Co3O4/介孔分子筛催化剂对苯催化完全氧化的研究

分别以介孔分子筛MCM-41、MCM-48、SBA-15为载体,采用等体积浸渍法制备了氧化钴/介孔分子筛催化剂,利用N₂吸附、X射线衍射、程序升温还原等技术对催化剂进行了表征,考察了Co₃O₄的负载量及载体的孔结构对催化剂完全催化氧化苯的性能的影响。结果表明,Co₃O₄的负载量为20%时,催化剂的催化活性最好;载体的孔径和催化剂的可还原性能是影响催化活性的主要因素,催化剂活性顺序为Co₃O₄ /SBA-15> Co₃O₄ /MCM41> Co₃O₄ /MCM-48。     

Long-term geochemical evolution of the near field repository: insights from reactive transport modelling and experimental evidences

The KBS-3 underground nuclear waste repository concept designed by the Swedish Nuclear Fuel and Waste Management Co. (SKB) includes a bentonite buffer barrier surrounding the copper canisters and the iron insert where spent nuclear fuel will be placed. Bentonite is also part of the backfill material used to seal the access and deposition tunnels of the repository. The bentonite barrier has three main safety functions: to ensure the physical stability of the canister, to retard the intrusion of groundwater to the canisters, and in case of canister failure, to retard the migration of radionuclides to the geosphere. Laboratory experiments (< 10 years long) have provided evidence of the control exerted by accessory minerals and clay surfaces on the pore water chemistry. The evolution of the pore water chemistry will be a primordial factor on the long-term stability of the bentonite barrier, which is a key issue in the safety assessments of the KBS-3 concept.In this work we aim to study the long-term geochemical evolution of bentonite and its pore water in the evolving geochemical environment due to climate change. In order to do this, reactive transport simulations are used to predict the interaction between groundwater and bentonite which is simulated following two different pathways: (1) groundwater flow through the backfill in the deposition tunnels, eventually reaching the top of the deposition hole, and (2) direct connection between groundwater and bentonite rings through fractures in the granite crosscutting the deposition hole. The influence of changes in climate has been tested using three different waters interacting with the bentonite: present-day groundwater, water derived from ice melting, and deep-seated brine. Two commercial bentonites have been considered as buffer material, MX-80 and Deponit CA-N, and one natural clay (Friedland type) for the backfill. They show differences in the composition of the exchangeable cations and in the accessory mineral content. Results from the simulations indicate that pore water chemistry is controlled by the equilibrium with the accessory minerals, especially carbonates. pH is buffered by precipitation/dissolution of calcite and dolomite, when present. The equilibrium of these minerals is deeply influenced by gypsum dissolution and cation exchange reactions in the smectite interlayer. If carbonate minerals are initially absent in bentonite, pH is then controlled by surface acidity reactions in the hydroxyl groups at the edge sites of the clay fraction, although its buffering capacity is not as strong as the equilibrium with carbonate minerals. The redox capacity of the bentonite pore water system is mainly controlled by Fe(II)-bearing minerals (pyrite and siderite). Changes in the groundwater composition lead to variations in the cation exchange occupancy, and dissolutionȁ3;precipitation of carbonate minerals and gypsum. The most significant changes in the evolution of the system are predicted when ice-melting water, which is highly diluted and alkaline, enters into the system. In this case, the dissolution of carbonate minerals is enhanced, increasing pH in the bentonite pore water. Moreover, a rapid change in the population of exchange sites in the smectite is expected due to the replacement of Na for Ca.     

Preconcentration of cadmium and copper ions on magnetic core–shell nanoparticles for determination by flame atomic absorption

Magnetic core–shell nanoparticles modified by (3-aminopropyl) trimethoxy silane were prepared and used as adsorbent for the extraction and preconcentration of cadmium and copper ions. The ions were desorbed with nitric acid followed by determination with flame atomic absorption spectrometry. The extraction conditions were investigated systematically. The method was applied for the determination of Cd(II) and Cu(II) ions in different water samples. The accuracy was also evaluated through analysis of certified reference material.     

佛山市臭氧浓度时间变化特征及主要影响因子

对佛山市2011—2014年O_3监测数据进行分析,结果表明,ρ(O_3)日变化呈现明显的单峰特征,2011—2014年O_3日最大8小时滑动均值(O3-8 h)的年评价值没有出现显著的下降趋势,超标值多出现在8—10月。夏季O3-8 h与日平均气温的相关系数较高,O_3污染多发生在气温30℃,相对湿度为50%~70%的气象条件下。相对湿度60%,气温为20~25℃,也可能出现O3污染。10℃时,不同的温度条件下,O_3与PM_(2.5)存在正相关关系。在不同的季节时段,O_3-8 h基本随着ρ(NO_2)/ρ(NO)增大而增大。     

上海市臭氧污染时空分布及影响因素

分析2006—2016年上海市的监测数据发现,臭氧(O_3)浓度存在逐年上升趋势,污染持续时间有所增加,但除水平风速有下降趋势外,其他相关气象因素的年际变化趋势并不显著。空间分析结果表明,上海市O_3超标主要集中在西南部郊区,但市区O_3超标潜势不容忽视。O_3污染高发季节的污染玫瑰图分析发现,上海市南部地区是影响上海市O_3污染的关键区域;对于NO_2减排的影响分析发现,尽管上海市O_3平均浓度总体处于上升趋势,但在NO_2下降幅度最为明显的内环市区和北部郊区,O_3上升幅度低于NO_2下降幅度较小的内外环区域和西部郊区,表明上海市的O_3污染控制仍需持续推进NOx的减排,并同步推进VOCs的减排。     

以绿化三维量分析植物群降解SO2的宏观效应

控制和降低城市上空ＳＯ２的环境浓度对于改善城市环境，促进城市生态的良性循环具有十分重要的意义。本文从上海市绿化三维量分布模型、与ＳＯ２浓度分布模型的相关分析入手，以季节变化作为对比因子，讨论了城市绿化植物群的数量及分布对城市上空ＳＯ２浓度分布的宏观影响；并据此提出了可有效地控制城市上空ＳＯ２浓度的绿地建设的基本原则。     

Upgrading of organic waste: production of the copolymer poly-3-hydroxybutyrate-co-valerate by Ralstonia eutrophus with organic waste as sole carbon source

Two types of fermented organic waste (trade and industry waste and fruit and vegetable waste) were successfully used as a sole carbon source to produce poly-3-hydroxybutyrate-co-valerate (PHBV) by Ralstonia eutrophus (formerly Alcaligenes eutrophus) via oxygen limitation.The production of PHBV could be optimized by optimizing the oxygen transfer through the fermentor. Thereby, a peak concentration of 1.1 g PHBV per liter cell suspension, 40 w% of cell dry weight, was obtained at an aeration rate of 0.24 mol O₂/h·kg biomass. The yield of PHBV on the fatty acid concentration in the organic waste was 0.16 g polymer/g volatile organic matter. The process obtained, compares well with the commercial production process of PHBV based on glucose.     

温敏性水凝胶对金属离子Y3+,UO2+2的浓集分离

利用合成的ＰＮＩＰＡＡｍ／ＡＡｃ交联共聚温敏性水凝胶分别对水溶液中微量的Ｙ＾２＋,ＣＵ２＾２＋离子进行浓集分离研究。实验结果表明,凝胶能有效浓集Ｙ＾２＋,ＵＯ２＾２＋离子,在ＰＨ＝１～４范围内,凝胶的溶胀比及对Ｙ＾３＋,ＵＯ２＾２＋的浓集率均随ＰＨ的增大而增大,浓集率分别达到８０％和９０％,凝胶溶胀比的增大浓集量分别为５．２９３ｍｇ．ｇ＾－１、３６．１６ｍｇ．ｇ＾－１凝胶的表面积也对浓集率有限大影     

Changes in bird‐migration patterns associated with human‐induced mortality

Many bird populations have recently changed their migratory behavior in response to alterations of the environment. We collected data over 16 years on male Great Bustards (Otis tarda), a species showing a partial migratory pattern (sedentary and migratory birds coexisting in the same breeding groups). We conducted population counts and radio tracked 180 individuals to examine differences in survival rates between migratory and sedentary individuals and evaluate possible effects of these differences on the migratory pattern of the population. Overall, 65% of individuals migrated and 35% did not. The average distance between breeding and postbreeding areas of migrant individuals was 89.9 km, and the longest average movement of sedentary males was 3.8 km. Breeding group and migration distance had no effect on survival. However, mortality of migrants was 2.4 to 3.5 times higher than mortality of sedentary birds. For marked males, collision with power lines was the main cause of death from unnatural causes (37.6% of all deaths), and migratory birds died in collisions with power lines more frequently than sedentary birds (21.3% vs 6.3%). The percentage of sedentary individuals increased from 17% in 1997 to 45% in 2012. These results were consistent with data collected from radio‐tracked individuals: The proportion of migratory individuals decreased from 86% in 1997–1999 to 44% in 2006–2010. The observed decrease in the migratory tendency was not related to climatic changes (temperatures did not change over the study period) or improvements in habitat quality (dry cereal farmland area decreased in the main study area). Our findings suggest that human‐induced mortality during migration may be an important factor shaping the migration patterns of species inhabiting humanized landscapes.     

The problem of estimating recent genetic connectivity in a changing world

Accurate understanding of population connectivity is important to conservation because dispersal can play an important role in population dynamics, microevolution, and assessments of extirpation risk and population rescue. Genetic methods are increasingly used to infer population connectivity because advances in technology have made them more advantageous (e.g., cost effective) relative to ecological methods. Given the reductions in wildlife population connectivity since the Industrial Revolution and more recent drastic reductions from habitat loss, it is important to know the accuracy of and biases in genetic connectivity estimators when connectivity has declined recently. Using simulated data, we investigated the accuracy and bias of 2 common estimators of migration (movement of individuals among populations) rate. We focused on the timing of the connectivity change and the magnitude of that change on the estimates of migration by using a coalescent‐based method (Migrate‐n) and a disequilibrium‐based method (BayesAss). Contrary to expectations, when historically high connectivity had declined recently: (i) both methods over‐estimated recent migration rates; (ii) the coalescent‐based method (Migrate‐n) provided better estimates of recent migration rate than the disequilibrium‐based method (BayesAss); (iii) the coalescent‐based method did not accurately reflect long‐term genetic connectivity. Overall, our results highlight the problems with comparing coalescent and disequilibrium estimates to make inferences about the effects of recent landscape change on genetic connectivity among populations. We found that contrasting these 2 estimates to make inferences about genetic‐connectivity changes over time could lead to inaccurate conclusions.