多光子解离CHClF_2富集~(13)C

用无氦TEA CO_2激光器(9μm带谱线)辐照F-22,选择性激发~(13)CHClF_2,使其达到离解,得到~(13)C的富集。测得选择系数α的峰值位置在1047cm~(-1),相对于~(13)CHClF_2的线性吸收峰位置红移了36cm~(-1),α随激光能量密度、F-22气压的增高而降低。     

基于胺法的旋流喷淋气液吸收烟气CO2的性能

为了强化CO_2捕集过程的气液传质,设计了一类多级旋流喷淋反应器,实验研究了典型的醇胺(乙醇胺(MEA)、二乙醇胺(DEA))脱除CO_2的分离效率和传质系数,并分析了操作条件的影响.结果表明:在相同的实验条件下,MEA的脱碳效率(最大值95%)大于DEA的脱碳效率(最大值92.3%).与相关研究数据的对比表明,多级旋流喷淋可以有效增强醇胺-CO_2喷淋反应系统的传质过程.醇胺溶液旋流气液吸收烟气CO_2的脱碳效率受操作条件的影响,其随着吸收剂质量分数、吸收剂流量和反应温度的增加而提高,随着烟气中CO_2体积分数和烟气流量的增加而降低.     

温室效应的作用过程及其后果

近年来,地球气候异常,科学界普遍认为这是温室效应所致。温室效应是怎么回事呢?可以这样简单地说:地表温度的变化是阳光对大气层作用的结果,太阳的一部分光被大气层的云、雪、冰反射回太空,但绝大部分为地球吸收,转化为热量。地球的一部分热量从地表上升后穿过温室效应气体屏障,但其中部分热量因气体分子振荡而反射回地面,从而加剧了热效应(如图所示)。温室效应气体包括二氧化碳(50％),沼气(20％),氯氟碳(15％),笑气(10％)及臭氧(5％)。由于温室效应气体的主要成份是二氧化碳CO_2,因此CO_2愈多,     

CO_2和水蒸气对稀燃NO_x催化转化器的影响

针对稀燃NOx催化转化器(LNT)在工作阶段CO_2和水蒸气的体积分数对稀燃汽油机经济性及排放性的重要影响,结合LNT工作过程对吸附过程进行了建模。LNT入口边界条件由试验数据测得,在缩核模型基础上通过建立LNT工作过程模型分别探究了CO_2、水蒸气以及二者同时存在时对LNT吸附过程的影响,通过分析BaO和Ba(OH)2的吸附机理研究了3种吸附载体BaO、Ba(OH)2及BaCO3在不同气体组分下的覆盖率变化。结果表明:CO_2会显著降低LNT对NO_x的吸附效率,且降低的效果与CO_2的体积分数基本无关;水蒸气在一定程度上会降低LNT工作过程的吸附效率,其影响比CO_2的影响小,且随着水蒸气体积分数的增大,LNT吸附效率降低更明显;CO_2和水蒸气同时存在时吸附效率介于单独CO_2条件和单独水蒸气条件二者之间。     

CO_2回收电解锰渣中可溶性锰的结晶动力学

为研究利用CO_2从电解锰渣中回收可溶性锰的结晶机理,采用Avrami-Erofeev等温结晶动力学模型分析了在不同温度条件下碳酸锰晶体的成核和生长特性.结果表明:在初始锰浓度2.5 g·L~(-1)、pH 6.6、CO_2体积分数15%、CO_2流量0.4 L·min~(-1)、搅拌速率600 r·min~(-1)的条件下,电解锰渣反洗液中碳酸锰晶核生成和晶体生长阶段的表观活化能分别为42.82 kJ·mol~(-1)和61.15 kJ·mol~(-1).在温度为318 K反应120 min时,锰通过形成碳酸盐,回收率可达99.98%,锰渣反洗液符合《污水综合排放标准》(GB 8978-1996)中总锰的一级排放标准.     

一个确定吸收介质特征参量的方法

提出了一个能同时测定横向弛豫时间T_2,小信号吸收系数α_0和饱和光强I_(?)等吸收介质特征参量的简单方法.用可调谐CW CO_2激光和SF_6气体为样品的实验证实了我们的理论分析结果.实验测得对SF_6(0.2托)T_2=1.24×10~(-11)s,α_0=0.27cm~(-1),I_(?)=1.11W/cm~2.     

用激光量热法测量红外光窗材料的光学吸收系数

本文介绍一种改进了的激光量热法,以测量高透明材料低吸收系数绝对值的方法。对于薄试样,β1<0.1的情况下,当CO_2激光束照射试样时,测试试样所吸收的能量。采用X—Y记录仪自动记录试样的温度随时间变化曲线,即温升与温降曲线。由曲线上求出激光关闭时相应温度点T_1的温升速率和温降速率。测量透射试样的激光功率。将实验数据代入考虑激光束在试样中多次反射的计算公式,即可求出试样的吸收系数。实验结果表明,用几瓦CW功率的CO_2激光器测得高阻GaAs材料试样的吸收系数β值在10~(-2)cm~(-1)数量级范围内。     

CO_2/CH_4在干酪根中竞争吸附规律的分子模拟

选取有机质作为研究对象,构建干酪根模型,采用巨正则系综蒙特卡罗(GCMC)方法和分子动力学方法(MD)研究不同摩尔分数、不同压力下CH_4和CO_2的气体的竞争吸附行为以及吸附引起的干酪根本体形变。结果表明:CH_4和CO_2单组分吸附时吸附量随着压力的增大而增大,CO_2吸附会在较小的压力时达到饱和,两种气体吸附符合Langmuir吸附规律,可以使用Langmuir方程进行拟合;在相同的压力和温度下,CO_2/CH_4吸附选择性会随着CO_2摩尔分数的增大而减小,CO_2更易被干酪根吸附;干酪根与CO_2有较强的相互作用,干酪根中不同的原子对吸附起着不同的作用;低压阶段吸附是引起体积应变的主要原因,高压阶段压力对体积应变发挥明显作用。     

溴代N-丁基吡啶离子液体的合成及吸收CO_2性能研究

以吡啶、溴代正丁烷为原料合成了溴代N-丁基吡啶离子液体([bpy]Br),使用红外光谱、核磁共振氢谱分析方法对产物结构进行了表征。运用热重-差示扫描量热仪(TG-DSC)对离子液体的热稳定性进行测定,结果表明离子液体[bpy]Br的液态温度为99.3~238.0℃。实验研究了离子液体[bpy]Br对CO_2的吸收性能和离子液体再生后对CO_2的吸收负荷。结果表明:随着离子液体[bpy]Br质量分数的增加,离子液体吸收CO_2的负荷增加;随着吸收温度的升高,离子液体吸收CO_2的负荷减少;随着通入CO_2流量的增加,离子液体吸收CO_2达到饱和的时间缩短。离子液体再生后对CO_2的吸收性能基本不变。     

氨水溶液同时吸收烟气中SO_2和CO_2的实验及模拟

燃煤电厂排放大量SO_2和CO_2等气态污染物,相应的减排技术研究十分必要。利用湿壁塔实验台对氨水溶液(质量分数为0.2%~7%)同时吸收SO_2和CO_2的传质特性进行了实验研究,并结合Aspen Plus速率模型分析了填料塔的吸收性能,对氨水溶液同时吸收SO_2和CO_2吸收系统的设计做了必要的探讨。实验结果表明:随着CO_2体积分数(5%~20%)的增加,SO_2选择性吸收因子有所降低,SO_2的传质系数变化较小且均高于CO_2的传质速率一个数量级;SO_2质量浓度(0~11 428mg/m3)和反应温度(20~80℃)的增加,对CO_2的吸收产生不利影响,氨水溶液趋向于选择性吸收SO_2。氨水溶液中SO_2负载量(SO_2在氨水溶液中相对NH3的摩尔浓度)在0.1~0.4之间增加时,CO_2的传质系数大幅降低。氨水溶液质量分数增加对CO_2及SO_2的吸收传质均有利,选择性吸收因子降低,且实验值和模型计算值符合良好。采用同时吸收SO_2和CO_2的填料吸收塔,结合控制氨挥发的氨洗塔及用于SO_2负载控制的离子交换装置的吸收系统,可以实现污染物的有效脱除。     

星载CO2探测频率步进扫描IPDA激光雷达回波信号反演及误差分析

设计了星载CO₂探测频率步进扫描积分路径差分吸收（IPDA）激光雷达,弥补了欧洲航天局A-SCOPE项目单波长CO₂探测IPDA激光雷达对波长依赖性较强等不足.仿真计算了一个扫描周期内的激光雷达回波信号和系统的相对随机误差、大气压强不确定性误差以及频率不稳定性误差.当频率步进扫描到on-line波长为6 361.235 0 cm-1时,在海面反射率为0.035 sr-1、大气压强不确定性为0.001以及激光频率不稳定性为0.3 MHz条件下,系统综合相对误差为0.084 2%.结果表明,采用频率步进扫描方法结合IPDA激光雷达技术探测大气CO₂浓度不仅可以观察到相对误差随on-line波长变化的关系,而且可以有效地减小测量误差,使其小于0.5×10-6.      

Impact of technology advances on China’s CO2 emission reduction

Global warming tends to be the major characteristics of the dramatic global climate change. To deal with these changes, the impact of reducing greenhouse gas (GHG) emission on Chinese future economic and social development has to be assessed. In this paper, a Regional Integrated model of Climate and the Economy (RICE), which is well known and accepted widely, has been used for Chinese economic assessment of climate change after introduction, assimilation and verification. Based on a sensitivity analysis of technical parameters in the RICE model and constrained targets proposed for energy saving and emissions reduction technological advance programs of China from 2000 to 2050, the economic impact of the programs is examined. The results indicate that when technology advances, Chinese CO₂ emission, climate loss, and the growth rate of atmospheric CO₂ concentration and temperature will all decrease. It is assumed that in 2010, the CO₂ emission is 20% lower than in 2005, CO₂emission in 2050 would only double the level in 2000, the accumulative CO₂ emission would be decreased by 12.4 GtC, and the atmospheric CO2 concentration and temperature in 2050 would reduce by 35 GtC and 0.04°C respectively from 2000 to 2050. The accumulative climate loss from 2000 to 2050 will drop down by 4.6 billion dollar, which only accounts for 6% of the global total benefits. However, the economic benefit the developed countries will obtain is 10 times that for China under such a technological advance scenario. The decrease of the CO₂ emission control rate is 1% in cooperation policy while 4.6% in non-cooperation policy, which would relieve China’s burden in the control of CO₂ total emission and thereby benefit China in participation of the international cooperation for CO₂ emission reduction.     

第一性原理研究MoS2的电子结构及光学性质

为了系统深入地研究MoS_2的电子能带结构和光电性质,基于密度泛函理论的第一性原理平面波赝势方法,计算和分析了材料MoS_2的电子结构及其光学性质,给出了MoS_2的能带结构、光吸收谱、电子态密度、能量损失谱、反射谱、介电函数谱等光学性质。计算结果表明:体材料MoS_2的电子跃迁形式是非垂直跃迁,具有间接带隙的半导体材料,带隙宽为1.126 eV;价带和导带的形成是由Mo和S的价电子起作用产生的。通过分析其光学性质,发现MoS_2的介电函数的实部和虚部的峰值都出现在低能区,当光子能量的升高,介电函数值会缓慢降低;材料MoS_2对可见紫外区域的光子具有很强的吸收,最大吸收系数为3.17×105cm~(-1);MoS_2在能量为18.33eV位置出现了共振现象,其它区域内能量的损失值都趋于为0,说明电子之间共振非常微弱。这些光学性质奠定了该材料在制作微电子和光电子器件方面的作用,尤其是在紫外探测器应用方面有着潜在的应用前景,为未来对MoS_2材料的进一步研究提供理论参考。     

MoTe2的电子结构及光学性质的理论研究

利用密度泛函理论第一性原理方法对MoTe_2的能带结构、能态密度和光学性质进行了理论计算,得到能带结构、态密度、光吸收谱、能量损失谱和介电函数等光学性质。结果表明:MoTe_2具有间接带隙宽度为1.066 eV的半导体材料,价带主要由Mo的5s4p价电子和Te的5s5p价电子起主要作用;导带由Mo和Te的4d价电子起主要作用。由获得的光学性质可知,介电函数的实部和虚部的峰值都出现在低能区;位于可见到紫外区域的光子具有很强的吸收,最大吸收系数为2.84×10~5cm~(-1);同时在光子能量为16.40 eV处出现了共振现象,其它区域内电子之间共振非常微弱。这些光学性质奠定了该材料在制作微电子和光电子器件方面的作用。     

理论研究半金属TiB2的电子结构和光学特性

为了系统地分析半金属TiB₂的能带结构及光学特性，采用密度泛函理论的第一性原理平面波赝势方法，计算分析了TiB₂的电子结构及光学特性。能带结构表明TiB₂具有直接带隙宽度为0.388 eV的半金属材料，在费米能级附近，态密度的价带主要由Ti的3p价电子和B的2p价电子起作用，导带由Ti的3d价电子起主要贡献。从获得的光学特性参数发现在光子能量为0.73 eV处，Ti的4s3p和B的2p电子发生共振，复介电函数的峰值主要出现在低能区，材料对紫外光的最大吸收系数为4.03×10⁵cm^-1。本研究得到的光学特性参数在光电子器件、微电子和紫外探测器等制作方面有着较好的参考作用。     

Trend, seasonal and diurnal variations of atmospheric CO2 in Beijing

The concentration of atmospheric CO₂ in Beijing increased rapidly at a mean growth rate of 3.7% · a⁻¹ from 1993 to 1995. After displaying a peak of (409.7±25.9) μmol · mol⁻¹ in 1995, it decreased slowly. Both the almost stable anthropogenic CO₂ source and increasing biotic CO₂ sink contribute to the drop of CO₂ concentration from 1995 to 2000. The seasonal variation of CO₂ concentration exhibits a clear cycle with a maximum in winter, averaging (426.8±20.6) μmol · mol⁻¹, and a minimum in summer, averaging (369.1±6.1) μmol·mol⁻¹. The seasonal variation of CO₂ concentration is mainly controlled by phenology. The mean diurnal variation of atmospheric CO₂ concentration for a year in Beijing is highly clear: daily maximum CO₂ concentration usually occurs at night, but daily minimum CO₂ concentration does in the daytime, with a mean diurnal difference more than 34.7 μmol·mol⁻¹. It has been revealed that the interannual variations of atmospheric CO₂ concentration in winter and autumn regulated the interannual trend of atmospheric CO₂, whereas the interannual variation of CO₂ concentration in summer affected the general tendency of atmospheric CO₂ in a less degree.     

Changes of photosynthetic capacity of some plant species under very high CO2 concentrations in Biosphere 2

Conclusions The initial slope of A/ light curve became steep under high CO₂ (700 μmol · mol^-1) compared with that under low CO₂ (350 μmol · mol^-1) for the C₃ species growing in very high CO₂(>2 200 μmol · mol^-1) for a long period. The light compensation points remained unchanged, but the light saturation points were found increased. The ϕ_m,_app and A_max of the C₃ species increased respectively by 79 % and 80 %, while those of C₄ species decreased by 10% and 14%, respectively. The shape of A/light curve of C₄ species did not change. Such results indicated that C₃ species increased the capacity of photosynthesis, while C₄ did not change, otherwise it decreased a little. This work only compared the changes of capacity in photosynthesis of some species under different CO₂ levels in Biosphere 2. We need further investigation on the effects of high CO₂ on the same species outside Biosphere 2, in order to fully undertand the effects and mechanism of response of plants to the elevated CO₂.     

Measurement of the absorption spectrum of H2O+ in the visible region

Together with the 74 lines belonging to (0,9,0)- (0,0,0) band, the high-resolution absorption spectrum of H₂O⁺ A²A₁-X²B₁ system was observed in the visible region of 16680 — 17300 cm^-1 using optical heterodyne magnetic rotation enhanced velocity modulation spectroscopy for the first time, which verifies the high sensitivity and high signal to noise ratio (S/N) of this technique.     

Bi~(3+)/Yb~(3+)共掺GdVO_4近红外发光性能研究

使用高温固相法制备了一种新的Bi3+,Yb3+共掺杂GdVO4量子裁剪近红外发光材料,该材料在波长为250~400nm的紫外光激发下发射出很强的近红外光(900~1100nm).由于体系中Bi3+离子的引入,相对于Gd0.9Yb0.1VO4,Gd0.87Yb0.1Bi0.03VO4在989nm处的近红外发光强度提高近120%,且其激发峰也从323nm红移至341nm,整个激发谱带更宽,更有利于实际应用.由于Yb3+离子既可以利用基质中的VO3-4电荷迁移态跃迁的能量,也可以同时利用Bi3+的1S0-3P1能级跃迁传递能量,相对于目前报道的理论量子裁剪效率最高的YVO4:Bi3+,Yb3+,GdVO4:Bi3+,Yb3+无论其近红外发光强度还是可见光发光强度强度皆有提升,是一种很有希望的紫外宽带激发近红外发光材料.     

Features of major greenhouse gases in loess, Shanxi Province, China

According to the investigations of five loess sections in Shanxi Province, China, it was found that the concentrations of the major greenhouse gases CO₂, CH₄ and N₂O in loess-paleosol sequences are generally high, even sometimes may be several times or scores of times higher than their atmospheric concentrations respectively. Although the CO₂ concentration in the same loess section shows poor regularity among different layers, it increases slowly from north to south in space. The CH₄ concentration in the layers under Malan Loess is much higher than that in the atmosphere, although it is not high in Malan Loess. Most of the δ¹³C values of CO₂ in loess are -11.14‰—15.48‰ (relative to PDB standard). Analysis of carbon isotopic compositions of CO₂ indicates that the main source of CO₂ in loess section is decomposition of ‘stable’ organic matters by microbes. The δ¹³C_g of CO₂ is a little heavier than organic source for exchanging carbon isotope with carbonate in loess. The abundant carbonate in loess not only makes the loess a huge carbon reservior but also adjusts