Fe-MnOx-CeO2/ZrO2低温催化还原NO性能研究

以纳米ZrO2为载体,用浸渍法制备出Fe-MnOx-CeO2/ZrO2催化剂,考察了活性组分配比和助剂负载量对催化剂低温NH3选择性催化还原NO活性的影响,并对催化剂进行了XRD、SEM、EDS和BET表征;探讨了温度、H2O和SO2对Fe-MnOx-CeO2/ZrO2催化剂低温下NH3选择性催化还原NO的影响,结果表明,无SO2和H2O条件下,8%Fe-10%MnOx-CeO2/ZrO2催化剂具有良好的催化活性和稳定性.120℃时,催化剂的脱硝效率为85.23%,当温度升至180℃时,脱硝效率可达到92.0%.SO2和H2O共存条件下,催化剂易失活,采用傅立叶变换红外光谱对各反应阶段的催化剂进行了表征,对其失活机制进行深入研究,结果表明,催化剂失活的主要原因是催化剂表面硫酸铵盐的沉积和催化剂本身活性成分的硫酸盐化.     

双季稻田CH4和N2 O排放特征及品种筛选研究

通过大田小区实验,采用静止箱-气相色谱法对早晚两季水稻品种CH4与N2O排放通量进行了观测.结果表明,早稻CH4排放季节变化呈单峰模式,N2O排放呈双峰模式;晚稻CH4与N2O排放季节变化均呈单峰模式.CH4、N2O季节平均排放通量品种间均存在显著差异(P<0.05).早稻品种CH4、N2O季节平均排放通量极差分别为0.58 mg.(m2.h)-1、5.89μg.(m2.h)-1,晚稻为4.06 mg.(m2.h)-1、5.70μg.(m2.h)-1;早稻品种温室气体排放的增温潜势、单位产量增温潜势极差分别为2.92 kg.hm-2、0.097 kg.kg-1,晚稻分别为2 256 kg.hm-2、0.28 kg.kg-1.增温潜势、单位产量增温潜势比较,常规稻>超级杂交稻>杂交稻.早稻无水稻种植区CH4、N2O季节排放通量分别是水稻种植区的27.1%～31.8%、33.6%～88.3%;晚稻分别是23.8%～28.8%、38.6%～45.3%.早稻适宜种植品种为陆两优819、金优402、湘早籼24号,晚稻品种为岳优9113、湘晚籼12号.     

华北平原玉米-小麦轮作农田N2O交换通量的研究

以华北地区冬小麦-夏玉米轮作农田为研究对象,运用静态箱法对正常施肥及正常施肥结合秸秆还田农田N2O交换通量进行了连续1 a对比研究.正常施肥及正常施肥结合秸秆还田样地N2O全年的累积排放量分别为7.61 kg.hm-2和12.6kg.hm-2,其中秸秆还田引起N2O排放明显增加主要发生在玉米生长季节.两种处理样地在玉米季N2O的排放量占全年累积排放的57%～86%,表明华北玉米-小麦轮作体系中N2O排放主要集中在玉米季.各次施肥后10 d内N2O的累积排放量约占全年总排放量的71%～88%,显然现有化肥极大促进了华北农田N2O排放.     

多层填料生物转鼓去除NO废气的效能比较研究

生物转鼓过滤器能有效去除一氧化氮(NO)废气,为进一步提高生物转鼓过滤器的去除效能,实验改变了生物转鼓的填料结构,并与单层填料的生物转鼓进行了比较研究.结果表明,多层填料生物转鼓比单层填料生物转鼓更能有效去除NO,运行也更加稳定.8个月的连续运行实验表明,多层填料生物转鼓对NO去除率稳定在53.9％ ～93.4％之间,平均去除效率79.8％,而单层填料生物转鼓的平均去除率仅有68.7％;在相同实验条件下,空床停留时间(EBRT)可从单层填料生物转鼓的86.4 s降至多层填料生物转鼓的57.6 s.多层填料生物转鼓的最优工艺条件为,营养液量为1.3～3L,转速为0.75 r·min-1,在以葡萄糖为碳源时,TOC＞ 1250 mg·L-1后,去除效率增长幅度趋于平缓.     

乙醇处理对树脂基纳米水合氧化铁结构及其除砷性能的影响

通过考察乙醇处理对树脂基纳米水合氧化铁(D201-HFO)结构及其除砷性能的影响,评价乙醇处理在复合材料制备中的必要性.结果表明,乙醇处理后负载水合氧化铁(HFO)在D201树脂内的分散性增加,材料对砷的饱和吸附量提高约20%,且复合材料的比表面积、孔容、孔径分别增加了52%、65%、28%;但乙醇处理对复合材料的机械强度和负载HFO的晶型无影响,在pH值、离子竞争对该材料除砷性能的影响趋势方面也无明显作用,对复合材料固定床除砷性能及再生方面也无明显作用.总体而言,乙醇处理对D201-HFO复合材料实际除砷性能影响不大,从技术经济性考虑可以省略.     

Effect of ammonium on nitrous oxide emission during denitrification with different electron donors

Nitrous oxide(N2O) emission during denitrification is receiving intensive attention due to its high potential to cause greenhouse effects.In this study,denitrifiers were acclimated in sequencing batch reactors with methanol or acetate as the electron donor and nitrate as the electron acceptor.The effects of ammonium on N2O emission were examined in batch experiments with various electron donors.With the addition of ammonium,N2O emission increased under all the examined conditions compared to experiments without ammonium addition.With different electron donors,the highest ratio of N2O emission to the removed oxidized nitrogen was 0.70% for methanol,5.34% for acetate,and 34.79% for polyhydroxybutyrate.     

FeⅡ(EDTA)络合协同RDB去除NO废气效能及过程分析

为进一步提高一氧化氮(NO)的去除效率,在新型生物转鼓反应器(rotating drum biofilter,RDB)中,以FeⅡ(EDTA)络合协同RDB生物转鼓的耦合技术强化难水溶性NO的气液传质速率,提高生物还原效能为目标进行了研究.结果表明,适量FeⅡ(EDTA)被添加到RDB底部营养液后,能迅速吸收气相中的NO并生成FeⅡ(EDTA)-NO络合物,进而可通过反硝化实现同步脱氮和络合剂再生.在转速0.5 r.min-1、空床停留时间(EBRT)57.7 s、温度30℃、pH 7～8的实验条件下,RDB的净化效能随络合剂的投加而显著改善;FeⅡ(EDTA)质量浓度从0增至500 mg.L-1后,NO去除率从61.1%提高到97.6%,去除负荷从16.2 g.(m3.h)-1上升到26.7 g.(m3.h)-1.分析了FeⅡ(EDTA)络合协同净化NO的反应过程,建立了NO净化效率与FeⅡ(EDTA)添加浓度的关联方程,可较好地拟合实验数据.     

胶州湾及邻近海域表层海水中一氧化氮浓度分布及其影响因素探讨

2011年2～3月利用化学发光法对胶州湾及邻近海域表层海水中一氧化氮(NO)浓度进行了监测.结合水文、化学和生物等要素的同步观测资料,对该海域NO浓度分布及其影响因素进行了探讨.结果表明,胶州湾内表层海水中NO浓度为0.080～0.493 nmol.L-1,平均值为(0.292±0.146)nmol.L-1,胶州湾外NO浓度为未检出～0.435 nmol.L-1,平均值为(0.160±0.130)nmol.L-1.总体来说,胶州湾表层海水中NO浓度呈现出自湾内向湾外递降的分布趋势,陆地径流和人为活动可能对NO浓度的分布造成一定程度的影响.胶州湾及邻近海域表层海水中NO浓度比开阔大洋高1个数量级.周日变化研究表明,NO浓度具有一定的变化特征,最大值出现在15:00,这可能主要受光照的影响.影响NO浓度分布的因素比较复杂,可能主要受亚硝酸盐、光强和pH等因素的影响.结果表明,2011年春季胶州湾及邻近海域表层海水是大气NO的源,通量约为1.09×10-15 mol.(cm2.s)-1.     

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.     

Kinetics of selective catalytic reduction of NO by NH3 on Fe-Mo/ZSM-5 catalyst

The catalyst of Fe-Mo/ZSM-5 has been found to be more active than Fe-ZSM-5 and Mo/ZSM-5 separately for selective catalytic reduction (SCR) of nitric oxide (NO) with NH3. The kinetics of the SCR reaction in the presence of O2 was studied in this work. The results show that the observed reaction orders were 0.74-0.99, 0.01-0.13, and 0 for NO, O2 and NH3, respectively, at 350-450℃. And the apparent activation energy of the SCR was 65 kJ/mol on the Fe-Mo/ZSM-5 catalyst. The SCR mechanism was also deduced. Adsorbed NO species can react directly with adsorbed ammonia species on the active sites to form N2 and H2O. Gaseous O2 might serve as a reoxidizing agent for the active sites that have undergone reduction in the SCR process. It is also important to note that a certain amount of NO was decomposed directly over the Fe-Mo/ZSM-5 catalyst in the absence of NH3.