空气氧化解吸NO络合吸收产物试验研究

Fe(Ⅱ) EDTA易被氧化为对NO无吸收能力的Fe(Ⅲ)EDTA,为实现Fe(Ⅱ)EDTA的循环使用,提出了Fe(Ⅱ)EDTA络合吸收-空气氧化解吸-铁屑还原再生组合脱除NO新工艺.采用空气氧化解吸络合吸收产物Fe(Ⅱ) EDTA (NO)中NO的方法,研究了温度及压力对Fe(Ⅱ)EDTA(NO)空气氧化解吸过程的影响.结果表明,0.4 MPa、333K为较优的解吸条件.该工艺可循环脱除NO,成本低、效率高,能有效回收NO2资源.     

制备条件对低温NH_3-SCR脱硝催化剂Mn-Ce/TiO_2结构与性能的影响

采用溶胶凝胶法制备了Mn-Ce/TiO2催化剂,以NH3为还原剂,通过程序升温反应考察其选择性催化还原NO的催化性能.同时,着重探讨了焙烧温度、焙烧时间、活性物质负载量及Mn、Ce负载比例对催化剂结构和性能的影响,并用BET、XRD等对催化剂进行了表征.结果表明,活性组分负载量由0增至20%时,NO转化率随着负载量的增加而提高,当(Mn+Ce)质量分数为20%,催化剂活性最高,此后随着活性组分负载量的增加,NO转化率明显下降;Mn与Ce的负载比例为0.85∶0.15时,催化剂比表面积最大,为112.31m2·g-1;焙烧温度500℃时催化剂晶相均为TiO2锐钛矿型结构,焙烧温度升高至600℃,催化剂晶相为TiO2锐钛矿型和金红石型混合结构,且催化剂比表面积急剧减小;焙烧时间对催化剂晶相结构影响不大,焙烧时间为5h时,Mn-Ce/TiO2的脱硝性能最好.     

武汉市耕地非农化的空间自相关分析

经济发展和城市扩张使包括耕地在内的大量开放空间被不断侵蚀,随着人们对耕地非市场价值和生态功能认识的不断加深,如何合理高效可持续地利用耕地被广泛关注。采用空间自相关分析方法从乡镇尺度定量研究了武汉市耕地非农化的空间关系,以探讨快速发展时期平原城市耕地非农化空间关系的变化及其原因。研究表明:(1)全局Morans I显示武汉市耕地非农化在1990~2011年的4个时期均呈现出显著的全局空间自相关,其聚集强度以2005年为分界点,前3个时期不断加强后有所下降;(2)通过EB修正的武汉市耕地非农化的LISA图显示武汉市耕地非农化的聚集区域由开始处于区域外围的LL型聚集为主导逐步转变为处于城乡交错区域的LH+HH型聚集为主导;(3)通过绘制不同时期不同聚集类型的重心移动路径可以发现LH+HH型聚集均出现先向东南再向东北移动的趋势,这种耕地非农化趋势与区域的产业布局有密切关系。通过空间自相关分析掌握武汉市耕地非农化的空间特征是开展耕地保护和实现耕地合理利用的基石,根据研究结果可以确定重点和优先管制区域以提升土地利用管制效果,协调好城市建设和耕地资源保护间的关系。     

Novel Co-Mg-Al-Ti-O catalyst derived from hydrotalcite-like compound for NO storage/decomposition

Catalysts of Co_1.5Mg_1.5/Al_0.9Ti_0.1O and Co_1.5Mg_1.5/AlO were successfully prepared by calcinations of corresponding hydrotalcite-like compounds at 800℃ for 4 hr. The derived oxides were of spinel phase and a small quantity of Ti substitution did not change the crystal purity. Their catalytic performance for the NO storage/decomposition was investigated. Ti incorporation enhanced the NO decomposition activity while has an opposite effect on the storage capacity of catalyst. In situ FT-IR spectra of the catalysts showed that the final adsorption species on the catalysts was coordinated nitrates/nitrites. In addition, NO storage/decomposition mechanism has been discussed on the basis of these observations.     

Effect of CeO2 and Al2O3 on the activity of Pd/Co_3O_4/cordierite catalyst in the three-way catalysis reactions (CO/NO/CnHm)

The present article studies the effect of CeO₂ and Al₂O₃ on the activity of Pd/Co₃O₄/cordierite catalyst in conversion of NO, CO, C_nH_m. The catalysts were characterized by temperature programmed reduction with hydrogen, X-ray diffraction, X-ray photoelectron spectroscopy and transmission electron microscopy. It is shown that the effect of CeO₂ on the properties of Pd/Co₃O₄/cordierite catalyst depends on preparation method. The catalyst obtained by co-deposition of cerium and cobalt oxides has higher activity in CO oxidation (CO + O₂ and CO + NO) and total hexane oxidation (C₆H₁₄ + O₂). Such phenomenon is probably caused by more than stoichiometric amount of formed oxygen vacancies, an increase in both mobility of surface oxygen and dispersity of components in the catalytic composition. It is demonstrated that CeO₂ addition promotes the SO₂ resistance of Pd/Co₃O₄/cordierite. The second support decreases the activity of Pd/Co₃O₄/cordierite catalyst in the reactions of CO and C₆H₁₄ with oxygen because of CoAl₂O₄ formation.     

Adsorption characteristics and mechanism of Cr （Ⅵ） on chitoan-yttrium porous microsphere

以壳聚糖和Y2（OH）5NO3为原料通过乳液交联法制备了壳聚糖-钇（Ch—Y）复合微球,通过扫描电镜、透射电镜、X射线衍射、红外光谱等方法对其表面形貌、结构进行了表征.探讨了溶液的pH值、反应时间、投加量、离子初始浓度对其吸附性能的影响.研究结果表明,壳聚糖-钇（Ch—Y）复合微球在pH值为3的酸性环境中对Cr（Ⅵ）保持了较高的吸附能力,吸附容量为52.39mg·g-1,其吸附行为符合Langmuir吸附等温模型;通过吸附机理的研究,发现壳聚糖-钇（Ch—Y）对Cr（Ⅵ）吸附是化学吸附静电吸附协同氧化Cr（Ⅵ）离子作用来实现的.     

鄂尔多斯十大孔兑区植被生产力变化趋势对土地利用转移的响应

归一化植被指数(Normalized difference vegetation index,NDVI)是衡量区域植被生产力变化的一个重要指标,而土地利用/覆盖变化(Land use/cover change,LUCC)进程深刻影响了陆地生态系统空间分布格局及其生产力变化。因此本文结合趋势分析和转移矩阵法,从中分辨率成像光谱仪(Moderate-resolution Imaging Spectroradiometer,MODIS)NDVI年际变化角度分析鄂尔多斯北部典型农牧交错区(十大孔兑地区)2000-2015年植被生产力的变化趋势与LUCC的关系。结果表明:(1)在农牧交错区植被生产力总体呈增加趋势,其中显著增加和不显著增加区域面积占总面积的89.41%,分别为22.01%和67.4%;其后依次为不显著减少区域、无变化区域和显著减少区域,面积比例分别为4.59%、3.32%和2.68%。(2)在不显著增加和显著增加区,土地转换面积分别为235146.08 hm2和82761.76 hm2,草地转为农田、林地、水体、建设用地和未利用地尤其是草地转为农田导致对应区域植被生产力增加。     

喷灌和沟灌方式对农田土壤NH3挥发的影响

研究了2016和2017年传统灌溉（沟灌）和节水灌溉（喷灌）方式氨（NH₃）挥发的季节年际动态变化特征及其影响因素.采用通气法进行原位监测,分析了土壤温度、体积含水量、铵态氮（NH₄⁺-N）、硝态氮（NO₃^--N）以及气温降水等因素对NH₃挥发的影响.结果表明,NH₃挥发速率的峰值出现在施用氮肥后1~2周,喷灌有效降低NH₃挥发峰值,喷灌和沟灌的NH₃挥发速率峰值在2016年分别为2.67kg/（hm²·d）和11.11kg/（hm²·d）,2017年分别为2.42kg/（hm²·d）和11.73kg/（hm²·d）;马铃薯生长季NH₃挥发存在明显的季节变化,挥发高峰主要发生在7~8月,追肥期高于基肥期.2016~2017年农田土壤NH₃累积挥发量均表现为喷灌<沟灌,与沟灌相比,喷灌分别减少58.15%和43.55%.NH₃挥发速率与土壤温度呈显著正相关（P<0.05）,与体积含水量、NH₄⁺-N、NO₃^--N浓度呈极显著正相关（P<0.01）.     

基于随机森林模型的中国近地面NO2浓度估算

NH₃针对传统近地面NO₂浓度空间模拟过程中NO₂浓度与其影响要素之间关系的复杂非线性机制解释不充分的缺陷,本研究基于随机森林（RF）算法、融合多源地理要素开展了近地面NO₂浓度空间分布模拟研究.以卫星OMI对流层NO₂柱浓度数据和多源地理要素（道路交通、气象因子、土地利用/覆盖、地形高程、人口数量）为输入变量,近地面NO₂浓度为输出变量,利用RF算法构建近地面NO₂浓度反演模型.通过对比地面观测数据与传统土地利用回归模型（LUR）检验RF模型的有效性,基于所构建的最优RF模型在不同时间尺度下模拟分析中国大陆地区近地面NO₂浓度空间分布特征.结果表明：（1）集成多源地理要素的RF回归模型精度高,月均模型整体拟合度R² 0.85,RMSE 6.08μg/m³,交叉验证的R² 0.84,RMSE 6.33μg/m³,显著高于LUR模型（拟合R² 0.53,RMSE 10.48μg/m³,交叉验证的R² 0.53,RMSE 10.49μg/m³）; （2）地面NO₂浓度与预测变量呈现显著的复杂非线性与时间尺度依赖关系,卫星OMI柱浓度对模型影响程度最大,重要性指标IncMSE介于97.40%~116.54%,多源地理特征变量对RF模型同样具有不可忽视的贡献力（IncMSE在23.34%~47.53%之间）;（3）中国大陆地区NO₂污染程度较高,年均模拟浓度为24.67μg/m³,存在明显季节性空间差异,NO₂浓度冬季（31.85μg/m³） > 秋季（24.86μg/m³） > 春季（23.24μg/m³） > 夏季（18.75μg/m³）,呈现以华北平原为高值中心、向外围逐渐减轻的空间分布格局.较已有研究揭示对流层NO₂柱浓度宏观分布特征,本研究对近地面NO₂污染特征的研究成果对于合理制定污染防控策略、降低居民暴露健康损害具有指导意义.     

Characteristics of roadside air pollution in Korean metropolitan city (Daegu) over last 5 to 6 years: temporal variations, standard exceedances, and dependence on meteorological conditions

The present study performed a roadside data analysis to provide baseline data for exploring associations between environmental exposure to four gaseous pollutants and health effects on residents living near roadways. The yearly roadside concentrations of CO and SO₂ showed a well-defined decreasing trend, whereas those of NO₂ and O₃ exhibited the reverse trend. In most cases, the diurnal trends of the roadside concentrations were well-defined for all seasons, plus the daytime concentrations were higher than the nighttime concentrations. In contrast to the other target pollutants, the daytime O₃ concentrations observed at the roadside sites were lower than those observed at the residential site, likely due to high-levels of fresh NO from traffic emissions that rapidly react with O₃, thereby reducing the O₃ roadside level. The Sunday roadside concentrations of CO, NO₂, and SO₂ were similar to or somewhat lower than the weekday concentrations. Conversely, for O_3, the Sunday roadside concentrations were similar to or somewhat higher than the weekday concentrations. The higher O₃ concentrations on Sunday may be due to the reduced titration from a decrease in NO_x emissions under VOC-limited conditions (low VOC/NO_x conditions). The monthly averages of O₃ concentrations exhibited the reverse seasonal variation to the other target compounds, with peak O₃ concentrations between April and June, and the second peak between August and October. It is also suggested that for O₃, the 8-h standard is more stringent than the 1-h standard, while for NO₂ and SO₂, the 1-h standard is more stringent than the 24-h standard. The multiple regression equations obtained from the relationship between the concentrations and five meteorological parameters indicated that the number and type of meteorological variables in the equations varied according to the pollutant, monitoring station, or season.