±2. 47)%和(44. 08±0. 27)%; N_2O的产生量分别为(32. 07±2. 03)、(21. 81±0. 85)和(17. 32±0. 95) mg·L~(-1); N_2O转化率(N_2O产生量在去除总氮中的比例)分别为(29. 75±0. 93)%、(30. 04±2. 17)%和(41. 69±0. 80)%.高盐高碱条件下,亚硝酸盐氧化菌(NOB)受到很强的抑制作用,硝化过程基本停留在亚硝酸盐阶段.由于高盐高碱环境对N_2O还原酶活性的抑制,使得异养反硝化过程产生了大量N_2O,随着碳氮比的增大,有更多的碳源用于反硝化过程,因而总氮去除率和N_2O产生量均随之增加.随着碳氮比的增大,N_2O转化率随之降低,这可能是由于异养反硝化过程氮素还原酶对电子的竞争所形成的,碳氮比越高,电子竞争越弱.高通量测序表明:在SBBR中,氨氧化细菌(AOB)被富集,而几乎不存在NOB;优势异养反硝化菌属主要是Thauera、Azoarcus和Gemmobacter.     

Catalytic performance of Fe3O4-CoO/Al2O3 catalyst in ozonation of 2-(2,4-dichlorophenoxy)propionic acid, nitrobenzene and oxalic acid in water

Fe3O4-CoO/Al2O3 catalyst was prepared by incipient wetness impregnation using Fe(NO3) 3·9H2O and Co(NO3) 2·6H2O as the precursors,and its catalytic performance was investigated in ozonation of 2-(2,4-dichlorophenoxy) propionic acid(2,4-DP) ,nitrobenzene and oxalic acid.The experimental results indicated that Fe3O4-CoO/Al2O3 catalyst enabled an interesting improvement of ozonation eciency during the degradation of each organic pollutant,and the Fe3O4-CoO/Al2O3 catalytic ozonation system followed a radical-type mechanism.The kinetics of ozonation alone and Fe3O4-CoO/Al2O3 catalytic ozonation of three organic pollutants in aqueous solution were discussed under the mere consideration of direct ozone reaction and OH radical reaction to well investigate its performance.In the catalytic ozonation of 2,4-DP,the apparent reaction rate constants(k) were determined to be 1.456×10-2 min-1 for ozonation alone and 4.740×10-2 min-1 for O3/Fe3O4-CoO/Al2O3.And O3/Fe3O4-CoO/Al2O3 had a larger Rct(6.614×10-9) calculated by the relative method than O3 did(1.800×10-9) ,showing O3/Fe3O4-CoO/Al2O3 generated more hydroxyl radical.Similar results were also obtained in the catalytic ozonation of nitrobenzene and oxalic acid.The above results demonstrated that the catalytic performance of Fe3O4-CoO/Al2O3 in ozonation of studied organic substance was universal to a certain degree.     

Cu2O光催化降解海水中苯酚的研究

利用水热法,以CuSO4和Na2SO3为原料,在HAc-NaAc缓冲溶液中制备出氧化亚铜(Cu2O)粉末.利用X射线粉末衍射仪(XRD)和扫描电镜(SEM)对产物进行表征.采用仿日光光源,研究了Cu2O光催化降解海水中苯酚的过程;探讨了Cl(-)对Cu2O光催化效率的影响以及机理.研究表明,Cu2O的光催化效率随溶液中...     

氮肥施用对紫色土-玉米根系系统N2O排放的影响

通过不同施氮水平与不同氮肥品种2个田间试验,结合静态箱-气相色谱法研究了川中丘陵区2005年5～9月石灰性紫色土-玉米根系系统的N2O排放变化.结果表明:1)施用氮肥显著地增加了N2O排放,在3个施氮水平下(0、150和250 kg·hm-2),N2O排放总量分别为0.88、2.19和2.52 kg·hm-2;施氮量越高,N2O排放量也越高.当施氮量超过一定水平后,施肥量高低对N2O排放总量的影响并不显著.由氮肥施用引起的N2O排放量占施氮量的0.87%(150 kg·hm-2)和0.66%(250 kg·hm-2).2)氮肥品种显著影响N2O排放,尿素(酰胺态氮肥)和硫酸铵(铵态氮肥)处理的N2O排放量分别为2.09和1.80 kg·hm-2,显著高于硝酸钾(硝态氮肥)处理(1.27 kg·hm-2),三者排放量分别占施氮量的0·80%、0.60%和0.27%.3)降雨是玉米生长季N2O排放的主要影响因子,而无机氮则是影响N2O排放的主要限制因子.     

O3/H2O2法降解甲基叔丁基醚（MTBE）的试验研究

采用自制鼓泡反应器对臭氧/双氧水(O3/H2O2)降解水中甲基叔丁基醚(MTBE)进行了试验研究,考察了进气(含O3)流量、H2O2 投加量、MTBE初始浓度、pH、温度等因素对MTBE降解的影响.结果表明,在MTBE初始浓度为10 mg·L-1,气体流量为0.5 L·min-1,温度293K, pH=6.5, H2O2 添加量为2.4mg·L1 条件下,反应30 min后, MTBE去除率可达75.5%, COD去除率为68.0%.降解得到的中间产物主要有叔丁基甲酯(TBF)、叔丁醇(TBA)、乙酸甲酯(MA)和丙酮(AC)等,据此探讨了O3/H2O2氧化MTBE的可能反应机理和降解途径.     

黄土高原苹果园土壤N_2O排放研究

从2007年5月1日到2009年4月30日对黄土高原苹果园氧化亚氮(N2O)排放采用静态箱气相色谱法进行了为期两年的监测.分别在距果树2.5m(D2.5)、1.5m(D1.5)、0.5m(D0.5)的位置采样.研究结果表明,苹果园N2O排放量年际变化较大,2008年5月到2009年4月的N2O排放量(2.74kg·hm-·2a-1)比2007年5月到2008年4月(2.27kg·hm-·2a-1)高20.7%,主要原因是2008年夏季降雨量是2007年夏季降雨量的1.92倍,使得2008年夏季N2O排放量是2007年夏季的2.81倍.2008年5月到2009年4月的排放系数(0.082%)是2007年5月到2008年4月排放系数(0.035%)的2.34倍.施肥后、冻融交替期、苹果树落叶的前期、降雨后苹果园都有高的N2O排放峰,N2O的季节变化受到这些短期事件的显著影响.而这些短期事件对N2O排放的激发效应又受到降雨量、土壤孔隙充水率(WFPS)和地温的调控.D2.5和D0.5两个处理的N2O排放与气温(p≤0.01)和地温(p≤0.01或p≤0.05)显著相关.D1.5处理N2O排放与气温(p≤0.05)显著相关.     

稻田土壤不同水分条件下硝化/反硝化作用及其功能微生物的变化特征

以湖南桃源县一长期种植水稻的酸性土壤为研究对象,在微宇宙培养条件下设置了4个水分梯度处理,分别为田间持水量(water holding capacity,WHC)的30%、60%、90%和淹水2 cm深.考察了水分条件变化对硝化和反硝化作用影响,并结合定量PCR和限制性末端片段长度多态性(T-RFLP)技术研究了硝化-反硝化微生物的响应特征.结果表明,30%WHC处理土壤无明显的硝化和反硝化作用发生,硝化作用主要发生于60%WHC和90%WHC处理土壤,90%WHC处理土壤硝化作用明显强于60%WHC,并检测到明显的N2O释放,表明该水分条件可能发生了硝化-反硝化耦合作用.淹水处理土壤氧化还原势Eh显著低于非淹水处理土壤,无明显的硝化作用发生,但能检测到N2O释放且释放量小于90%WHC处理土壤.除培养初期(7 d)外,反硝化功能基因nirS和nirK,以及氨氧化细菌(AOB)amoA基因的丰度先随着水分增加而增加,并在淹水处理中小幅下降,三者之间呈明显的正相关关系,且AOB amoA、nirS和nirK基因丰度均在90%WHC处理中最高,与该处理中硝化和反硝化活性最高相一致.T-RFLP结果表明,培养2周后,nirS基因为代表的反硝化微生物群落组成对水分梯度变化产生明显响应,Eh和含水率Cw是影响其群落组成的主要因子.     

除草剂对氮肥反硝化损失与N2O排放的影响

在华北平原潮土上,采用原状土柱培养乙炔抑制法研究玉米地氮肥反硝化损失和N2O排放量以及喷施3种除草剂(乙莠、丁莠和旱锄)的影响.结果表明,氮肥的反硝化损失量为2.66kgN/hm2,占施肥量的1.77%;氮肥产生的N2O排放量为3.14kgN/hm2,占施氮量的2.09%,反硝化不是该地区旱作系统氮肥损失的主要途径,但氮肥的施用大大增加N2O排放量.喷施除草剂显著或极显著降低氮肥的N2O排放量和反硝化损失量,比单施尿素处理分别降低2.01~2.85kgN/hm2和2.56~3.16kgN/hm2.     

Sources of nitrous and nitric oxides in paddy soils：Nitrification and denitrification

Rice-paddies are regarded as one of the main agricultural sources of N 2O and NO emissions. To date, however, specific N2O and NO production pathways are poorly understood in paddy soils. ^15N-tracing experiments were carded out to investigate the processes responsible for N2O and NO production in two paddy soils with substantially different soil properties. Laboratory incubation experiments were carried out under aerobic conditions at moisture contents corresponding to 60% of water holding capacity. The relative importance of nitrification and denitrification to the flux of NaO was quantified by periodically measuring and comparing the enrichments of the N2O, NH~-N and NO3-N pools. The results showed that both N2O and NO emission rates in an alkaline paddy soil with clayey texture were substantially higher than those in a neutral paddy soil with silty loamy texture. In accordance with most published results, the ammonium N pool was the main source of N2O emission across the soil profiles of the two paddy soils, being responsible for 59.7% to 97.7% of total N2O emissions. The NO3-N pool of N2O emission was relatively less important under the given aerobic conditions. The rates of N2O emission from nitrification （N2On） among different soil layers were significantly different, which could be attributed to both the differences in gross N nitrification rates and to the ratios of nitrified N emitted as NzO among soil layers. Furthermore, NO fluxes were positively correlated with the changes in gross nitrification rates and the ratios of NO/N2O in the two paddy soils were always greater than one （from 1.26 to 6.47）. We therefore deduce that, similar to N2O, nitrification was also the dominant source of NO in the tested paddy soils at water contents below 60% water holding capacity.     

Effect of fertilizer and water content on N2O emission from three plantation soils in South China

Introduction Nitrousoxide(N2O)isoneofthemostimportantgreen housegases,whichcontributestoglobalwarmingand consumptionofO3inthestratosphere(Breuer,2000,Solomon,1999).N2Oconcentrationincreasesatarateof0.25%peryear,57%ofwhichisderivedfromthesoildue tonitrific…     

放牧对草原十壤N2O产生及微生物的影响

利用AIM乙炔抑制法 ,首次测试了我国内蒙古放牧和非放牧羊草草原土壤N2 O产生的微生物过程 ;通过分析不同类型草原土壤N2 O产生的微生物过程和相关微生物菌群的季节变化 ,研究了放牧行为对于草原土壤N2 O微生物产生过程的影响 .放牧行为改变了土壤结构 ,有利于土壤微生物反硝化作用的发生 ,在一定程度上降低了草原土壤N2 O的排放 .揭示了内蒙古草原土壤N2 O产生是以异养硝化作用过程为主的微生物过程 ,解释了内蒙古典型草原土壤N2 O通量较低和其季节变化的微生物学机理     

亚洲地区稻田N2O排放影响因子统计模拟分析

关于稻田N2O排放大样本统计分析大多只涉及水分因子和肥料因子,本研究收集历年亚洲稻田N2O排放资料和更多影响因子(水分管理、肥料类型及用量、土壤属性、气候和水稻类型等)的相关信息,从中筛选出具有统计学意义的因子,构建排放通量和上述因子的统计模型.具有统计学意义的因子包括不同水分管理措施、肥料用量、不同有机肥类型、不同p...     

Effects of long-term amendment of organic manure and nitrogen fertilizer on nitrous oxide emission in a sandy loam soil

To understand the effects of long-term amendment of organic manure and N fertilizer on N2O emission in the North China Plain, a laboratory incubation at different temperatures and soil moistures were carried out using soils treated with organic manure （OM）, half organic manure plus half fertilizer N （HOM）, fertilizer NPK （NPK）, fertilizer NP （NP）, fertilizer NK （NK）, fertilizer PK （NK） and control （CK） since 1989. Cumulative N2O emission in OM soil during the 17 d incubation period was slightly higher than in NPK soil under optimum nitrification conditions （25℃ and 60% water-filled pore space, WFPS）, but more than twice under the optimum denitrification conditions （35℃ and 90% WFPS）. N2O produced by denitrification was 2.1-2.3 times greater than that by nitrification in OM and HOM soils, but only 1.5 times greater in NPK and NP soils. These results implied that the long-term amendment of organic manure could significantly increase the N2O emission via denitrification in OM soil as compared to NPK soil. This is quite different from field measurement between OM soil and NPK soil. Substantial inhibition of the formation of anaerobic environment for denitrification in field might result in no marked difference in N2O emission between OM and NPK soils. This is due in part to more rapid oxygen diffusion in coarse textured soils than consumption by aerobic microbes until WFPS was 75% and to low easily decomposed organic C of organic manure. This finding suggested that addition of organic manure in the tested sandy loam might be a good management option since it seldom caused a burst of N2O emission but sequestered atmospheric C and maintained efficiently applied N in soil.     

不同有机物料对土壤N2O排放的影响与调控

通过向土壤施加15N标记的莴笋残体(处理R)、废纸浆(处理P)及二者混合物(处理RP),并利用不同的压力使其成为3种不同容重处理的土壤样本,进行密闭培养,定时测定土壤N2O排放量及土壤溶液中NO3-与NH4 的动态变化,以探讨N_2O的产生与调控机制.结果表明,8d N2O释放量为R处理最大,RP处理其次,P处理最小.短期内(8d)R处理N2O释放最大量为空白对照(CK)的15倍,增加了土壤反硝化作用;P处理在同期内不能增加N2O释放量,证明这种废纸浆可少量(<2.5%)施用于农田中.RP与CK、P处理比较,可以刺激微生物活性和增加土壤反硝化作用;与R处理相比较,可以增加氮的固定.增加有机质的添加量使同一容重水平的RP处理N2O释放量高于R处理.70%的土壤样本随容重增加N2O释放量增加.土壤容重的增加同时影响了废纸浆的分解速率和土壤溶液中NO3-与NH4 浓度.     

黄绵土N2O排放的水分效应及动力学特征

通过室内模拟试验,研究湿度对西北地区黄绵土N2O排放的影响.结果表明:在试验温度下,随着土壤湿度增加,土壤N2O捧放量增加;但土壤孔隙含水量(WFPS)为20.67%时例外.此时黄绵土对空气中N2O有吸附现象,即在低含水量时,黄绵土有可能是N2O的汇.在试验设计的土壤湿度范围内,15℃条件下土壤N2O排放的最大水分效应区间在49.18%～57.86%(WFPS)之间,20℃条件下在38.14%～49.18%(WFPS)之间,25℃、30℃和35℃时累积量湿区在20.67%～38.14%(WFPS)之间,即随着温度的升高,N2O的最大水分效应区间提前.土壤N2O累积排放量(y)动力学曲线符合修正的Elovich方程(P<0.01),随着湿度的增加,表观排放速率(b)增大,25℃、300C和35℃时,N2O初始排放量(a)也随着湿度增加而增大;15℃、20℃和25℃时,土壤湿度(20.67%～57.86%WFPS)对农田土样N2O排放总量的作用表现为线性关系,30℃和35℃时表现为对数关系.