磁性壳聚糖微球固定化褐藻酸酶的研究

利用反相悬浮交联法制备磁性壳聚糖微球(magnetic chitosan microspheres，M—CS)，并对褐藻酸酶进行固定化研究。结果表明，M—CS呈规则的圆球形，具有较好的磁响应性，可稳定地保存在弱酸和弱碱中。其弱碱交换量随着戊二醛用量的增加而减少，悬挂醛基则相应地增加。M—CS对褐藻酸酶的吸附动力学实验表明，M—CS容易吸附褐藻酸酶，但吸附的酶量受载体与酶的比例、溶液的离子浓度、戊二醛的用量、溶液pH的影响明显，而温度对吸附的酶量的影响则相对较弱。酶学性质研究表明，相对于游离的褐藻酸酶，固定化酶的最适温度略有升高，可明显改善其热稳定性和酸碱稳定性，与底物的亲和力也有所增强。     

2-萘酚吸附树脂热解和燃烧特性的研究

利用热重-差热分析仪对染料化工企业产生的2-萘酚吸附树脂在4种不同气氛下的热重（TG）和微分热重（DTG）曲线进行研究。试验结果表明：2-萘酚吸附树脂在高温、氧化条件下不稳定，易于分解，其热分解失重率受气氛变化的影响较大。提出了2-萘酚吸附树脂热解和燃烧机理，给出了热解反应动力学参数和模型。     

锌锡复合掺杂纳米二氧化钛的光催化性能研究

采用溶胶—凝胶法制备了Zn2+、Sn4+复合掺杂的TiO2光催化剂,通过XRD、TEM、UV—Vis测试手段对样品进行分析,以对硝基苯酚为研究对象,对其进行光催化降解。结果表明:复合掺杂Zn2+、Sn4+提高了催化剂对波长在200—450 nm范围内的光的吸光度,发生"红移"。在氙灯激发下,其催化活性优于纯TiO2。     

弱频散条件下大气运动的非线性演变过程

研究非线性过程对大气运动影响的一个常用方法是在一定条件下,将大气运动力学方程化为一些熟知的典型非线性演变方程,再利用数学中已有的结果进行讨论。Long、Redekopp等从地转涡度方程出发,证明了迭加在带状切变气流中的长的Rossby波的演变可以用著名的Kdv方程来描述。此     

城市热岛成因及其对污染物扩散影响的数值模拟

采用大涡模拟方法,通过数值求解可压缩流体的动力学方程和欧拉型的浓度扩散方程,建立了不同的地表模型,将城市地表差异等因素作为地面热通量的边界条件引入,得到了简单区域上的温度场和流场的三维结构,证实了城乡地表差异是引起热岛现象的根本原因之一,成功再现了城市热岛现象,并研究了城市热岛效应的存在对污染物扩散的影响。     

湿位涡、热力学参数CD与涡度、散度演化

从湿斜压原始方程出发,将热力学方程引入散度方程,导出了显示包含热力学参数CD影响的散度方程。在此基础上,结合湿位涡方程,分析了湿斜压大气中湿位涡水平分量MPV2及其热力学参数CD的动力学性质,揭示了由热力学参数CD表征的斜压动力过程激发对流层中低层涡、散场演变的动力机制,阐明了应用热力学参数CD诊断暴雨中尺度系统发生发展和预报暴雨的理论依据。     

强降雨区传播效应对双基地系统辅站雷达探测能力的影响

以电磁场散射理论为基础,在已有的小椭球粒子群双基地多普勒雷达气象方程中加入了传播效应项,利用此方程探讨旋转椭球雨滴群旋转轴一致铅直向上,双基地系统在探测均匀雨区、移动雨区和不均匀分布雨区时传播效应的影响。通过与单基地雷达回波功率比较可知,传播效应的存在使得双基地系统辅站一侧回波功率比高值区的范围变大,主站雷达一侧,传播效应对回波功率的影响与入射波的偏振关系有关。      

降水条件对人工影响天气外场作业的影响及预报方法初探

利用国家气象中心所提供的T106等格点资料,对呼市地区实施人工影响天气作业前的天气条件进行诊断分析,根据呼市地区降水系统的天气动力学的演变特征,筛选出了能较好反映降水系统的天气动力学的特征因子,采用PP方法,依次建立呼市地区4-9月稳定性和对流性降水的预报方程.以此来定量分析实施人工影响天气作业的天气系统以及确定人工影响天气作业的具体方法.     

大气动力学方程组的定性理论及其应用

基于完整的湿大气动力学方程组,利用无穷维动力系统的新理论和新方法,系统讨论了强迫耗散的非线性大气系统的定性理论及其应用。将完整的强迫耗散非线性湿大气动力学方程组化为Hilbert空间中一个等价的算子方程,研究了算子的性质及其物理意义,在此基础上得到湿大气系统全局吸引子的存在性定理,揭示出系统向外源的非线性适应特征,并把结果推广到有地形动力作用和非定常外源强迫的情形。同时探讨了大气方程组惯性流形的存在,大气多平衡态产生的根源以及强迫、耗散和非线性对系统解的渐近行为的影响。在理论结果的基础上,提出强迫耗散的非线性动力系统中存在三类时间边界层、方程组简化准则、分解算法的算子约束原则以及支撑吸引子基底的少数自由度的构造方法,探讨了理论在非线性发展方程差分格式的设计和计算稳定性分析、多平衡态的数值分析、数值模式延伸预报的改进、短期气候预测以及一类中尺度系统分析与预测中的应用,指出描述长期过程动力学模式的必备条件,给出初值与模式相协调的合理解释。最后,对今后的研究方向作了展望。     

沙尘表面非均相吸附系数不确定性及其影响的数值模式研究

本文从实验气溶胶样品、实验技术和分析方法三个方面对以往的实验室研究结果进行综合分析, 归纳总结出适合东亚地区沙尘气溶胶的非均相吸附系数γ的参考值, 并利用区域大气化学模式, 模拟研究了非均相吸附系数γ的不确定性对东亚地区沙尘气溶胶非均相化学过程的影响。为了研究非均相反应对γ的敏感性, 针对其中四种物质(HNO3、N2O5、O3和SO2) 的γ上限值和下限值, 分别进行了T-up (上限值) 和T-low(下限值)两个敏感实验; 针对相对湿度对HNO3和N2O5非均相吸附系数的影响进行了T-rh敏感实验。模拟结果与观测资料进行了对比分析, 结果表明模式可以比较好地反映气态物质、气溶胶浓度的演变过程和非均相反应过程。考虑非均相反应后模拟的硫酸盐和硝酸盐浓度与观测值更接近一些。采用γ参考值的模拟结果总体上比采用γ上限值和γ下限值更合理, 把γ系数作为相对湿度的函数来处理比作为常数处理更合理。沙尘气溶胶通过非均相化学反应, 可以使模拟区域内SO2、NOx和O3的平均浓度下降, 使硫酸盐和硝酸盐颗粒物浓度增加, 采用γ参考值计算得到3 km以下的上述物质的变化率分别为－3.44%、－5.92%、－1.75%、5.22%和23.25%, 显示沙尘表面非均相化学反应对大气化学成分特别是气溶胶有较大的影响; 不同γ取值对上述物质变化率有一定影响, 其中对硝酸盐和臭氧的影响较大, T-up和T-low 模拟结果之间可以相差13.4%和10.1%。     

Rapid change in nitrate and sulfate concentrations observed in early stage of precipitation and their deposition processes

The concentrations of H⁺, nitrate (NO₃ ^-), and sulfate (SO₄ ^2-) in rainwater and their temporal changes were analyzed on the basis of continuous observation from 1 July 1991 to 30 June 1992 at a suburb of Nagoya, Japan. The yearly average for pH was 4.4. In general, an increasing pH with increase in precipitation amount was observed for rain events. Relatively high pH rainwater was sometimes observed at the beginning of rainfall, even though high concentrations of NO₃ ^- and SO₄ ^2- were involved. The high pH values were considered to be caused by the neutralization process with particulate matter containing cations. The yearly averaged ratio of equivalent concentration of nitrate to sulfate (N/S) in rainwater was 0.58. In the early stage of rain, the N/S value was usually more than 1.0 due to the difference of scavenging process between NO₃ ^- and SO₄ ^2-. High values of N/S ranging from 5 to 10 were found under the atmospheric conditions of calm winds and low humidity, during which it is possible that atmospheric particles float for a long time in the air before a rain event. The adsorption of NO₃ ^- in the early stage of rainfall by particulate matter was suggested from the difference in scavenging processes of NO₃ ^- and SO₄ ^2-. A possible scavenging process, called limb cloud scavenging, is presented to explain the interaction of particles and nitrate ions at the early stage of rain. In limb cloud scavenging, the repeated migration of cloud particles or raindrops between the inside and outside of clouds increases the absorption of ions to a highly condensed level, thus increasing the N/S value of rainwater. The influence of global scale seasonal phenomena with large amounts of particulates, such as typhoons or Asian dust storms, was also studied.     

The Effect of Atmospheric Organic Compounds on the Fe-Catalyzed S(IV) Autoxidation in Aqueous Solution

Laboratory experiments were conducted with real atmospheric aerosol particles as well as with synthetic solutions under dark conditions, to simulate some of the chemical features of aerosols. In solutions obtained by the leaching of aerosols (size range >D _ae: 0.4–1.6 m) that contained sufficient amounts of transition metal ions (e.g. Fe) and organic species (e.g. oxalate), S(IV) oxidation rates were significantly lower than those expected from the Fe-catalyzed S(IV) autoxidation in Milli-Q water. The results suggest that oxalate is responsible for much of the observed inhibition. Acetate and formate also inhibit the reaction, but to a much lesser extent. Oxalate has a strong inhibiting effect on the Fe-catalyzed S(IV) autoxidation at all investigated pH values (2.8, 3.7 and 4.5). It was established that Fe(III)-oxalato complexes affect the redox cycling of Fe(II)/Fe(III) and that the observed decrease of the reaction rate is caused by the reduced amount of catalytically active Fe(III) due to the complexation with oxalate. For the system Fe-S(IV)-O₂-oxalate at initial pH 3.7 the reaction rate was calculated using exponential simplification to account for oxalate influence on the amount of free Fe(III) by the following equation:–r_S(IV) = k · [S(IV)] · [Fe(III))] · e ^-b·[Ox]     

On the effect of large-scale atmospheric transport on chemistry and amount of atmospheric precipitation in the center of European Russia

The dependence of precipitation amount, acidity, and ionic composition on the atmospheric circulation is studied based on the computation of the back trajectories over the period of 1982–1993. Quantitative estimates of basic parameters of trajectories are derived, and their significant difference in the summer and wintertime is considered. The trajectory frequency for the cases with precipitation in the center of European Russia is computed at the regular grid points depending on the diurnal precipitation amount, acidity, and sulfate/chloride ratio. It is shown that in case of abundant precipitation both in summer and winter the highest frequency of trajectories is observed in the same regions. In the case of low precipitation, seasonal differences are observed. It is revealed that precipitation with pH > 5 is mostly connected with the air inflow from Scandinavia and the north of European Russia, while during the trajectory passage over Central and Southern Europe pH < 5 prevails in precipitation. The chlorine ions prevail most often when trajectories pass over central regions of the Mediterranean and of Middle Asia and (although somewhat less) over Scandinavia and northern Russian seas.     

Water Resources Implications of Global Warming: A U.S. Regional Perspective

The implications of global warming for the performance of six U.S. water resource systems are evaluated. The six case study sites represent a range of geographic and hydrologic, as well as institutional and social settings. Large, multi-reservoir systems (Columbia River, Missouri River, Apalachicola-Chatahoochee-Flint (ACF) Rivers), small, one or two reservoir systems (Tacoma and Boston) and medium size systems (Savannah River) are represented. The river basins range from mountainous to low relief and semi-humid to semi-arid, and the system operational purposes range from predominantly municipal to broadly multi-purpose. The studies inferred, using a chain of climate downscaling, hydrologic and water resources systems models, the sensitivity of six water resources systems to changes in precipitation, temperature and solar radiation. The climate change scenarios used in this study are based on results from transient climate change experiments performed with coupled ocean-atmosphere General Circulation Models (GCMs) for the 1995 Intergovernmental Panel on Climate Change (IPCC) assessment. An earlier doubled-CO₂ scenario from one of the GCMs was also used in the evaluation. The GCM scenarios were transferred to the local level using a simple downscaling approach that scales local weather variables by fixed monthly ratios (for precipitation) and fixed monthly shifts (for temperature). For those river basins where snow plays an important role in the current climate hydrology (Tacoma, Columbia, Missouri and, to a lesser extent, Boston) changes in temperature result in important changes in seasonal streamflow hydrographs. In these systems, spring snowmelt peaks are reduced and winter flows increase, on average. Changes in precipitation are generally reflected in the annual total runoff volumes more than in the seasonal shape of the hydrographs. In the Savannah and ACF systems, where snow plays a minor hydrological role, changes in hydrological response are linked more directly to temperature and precipitation changes. Effects on system performance varied from system to system, from GCM to GCM, and for each system operating objective (such as hydropower production, municipal and industrial supply, flood control, recreation, navigation and instream flow protection). Effects were generally smaller for the transient scenarios than for the doubled CO₂ scenario. In terms of streamflow, one of the transient scenarios tended to have increases at most sites, while another tended to have decreases at most sites. The third showed no general consistency over the six sites. Generally, the water resource system performance effects were determined by the hydrologic changes and the amount of buffering provided by the system's storage capacity. The effects of demand growth and other plausible future operational considerations were evaluated as well. For most sites, the effects of these non-climatic effects on future system performance would about equal or exceed the effects of climate change over system planning horizons.     

Analysis of bulk precipitation chemistry in Serbia for the period from 1982 to 2010

Bulk precipitation samples collected daily through bulk collectors at eight meteorological stations in Serbia were analyzed for their chemical composition. The data covers time series, from 20 to 28 years, in the period between 1982 and 2010. The most abundant ion in the samples was sulfate. Only 0.17 % of all samples were from strong acid rains (pH < 3.5). The relatively high average pH values (5.94–6.26) of the collected precipitation indicate the neutral or alkaline nature of local rainwater. Trends in both the annual amount and the composition of precipitation were tested by the nonparametric Mann–Kendall test and Sen’s slope estimator. Significant increasing trend of precipitation was identified for almost all stations. Rebuilding activities after the bombing of Serbia in 1999 were identified as a possible anthropogenic cause of the sharp increase of some ions (Ca²⁺) in the first year following the bombing. The origin of air masses arriving at one particular station was examined using two-dimensional backward trajectories. Western sectors (W, SW and NW) accounted for almost half (44.3 %) of all rainy days, while eastern sectors (SE, E and NE) brought only 10.4 % of all rainy days. The distribution, per sector, of volume-weighted concentrations of sulfate, nitrate, ammonium, calcium, potassium, magnesium, chloride and sodium ions, as well as the amount of precipitation and its pH values for one station, was also analyzed. Rainwater from the SE and S sectors was the most polluted.     

Ultraviolet radiation in the background region over Northeast China

Measurements of broadband global solar and ultraviolet radiation (UV-KZ) by a Kipp & Zonen radiometer from 2005 to 2011 at three sites in the background region over Northeast China were used to investigate the characteristics of the temporal variability of UV-KZ radiation in Northeast China. The highest annual mean daily values of UV-KZ (0.53 MJ m^?2 d^?1) were observed at Sanjiang and Changbai Mountain. The lowest value (0.49 MJ m^?2 d^?1) was measured at Hailun due to the high aerosol burden and the long path of solar radiation. The diurnal variation in UV-KZ radiation on four clear days near the equinoxes and solstices exhibited bell-shaped curves, with a maximum at approximately noon. There was little difference in UV-KZ radiation between representative spring and autumn days except that the amount of UV-KZ radiation during the spring was higher than that during the autumn. The relationship between the maximum values of UV-KZ radiation and clearness index can be accurately demonstrated with three polynomial equations. An empirical estimation model suited for all weather conditions was developed using measurements collected at Hailun. The slope of the linear regression between the measured and modeled UV-KZ radiation was approximately 1, the intercept of the linear regression equation was near zero, and the relative error of the equation was less than 8.5 %. These validation results suggest that this model can accurately estimate the UV-KZ radiation based on more conventional measured radiation data. The empirical estimation model can also serve as a valuable method for the study of ecological processes in other regions.     

Adsorption and reaction of trichlorofluoromethane on various particles

As a possible tropospheric sink of trichlorofluoromethane (CCl₃F), its adsorption and reaction on solid particles were studied with or without UV light longer than 310 nm. The adsorption and photodesorption occurred for most of the particles examined. The amounts depended not only on the BET surface area but also on the chemical property of the particles. The reaction rates were less than 0.1% h^-1. The surface induced degradation of CCl₃F in air was confirmed under photoirradiation at room temperature by the detection of Cl^- or F^- on some metal oxides. When the particles were pretreated with heat and evacuation, the reaction rate became larger and disproportionation of CCl₃F took place. The tropospheric lifetime of CCl₃F was reevaluated based on a reported model. It is suggested that the heterogeneous reaction of CCl₃F on particles may be a possible tropospheric sink.     

1980～2013年华东小雨减少及其主要影响因子分析

本文通过对1980～2013年华东区域447站各等级降水的时空分布特征进行分析,从低空气温、水汽、相对湿度入手,采用经验正交函数分析（Empirical Orthogonal Function,简称EOF）、合成分析等诊断方法揭示小雨与低空气温、水汽、相对湿度之间的关系;根据克劳修斯-克拉珀龙（Clausius-Clapeyron）方程,从物理角度对温度和水汽含量变化对小雨减少的相对贡献进行分析,并选取长三角区域利用能见度资料分析小雨减少的特征。研究主要得出以下结论:（1）华东区域1980～2013年总降水日和总降水量分布呈现南多北少随纬度增加递减趋势,总降水日主要以小雨日为主,小雨日占总降水日的71.84%。除暴雨外,其它各等级降水均呈现出减少趋势,以小雨的减少最为显著,小雨日和小雨量区域平均减少趋势为－3.37 d (10 a)-1、－6.52 mm (10 a)-1。小雨日EOF分解的第一模态呈现了华东区域小雨日一致减少的分布特征;第二模态则体现了小雨日变化的不均匀性,具有明显的区域差异。（2）小雨日的减少是伴随着低空增温发生的,低空温度上升了0.32 K (10 a)-1,同时可降水量呈现微弱的减少趋势。小雨日的变化与低空相对湿度有很好的正相关关系,EOF分解结果也揭示了低空相对湿度具有与小雨一致的空间分布特征。合成分析表明低空气温偏高（低）年,小雨日偏少（多）,可降水量偏多（少）年,小雨日偏多（少）,相对湿度偏高（低）年,小雨日偏多（少）。（3）根据Clausius-Clapeyron方程和相对湿度公式,低空增暖使饱和水汽压增加6% K-1～7% K-1,饱和水汽压增加在水汽微弱减少的前提下,导致了低空相对湿度的显著减少,从而导致了小雨的减少。对低空温度,比湿变化对小雨的影响进行分析,发现单纯由温度变化引起的相对湿度减少为－4.83%,而单纯由于比湿变化引起的相对湿度变化为－1.91%,分析表明了低空增暖是引起小雨日减少的主要原因。（4）能见度较差的区域,年均小雨日和小雨量偏少,但是小雨的长期减少趋势主要还是由低空增暖引起的相对湿度的减少导致的。     

H2释放扰动电离层的数值模拟

由于电离层中分子性离子与电子的复合要比氧离子与电子的复合快得多,因此H₂在电离层高度释放可有效地引起电子的消耗。本文基于一个包括中性气体扩散方程和离子化学反应方程的二维动力学模型,对H₂在电离层高度释放过程进行了数值模拟研究,并分析了不同释放条件下的电子扰动特性。结果表明:1)500 mol H₂释放后,迅速向周围空间扩散,释放中心处的电子密度30 s内下降了近4%,F₂层临界频率下降了1%左右;2)在不同高度处释放H₂时,最大的电子密度相对变化率并不是在峰值高度附近处释放时出现的;3)释放化学物质的量越多,电子密度的扰动幅度也越大,但两者之间并不存在线性关系;4)相同量的H₂在电离层峰值高度处释放,白天的电子密度扰动幅度要大于夜间的扰动幅度。