La3+掺杂对吸附相反应制备TiO2复合催化剂的结晶过程及弱紫外光下活性的影响

利用吸附相反应技术制备弱紫外光响应的高效催化剂,并通过XRD、XPS以及HRTEM探索了不同焙烧温度下La3+掺杂量对TiO2结晶过程的影响.结合弱紫外光下甲基橙的降解反应,深入研究催化剂结晶过程的变化对弱紫外光下催化剂活性的影响.结果表明,La3+掺杂会抑制TiO2的结晶过程.当焙烧温度或者掺杂量较低时,La3+不能进入TiO2的晶格结构但会轻微地抑制TiO2的结晶过程;未进入晶格结构的La3+存在会引入光生载流子的浅能级捕获中心,在弱光体系中极大提升了催化剂的活性.当La3+的掺杂量为0.05%(原子分数)时,经过900℃焙烧后催化剂降解能力最高,其活性超过商用P25的2倍多.在较高La3+掺杂量(超过0.20%)时,900℃焙烧后一定量La3+进入TiO2的晶格结构而大大抑制了TiO2结晶;这种强烈的抑制作用使得催化剂中存在大量无定形结构TiO2,无定形TiO2甚至多于700℃焙烧后的催化剂,反而大大抑制了弱光体系中催化剂活性.     

Carbon dioxide and methane fluxes in the littoral zones of two lakes,east Antarctica

During the summertime of 2007/2008, carbon dioxide (CO₂) and methane (CH₄) fluxes across air–water interface were investigated in the littoral zones of Lake Mochou and Lake Tuanjie, east Antarctica, using a static chamber technique. The mean fluxes of CO₂ and CH₄ were ?70.8 mgCO₂ m^?2 h^?1 and 144.6 μgCH₄ m^?2 h^?1, respectively, in the littoral zone of Lake Mochou; The mean fluxes were ?36.9 mgCO₂ m^?2 h^?1 and 109.8 μgCH₄ m^?2 h^?1, respectively, in the littoral zone of Lake Tuanjie. Their fluxes showed large temporal and spatial dynamics. The CO₂ fluxes showed a significantly negative correlation with daily total radiation (DTR) and a weakly negative correlation with air temperature and water temperature, indicating that sunlight intensity controlled the magnitude of CO₂ fluxes from the open lakes. The CH₄ fluxes significantly correlated with local air temperature, water table and total dissolved solids (TDS), indicating that they were the predominant factors influencing CH₄ fluxes. Summertime CO₂ budgets in the littoral zones of Lake Mochou and Lake Tuanjie were estimated to be ?152.9 gCO₂ m^?2 and ?79.7 gCO₂ m^?2, respectively, and net CH₄ emissions were estimated to be 312.3 mgCH₄ m^?2 and 237.2 mgCH₄ m^?2, respectively. Our results show that shallow, open, alga-rich lakes might be strong summertime CO₂ absorbers and small CH₄ emitters during the open water in coastal Antarctica.     

Historical change of mercury pollution in remote Yongle archipelago, South China Sea

We collected three ornithogenic coral sand sedimentary profiles from Jinyin Island, Jinqing Island and Guangjin Island of Yongle archipelago, South China Sea and reconstructed the deposition flux of anthropogenic Hg over the past 700 years in the study area. On the whole, the anthropogenic Hg flux is relatively low; it remained at a low level before the Industrial Revolution with a small peak at about 1450-1550 AD, which may record the enhanced metallurgy activity in Ming Dynasty of China. During the 20th century, the deposition flux of anthropogenic Hg increased rapidly, but two troughs occurred during the periods around 1940s and 1970s, corresponding to the economic depression caused by World War II, Civil War in China (1945-1949), and the Culture Revolution (1966-1976) in China. Since the 1970s the deposition flux of anthropogenic Hg has been persistently increasing, apparently the result of fast economic development in East and Southeast Asia countries around South China Sea.     

Methane fluxes from tundra soils and snowpack in the maritime Antarctic

Methane fluxes were measured from three exposed tundra sites and four snowpack sites on the Fildes Peninsula in the maritime Antarctic in the summertime of 2002. The average fluxes at two normal tundra sites were −15.3 μg m⁻² h⁻¹ and −14.3 μg m⁻² h⁻¹, respectively. The fluxes from tundra site with fresh penguin dropping addition showed positive values with the average of 36.1 μg m⁻² h⁻¹, suggesting that the deposition of fresh droppings greatly enhanced CH₄ emissions from the poor Antarctic tundra during penguin breeding periods. The summertime variation in CH₄ flux was correlated with surface ground temperature and the precipitation. The correlation between the flux and PT₀, which is the product of the precipitation and surface ground temperature, was quite strong. The diurnal cycle of CH₄ flux from the tundra soils was not obtained due to local fluky weather conditions. The fluxes through four snowpack sites were also obtained by the vertical CH₄ concentration gradient and their average fluxes were −46.5 μg m⁻² h⁻¹, −28.2 μg m⁻² h⁻¹, −46.4 μg m⁻² h⁻¹ and −17.9 μg m⁻² h⁻¹, respectively, indicating that tundra soils under snowpack also consume atmospheric CH₄ in the maritime Antarctic; therefore these fluxes could constitute an important part of the annual CH₄ budget for Antarctic tundra ecosystem.     

Nitrous oxide emissions from tundra soil and snowpack in the maritime Antarctic

The nitrous oxide emissions were measured at three tundra sites and one snowpack on the Fildes Peninsula in the maritime Antarctic in the summertime of 2002. The average fluxes at two normal tundra sites were 1.1 ± 2.2 and 0.6 ± 1.7 μg N₂O m⁻² h⁻¹, respectively. The average flux from tundra soil site with penguin dropping addition was 3.7 ± 2.0 μg N₂O m⁻² h⁻¹, 3–6 times those from the normal tundra soils, suggesting that the deposition of fresh droppings enhanced N₂O emissions during penguin breeding period. The summer precipitation had an important effect on N₂O emissions; the flux decreased when heavy precipitation occurred. The diurnal cycle of the N₂O fluxes from Antarctic tundra soils was not obtained due to local fluky weather conditions. The N₂O fluxes through four snowpack sites were obtained by the vertical N₂O concentration gradient and their average fluxes were 0.94, 1.36, 0.81 and 0.85 μg N₂O m⁻² h⁻¹, respectively. The tundra soils under snowpack emitted N₂O in the maritime Antarctic and increased local atmospheric N₂O concentrations; therefore these fluxes could constitute an important part of the annual N₂O budget for Antarctic tundra ecosystem.     

纳米刻蚀法制备氧化锰介孔材料及其降解高含盐废水中罗丹明B

为了有效去除高含盐废水中的有机染料污染物,利用有序介孔硅材料作为模板剂,通过硬模板法制备了新型锰系氧化物（MnO_x）介孔材料作为类Fenton催化剂.催化剂的结构表征结果表明,模板剂在锰前驱物溶液中浸渍和后续煅烧成型过程决定了氧化锰介孔材料的结构.浸渍-煅烧成型重复次数越多,MnO_x介孔材料中孔道结构的有序度和氧化锰的结晶度越好.浸渍-煅烧成型次数过少,MnO_x介孔材料中孔道呈现无序状态,比表面积较大但氧化锰结晶度不足;次数过多则形成更为致密的小孔径的孔道结构,从而使MnO_x介孔材料的比表面积减小.由于对罗丹明B（RhB）良好的选择性吸附能力和较多的Mn³⁺/Mn⁴⁺对,具有有序规则孔道的氧化锰介孔材料具有优异的类Fenton催化活性,对高含盐废水中RhB的5 h降解去除率最高可达90%左右.     

Multilevel air quality evolution in Shenyang: Impact of elevated point emission reduction

Visibility observed at different altitudes is favorable to understand the causes of air pollution. We conducted 4-years of observations of visibility at 2.8 and 60 m and particulate matter(PM) concentrations from 2015 to 2018 in Shenyang, a provincial city in Northeast China. The results indicated that visibility increased with the increasing height in winter(especially at night), and decreased with height in summer(especially at the daytime). PM concentration exhibited opposite vertical variati...     

Fluoride Content in Bones of Adelie Penguins and Environmental Media in Antarctica

Fluoride (F) distribution and its effects (fluorosis) were investigated in Antarctica. Droppings (L) excreta selected of aquatic birds, lake water, soil and moss (Polytrichum alpinum) showed a high F concentration. Although bones of Adelie penguin (Pygiscelis adeliae) and skua (Catharacta maccormicki) showed exceptionally very high F concentration in the range of 832 to 7187 mg kg(-1), their radiographs did not show any evidence of skeletal fluorosis. The possible reason and geochemical aspects of F in Antarctica region are discussed.     

南极菲尔德斯半岛植被微区CO2浓度的监测

在南极苔藓植被的微环境区内 ,CO2 的浓度在 4 73 5mg·m- 3以上 ,大大高于全球CO2 的平均浓度 (3 56mg·m- 3) ,可见苔藓等植被区可能是大气CO2 的源之一 .这与特殊的南极条件下植被的生理生态特性有关 .在苔藓分布区 ,CO2 浓度日变化的主要影响因素是光照和温度 .菲尔德斯半岛变化无常的天气状况使得CO2 浓度昼夜变化规律出现局部波动 ,不同的天气状况也使CO2 浓度发生变化 .研究表明 :光照条件是CO2 浓度变化的主导影响因素 ,从CO2 浓度的季节变化中可以看出 ,CO2 浓度变化与大气温度呈负相关 ;与降水量和空气相对湿度呈正相关 .本文首次给出了极地环境下植被微区的CO2 浓度变化及其影响因素 ,为极地温室气体的研究提供了新的材料     

TiO2表面沉积Ag粒子及其可见光下降解含盐废水中的苯酚

为了制备可见光激发下能高效降解含盐废水中有机物的光催化剂,首次以商用TiO_2光催化剂(P25)为载体,利用吸附相反应技术一步获得了Ag沉积的可见光响应复合光催化剂.同时,通过XPS、TEM、HRTEM及紫外可见漫反射光谱图,结合多种高含盐水体系中苯酚的光催化降解过程,研究了不同Ag沉积对催化剂可见光活性的影响.结果发现,吸附平衡后P25表面富含水的吸附层可作为反应和粒子的生成场所,生成量子尺寸的Ag粒子.另外,在吸附层中生成的Ag粒子均匀分布于P25表面并与之紧密结合,并在TiO_2晶格结构中引入晶格交错结构.Ag与TiO_2的表面等离子体共振效应和晶格交错结构共同提升了催化剂的可见光响应和电荷的分离效率,增强了催化剂对苯酚的可见光催化性能.在含盐废水体系中,盐离子数量越多,催化剂在可见光下降解苯酚过程受到的干扰越大.