复合氧化物汽车尾气净化催化剂抗SO2中毒机理研究

复合氧化物催化剂(ASC)具有较高的活性和良好的抗SO_2中毒性能.用IR、XPS、TPD等技术研究了该催化剂抗SO_2中毒机理,结果表明,与易失活催化剂相比,ASC经500h反应(反应气含SO_2约20ppm),其活性组分价态无显著变化,仅表面发生SO_2的化学吸附,经与约500ppm的SO_2作用20h后,发现仅有少量SO_4~(2-)形成.这是由于在ASC催化剂中添加了特殊助剂,而使催化剂活性组分得到保护的缘故.     

Greenhouse impacts of anthropogenic CH4 and N2O emissions in Finland

The Finnish anthropogenic CH₄ emissions in 1990 are estimated to be about 250 Gg, with an uncertainty range extending from 160 to 440 Gg. The most important sources are landfills and animal husbandry. The N₂O emissions, which come mainly from agriculture and the nitric acid industry are about 20 Gg in 1990 (uncertainty range 10–30 Gg). The development of the emissions to the year 2010 is reviewed in two scenarios: the base and the reduction scenarios.According to the base scenario, the Finnish CH₄ emissions will decrease in the near future. Emissions from landfills, energy production, and transportation will decrease because of already decided and partly realized volume and technical changes in these sectors. The average reduction potential of 50%, as assumed in the reduction scenario, is considered achievable.N₂O emissions, on the other hand, are expected to increase as emissions from energy production and transportation will grow due to an increasing use of fluidized bed boilers and catalytic converters in cars. The average reduction potential of 50%, as assumed in the reduction scenario, is optimistic.Anthropogenic CH₄ and N₂O emissions presently cause about 30% of the direct radiative forcing due to Finnish anthropogenic greenhouse gas emissions. This share would be even larger if the indirect impacts of CH₄ were included. The contribution of CH₄ can be controlled due to its relatively short atmospheric lifetime and due to the existing emission reduction potential. Nitrous oxide has a long atmospheric lifetime and its emission control possiblities are limited consequently, the greenhouse impact of N₂O seems to be increasing even if the emissions were limited somehow.     

不同温湿度条件下微米硼的氧化过程研究

目的 探究不同温湿度条件下微米硼的氧化层结构特征。方法 利用高温水浴浸泡处理去除原料微米硼的表面氧化层,然后在恒温恒湿条件下对微米硼进行加速氧化,利用扫描电子显微镜、透射电子显微镜和X射线光电子能谱对加速氧化后硼颗粒的氧化层厚度及组成进行分析,总结表面氧化层结构及成分组成变化规律,揭示温湿度条件下微米硼的氧化机制。结果 微米硼经高温水浴浸泡处理后,表面氧化层去除率达到50%。随着加速氧化时间的延长,硼颗粒氧化层的厚度逐渐增大,由内向外硼颗粒表面可以用B-BxOy-B2O3三层结构来表示,BxOy总是伴随着B2O3同时出现的,且随着氧化反应的进行,颗粒表面BxOy的含量将超过B的含量。结论 不同温湿度条件下微米硼的氧化机制为O2向B颗粒内部单向扩散的反应机制,B先与O2反应,形成低氧化物BxOy,BxOy进而与O2反应生成B2O3。随着氧化层厚度的增加,O2向B颗粒内部扩散的阻力增大,氧化反应速率随之降低。相比湿度的影响,温度的升高可显著加快硼表面氧化层的形成;温度一定时,湿度的增加可促进硼氧化层的形成。     

天津市滨海河流N2O扩散通量及控制因子

河流是大气温室气体重要的排放源.为了探讨天津市典型景观滨海河流N₂O释放空间特征及影响因素,以天津市6条不同土地利用类型的滨海河流为研究对象,通过顶空-气相色谱法测定了N₂O浓度、饱和度和扩散通量.结果表明,天津市不同景观河流N₂O浓度都处于过饱和状态,表现为大气N₂O的源;N₂O浓度、饱和度和扩散通量均值为（23.85±15.20）nmol·L^-1、（309.71±197.38）%和（27.04±16.46）μmol·（m²·d）^-1,范围分别为12.70～115.69 nmol·L^-1、 164%～1 502%和9.17～244.79μmol·（m²·d）^-1.天津市不同土地利用类型河流N₂O浓度和扩散通量具有较大的空间异质性,表现为：排污河>城市河流>郊区河流>农业河流.天津滨海河流N₂     

商陆和烟草对锰胁迫的抗氧化响应研究

研究植物的重金属累积能力对于植物修复和植物冶金意义重大.Mn超累积植物商陆(Phytolacca americana L.)的耐性/累积机制至今还不清楚,为了研究商陆在Mn胁迫下的抗氧化酶作用,将萌发6周的商陆和烟草幼苗分别放入1 mmol·L~(-1)或3 mmol·L~(-1)的1/2 Hoagland营养液处理4 d,实验表明商陆叶片光合速率降低幅度显著低于烟草,而烟草MDA含量和电解质渗漏量增加幅度大于商陆.如1 mmol·L~(-1) Mn处理4 d后,与对照相比,商陆和烟草的光合速率分别降低13.3%和75.5%;烟草MDA含量和电解质渗漏量分别增加347.3%和120.1%,而商陆的MDA含量和电解质渗漏量没有明显增加,表明Mn胁迫对超累积植物引起的氧化损伤明显低于非累积植物.随着Mn处理浓度的提高和时间的延长,2种植物叶片SOD和POD活性均迅速增加,其中商陆SOD活性的增加幅度大于烟草;另外,商陆CAT活性持续上升,而烟草CAT活性显著下降.如在1 mmol·L~(-1) Mn处理下,商陆SOD、POD和CAT活性分别提高161.1%、 111.3%和17.5%;烟草SOD和POD提高55.5%和206.0%,而CAT下降15.6%,表明商陆的抗氧化酶,特别是CAT,能够有效地清除Mn毒产生的自由基.这些结果说明抗氧化酶的抗氧化能力是重金属累积植物商陆的Mn耐性机制之一.     

电化学微传感器检测水中痕量铜离子

为改善微电极在阳极溶出伏安法检测重金属离子过程中低电流响应和低电催化能力的缺点,提出了一种在碳纤维微电极表面合成还原氧化石墨烯/纳米金材料制得还原氧化石墨烯纳米金修饰碳纤维微电极（rGO/AuNPs CFMEs）的方法.通过SEM表征,所制备的rGO/AuNPs CFMEs具有比表面积高、吸附能力强和催化活性好的特点,因此改性微电极适合作为方波阳极溶出伏安法（SWASV）测定水中铜离子（Cu²⁺）的工作电极.在构建微传感器测试水中痕量铜离子系统后,对pH值、电导率、富集时间和富集电位等检测条件进行了优化.在pH值为4,电导率为36.1S/m,富集时间为360s,富集电位为-1.2V的最佳条件下,铜的线性范围和检出限分别0~1.0μmol/L和2.4nmol/L.此外,微传感器的可重复性、长期稳定性以及选择性也得到了验证.     

IL/GO/88A的制备及其对四环素的光催化降解性能

使用离子液体(ILs)辅助生长新型光催化材料IL/GO/88A用于降解四环素(TC),使用XRD、FTIR、SEM、N₂吸附-脱附、UV-vis、EIS等方法分别对催化材料进行了表征分析,考察了催化剂投加量、pH、TC浓度对TC降解的影响。该复合材料表现出高效的TC降解效率。在催化剂投加量为0.30 g·L⁻¹、pH为5.7、TC溶度为10 mg·L⁻¹的条件下,光照180 min后,IL/GO/88A对TC的去除率达到95.7%。催化剂在重复利用3次后仍能保持稳定的性能。此外,阐明了吸附-光催化协同机理,并推断·OH、h⁺是主要的活性物种。本研究结果对开发高效MOFs光催化复合材料并用于处理含四环素废水提供了新思路。     

氧化镁基生物质炭高效去除水体中磷的特性

利用花生壳为前驱体,在高温限氧条件下,将氧化镁(MgO)负载于生物质炭(BC)表面制备出氧化镁基生物质炭(MgOBC)复合材料.系统研究了MgO-BC对水体中P的吸附特性,并探讨了溶液pH值、接触时间、竞争离子等因素对P的吸附效果的影响.结果表明,P的最佳吸附初始pH为7~9,过酸过碱的环境均不利于P的吸附;P的吸附过程可在540 min内达到平衡,且动力学曲线较好地符合伪一级和伪二级动力学模型,拟合系数可达97.3%和99.0%;当Cl~-、HCO_3~-、NO_3~-等共存离子的量浓度达到P的10倍时,MgO-BC对P仍具有较强的吸附能力;P的吸附过程较好地符合Langmuir等温模型,拟合系数达99%,理论最大吸附容量为138.07 mg·g~(-1),远高于其它未经改性或改性的生物质炭和几种典型P吸附剂的吸附容量.此外,吸附P后的复合材料可作为肥料施入土壤,可有效实现P的再利用.综上所述,该MgO-BC复合材料在净化实际P污染水体中有着广阔的应用前景.     

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.     

用电解锰阳极泥和含SO_2工业尾气制备硫酸锰

以电解锰阳极泥与电解锌生产中产生的含SO_2尾气为原料,经过反应、浸出、浸出液两次净化和浓缩结晶制备硫酸锰,考察了反应时间、含SO_2尾气的流量及反应温度对Mn~(4+)转化率的影响.实验结果表明:在反应时间45 min、反应温度20～30 ℃、含SO_2尾气流量16 L/min的条件下,Mn~(4+)转化率达90%以上;尾气中SO_2利用率随尾气流量增加而降低;所得MnSO_4·H_2O产品质量达到GB1622-86<工业级硫酸锰标准>.