Heterogeneous Fenton-like degradation of 4-chlorophenol using iron/ordered mesoporous carbon catalyst

Ordered mesoporous carbon supported iron catalysts(Fe/OMC) were prepared by the incipient wetness impregnation method and investigated in Fenton-like degradation of 4-chlorophenol(4CP) in this work. XRD and TEM characterization showed that the iron oxides were well dispersed on the OMC support and grew bigger with the increasing calcination temperature. The catalyst prepared with a lower calcination temperature showed higher decomposition efficiency towards 4CP and H2O2, but more metals were leached. The effect of different operational parameters such as initial pH, H2O2 dosage, and reaction temperature on the catalytic activity was evaluated. The results showed that 96.1% of 4CP and 47.4% of TOC was removed after 270 min at 30°C, initial pH of 3 and 6.6 mmol/L H2O2. 88% of 4CP removal efficiency was retained after three successive runs, indicating Fe/OMC a stable catalyst for Fenton reaction. 4CP was degraded predominately by the attack of hydroxyl radical formed on the catalyst surface and in the bulk solution due to iron leaching. Based on the degradation intermediates detected by high performance liquid chromatography, possible oxidation pathways were proposed during the 4CP degradation.     

江汉平原农田土壤有机碳分布与变化特点:以潜江市为例

以地处江汉平原腹地的潜江市农田土壤(水田、旱地)为研究对象,于2011年实地采样分析表层土壤(0~20 cm)有机碳的分布现状,并对比第二次土壤普查(1983年)资料,探讨28 a来江汉平原农田土壤有机碳的分布与变化特点.结果表明,2011年潜江市农田表层土壤有机碳密度为30.50 t·hm-2,碳储量为452.82×104t,与1983年相比有明显下降,下降速率分别为0.10 t·(hm2·a)-1和1.53 t·a-1,碳储量共损失了9%.两个时期水田土壤有机碳密度均明显高于旱地土壤,分别是旱地土壤的1.6倍和1.3倍,但是经过28年的常规耕作管理,水田土壤有机碳密度呈下降趋势,下降速率为0.23 t·(hm2·a)-1,导致的有机碳损失为52.83×104t,损失比例达16%;而旱地土壤有机碳则以0.05 t·(hm2·a)-1的速率缓慢增长,碳储量共增加了8.57×104t,增加比例为5%,远不能抵消水田土壤的有机碳损失.水田土壤碳储量的损失主要来自于低产潜育型水稻土碳密度的大幅下降所致(尽管其所占面积比例较小),其碳损失量占水田碳损失量的比例达80%;其次为占水田面积比例最大的潴育型水稻土,其碳损失量占水田碳损失量的15%.旱地土壤碳储量增长缓慢,完全来自于面积占96%的灰潮土有机碳密度的增长.因此,江汉平原区水田土壤有机碳的变化决定了农田土壤有机碳的整体动向,今后需着力提升有机碳下降迅速的低产水田以及面积较大的土壤类型的有机碳积累和固持能力.     

黄土丘陵区不同有机碳背景下侵蚀坡面土壤呼吸特征

以黄土丘陵区5个不同有机碳背景的坡面S型小区(坡顶为对照区、坡中为侵蚀区、坡脚为沉积区)为研究对象,通过对土壤呼吸速率的动态观测,分析坡面不同类型区土壤呼吸特征及其与土壤温湿度、有机碳和坡位的关系.结果表明,土壤温度的变化对沉积区土壤呼吸影响较大,土壤湿度的变化对侵蚀区土壤呼吸影响较大.有机碳是影响土壤呼吸的首要因子,可解释土壤呼吸变异的54.72%;其次是土壤湿度、坡位和土壤温度,分别可解释土壤呼吸变异的18.86%、16.13%和10.29%.侵蚀对坡面土壤呼吸的影响具有明显的原位和异位效应,侵蚀导致坡面侵蚀区土壤呼吸减小了21.14%,沉积区土壤呼吸增大了21.93%.侵蚀坡面土壤碳排放的源汇效应与有机碳水平有关,当土壤有机碳含量大于6.82 g·kg-1时,坡面侵蚀趋向于碳汇过程;当有机碳含量小于3.03 g·kg-1时,坡面侵蚀趋向于碳源过程.文中模型可以较好地反映有机碳和土壤温湿度与土壤呼吸的关系.     

温度对厨余垃圾两相厌氧消化中水解和酸化过程的影响

实验考查了厨余垃圾在4个温度(25℃、37℃、40℃、50℃)条件下的水解率、挥发酸(VFA)产量和速率、乳酸产量和有机酸的组成.结果表明:温度对水解和酸化过程均有较大影响,在小于37℃范围内水解率和酸化率均随温度升高而增加,最大的VFA浓度在37℃下获得,达34.4g/L.超过37℃,酸化率下降而水解率继续增加,最大水解率在50℃下获得达82%.VFA中以甲酸和乙酸为主,并有少量丙酸和丁酸产生,同时乳酸浓度一直较高.通过实验确定了厨余垃圾水解酸化过程的最优温度条件为37℃.     

Successful Treatment of Low PAH-Contaminated Sewage Sludge in Aerobic Bioreactors (7 pp) *

Background, Aims and Scope Polycyclic Aromatic Hydrocarbons (PAHs) are known for their adverse and cumulative effects at low concentration. In particular, the PAHs accumulate in sewage sludge during wastewater treatment, and may thereafter contaminate agricultural soils by spreading sludge on land. Therefore, sludge treatment processes constitute the unique opportunity of PAH removal before their release in the environment. In this study, the ability of aerobic microorganisms to degrade light and heavy PAHs was investigated in continuous bioreactors treating trace-level PAH-contaminated sludge. Methods Several aerobic reactors were operated under continuous and perfectly mixed conditions to simulate actual aerobic sludge digesters. Three sterile control reactors were performed at 35°C, 45°C or 55°C to assess PAH abiotic losses under mesophilic and thermophilic conditions. Three biological reactors were also operated at 35°C, 45°C or 55°C. Furthermore, 250 mM methanol were added in an additional mesophilic reactor (35°C). All reactors were fed with long-term PAH-contaminated sewage sludge, and PAH removal was assessed by inlet/outlet mass balance. In this study, PAH compounds ranged from 2 to 5-unsubstituted aromatic rings, i.e. respectively from Fluorene to Indeno(123cd)pyrene. Results and Discussion Significant abiotic losses were observed for the lightest PAHs (fluorene, phenanthrene and anthracene), while biodegradation occurred for all PAHs. More than 80% of the lightest PAHs were removed. Biodegradation rates inversely correlated with the increasing molecular weight, and seemed limited by the low bioavailability of the heaviest PAHs (only 50% of removal). The enhancement of PAH bioavailability by increasing the process temperature or adding methanol was tested. A temperature increase from 35°C to 45°C and then to 55°C significantly enhanced the biodegradation of the heaviest PAHs from 50% to 80%. However, high abiotic losses were observed for all PAHs at 55°C, which was attributed to volatilization. Optimal conditions were found at 45°C considering the low abiotic losses and the high PAH biodegradation rates. Similar performances were achieved by addition of methanol in the sludge. It was concluded that increasing temperatures or addition of methanol favored PAH diffusion from solids to an aqueous compartment, and enhanced their bioavailability to PAH-degrading microorganisms. Conclusion In this study, the use of long-term acclimated aerobic ecosystems showed the high potential of aerobic microorganisms to degrade a wide range of PAHs at trace levels. However, PAH biodegradation was likely controlled by their low bioavailability. Two aerobic processes have been finally proposed to achieve efficient decontamination of sewage sludge, at 45°C or in the presence of methanol. The PAH concentrations in reactor outlet were lower than the French requirements, and allow the treated sludge to be spread on agricultural land. Recommendations and Outlook The two proposed aerobic processes used physical or chemical diffusing agents. The global ecological impact of using the latter agents for treating trace level contamination must be considered. Since methanol was completely removed during the process, no additional harm is expected after treatment. However, an increase of temperature to 45°C could drastically increase the energy demand in full-scale plants, and therefore the ecological impact of the process. Moreover, since bioavailability controls PAH biodegradation, efficiency of the processes could also be influenced by the hydraulic parameters, such as mixing and aeration rates. Further experimentations in a pilot scale are therefore recommended, as well as a final assessment of the global environmental benefit of using such aerobic processes in the bioremediation of trace level compounds. - Abbreviations (PAHs): Ant – anthracene; B(a)A – benzo(a)anthracene ; B(b)F – benzo(b)fluoranthene; B(k)F – benzo(k)fluoranthene; B(ghi)P – benzo(g,h,i)perylene; B(a)P – benzo(a)pyrene; Chrys – chrysene; DB – dibenzo(a,h)anthracene; Fluor – fluoranthene; Fluo - fluorene; Ind – indeno(1,2,3-c,d)pyrene; Phe - phenanthrene; Pyr – pyrene - * The basis of this peer-reviewed paper is a presentation at the 9th FECS Conference on 'Chemistry and Environment', 29 August to 1 September 2004, Bordeaux, France.     

Relevance for decision making of spatially explicit,participatory scenarios for ecosystem services in an area of a high current demand

Participatory ecosystem services scenarios can be used to inform decision making on the sustainable or wise use of biodiversity and ecosystem services (ES). To establish the plausibility and coherency of the recently constructed Biscay participatory scenarios, and to analyze policy options for improving sustainability of land use and the supply of ecosystem services, a spatially explicit analysis of land cover change was carried out. The modelling used an innovative methodology which included feedback from key stakeholders. Our study showed that scenario mapping can be a way of testing the credibility and internal consistency of scenarios, and a methodology for making them more coherent; it was also useful for highlighting land use trade-offs. The sustainability analysis for the ES supply side showed the benefits of promoting two land use/cover trends in the Biscay region: (i) an increase of sustainable arable land in the valley zones to reinforce biocapacity and self-provisioning while preserving agroecosystems’ ES flow; and (ii) natural forest regeneration in mountainous and other zones to increase carbon storage and sequestration while enhancing biodiversity and other ES flows. We argue that even if already protected public agro-forest lands may be the best places to start promoting these changes, additional measures are needed to involve private landowners and guarantee changes at a landscape level. Finally, we reflect on the need to make complementary analyses of ES supply and demand as a way of contributing to a broad sustainability agenda.     

Impact of Carbon Storage Through Restoration of Drylands on the Global Carbon Cycle

   Using estimates of land suitable for restoration in woodlands, grasslands, and deserts, as well as estimates of the rate at which restoration can proceed, we estimate that carbon storage in these biomes can range up to 0.8 billion tons of carbon per year (Gt C/yr), for a combination of land management strategies. This corresponds to a reduction in atmospheric buildup of 0.5 Gt C/yr, which represents up to 15% of the average annual atmospheric carbon buildup in the next century, 3.5 Gt C/yr, assuming the IPCC 92d scenario. A global strategy for reducing atmospheric carbon dioxide concentration will require the implementation of multiple options. The advantage of carbon storage in restored drylands is that it comes as a side benefit to programs that are also justifiable in terms of land management.     

应对二氧化碳浓度上升问题的研究:CO_2的捕获、储存与利用

为了缓解日益严重的CO2浓度升高导致的温室效应等环境问题,针对各国CO2过量排放与温室效应逐渐加剧的现状,讨论传统CO2减排方法与CO2的捕获、储存与利用(CCSU)的优缺点和优势互补,论述针对大型CO2排放点的减排措施——CCSU的必要性。对CCSU进行系统的介绍和认识,并对CCSU所包含的各种捕获技术、储存技术以及利用技术的特点进行对比和分析,论述其适用范围、地域和经济因素。结合国外一些现有的应用CO2的先进技术和经验,对CO2的捕获与利用的联用作出分析和展望。尤其是CO2的化工利用具有广阔的研发和发展前景,CO2EOR(CO2提高采收率技术)在技术和经济上具有实际应用意义。为新型环保型能源体系的建设提供参考。     

三江源地区1961~2005年气温极端事件变化

利用三江源地区11个气象台站1961~2005年逐日最高气温和最低气温资料，分析了三江源地区极端高温和极端低温的变化趋势。研究表明：近45年来，白天和夜间温度极端偏高的日数明显增多，分别以26 d/10 a和44 d/10 a速度在增加;白天和夜间温度极端偏低的日数显著减缓，分别以41 d/10 a和85 d/10 a的速度显著减少;年极端低温和极端高温分别以042℃/10 a和029℃/10 a的速度增加;白天和夜间温度极端偏高的日数增加主要发生在冬季和夏季，而白天和夜间温度极端偏低的日数减少主要发生在春季和秋季，夜间温度极端偏低的日数减少趋势最为明显;长江源地区极端气温变化对区域增温的响应更为敏感。