Co负载量对Co/TiZrO4催化CO2氧化乙烷脱氢制乙烯反应性能的影响

Co基催化剂在低碳烷烃直接脱氢及氧化脱氢制烯烃方面表现出良好的应用潜力.为了探究Co物种的价态对CO₂氧化乙烷脱氢制乙烯的影响,以共沉淀法制备的TiZrO₄固溶体为载体,采用浸渍法制备了一系列X%Co/TiZrO₄(X=0.5、1、3、5和7.5)催化剂.结果表明,0.5%Co/TiZrO₄和1%Co/TiZrO₄催化剂的催化活性较差,但保持了相当高的C₂H₄选择性(>90%)和碳平衡(≈100%);3%Co/TiZrO₄催化剂在反应过程中表现出良好的C₂H₆和CO₂活化能力,在650℃、质量空速WHSV=9000 mL?g^-1?h^-1的反应条件下获得了约25%的乙烯收率;而5%Co/TiZrO₄和7.5%Co/TiZrO₄催化剂则在600℃及以上温度反应...     

两种生物炭对稻米中砷累积的影响研究

为探究土壤添加低剂量生物炭对稻米中砷累积的影响及作用机理,使用矿区砷污染土壤添加小麦和棉花秸秆生物炭进行盆栽和模拟试验.盆栽试验结果表明:添加质量分数为0.5％的低剂量小麦和棉花秸秆生物炭,可以降低稻米(糙米)砷浓度(约10％),作用有限.糙米中砷浓度的降低主要是由于其生物量增加所致.模拟试验结果表明:添加质量分数为1％?—?5％的高剂量生物炭可以显著促进土壤中砷释放,相比对照组,生物炭添加组土壤溶液中砷浓度增加了69％?—?243％,推测其可能是生物炭促进了微生物作用下铁氧化物的还原,进而导致砷释放.研究表明:土壤中施加低剂量小麦和棉花秸秆生物炭对减少水稻砷累积作用可能有限,而高剂量可能增加水稻砷污染健康风险.     

拉萨市垃圾焚烧飞灰重金属特性分析及风险评价

焚烧是城市垃圾处理主流技术,飞灰作为垃圾焚烧主要污染物成为垃圾焚烧污染控制关键环节。采集拉萨市垃圾焚烧发电厂飞灰样品,分析了飞灰中重金属含量及浸出毒性特征,并采用改进的潜在风险评价法及健康风险评价法评价飞灰中重金属的潜在风险。结果表明:拉萨市飞灰中重金属含量较高,且Pb的浸出浓度超过GB 5085.3-2007《危险废物鉴别标准 浸出毒性鉴别》浸出液最高允许值的16倍。污染评价结果表明,拉萨市飞灰中Pb对环境具有极强的污染风险。健康风险评价结果表明,飞灰中重金属对人体的致癌风险在可接受范围内,但其非致癌风险值高于美国国家环境保护局(EPA)推荐的非致癌风险值(HQ ≤ 1),对人体具有较高的非致癌风险。其中 Pb对成人和儿童的非致癌风险值分别为3.8975和9.7458,是非致癌风险的主要贡献者。     

New mechanism of FA in composted sludge inducing Cu fixation on Albite in open-pit mine soil

Fulvic acid (FA), typical organic matter derived from humification process in composted sludge, possesses the potential to remediate mine soils contaminated by heavy metals. To understand the cooper (Cu) immobilizing process in open-pit mine soil induced by FA, changes of Cu speciation in mixture of open-pit mine soil and composted sludge was tracked over 180 days. It was observed that the organic-bound and residual fraction of Cu increased dramatically with the corresponding decrease of Fe/Mn oxide-bound Cu in the first 60 days, then the organic-bound fraction decreased to about its initial proportion during 60-120 days, while residual fraction still increased, and the proportion of residual Cu accounted for over 85% and became stable after 120 days. To reveal the mechanism of FA inducing Cu fixation on Albite which is the main phase of soil primary ore, two groups of Cu adsorption experiments with and without FA were designed. With the addition of FA, the adsorption capacity of Cu by Albite increased by 1.55 times and the content of residual Cu in Albite increased by 7.7 times. It was found that the Cu absorbed in smaller Albite particle induced by FA formed a secondary mineral——Chrysocolla, causing increase of residual fraction of Cu. These results revealed the mechanism: FA was absorbed on the surface of Albite after complexing with Cu ions in the solution, and then it induced Cu into the interlayer and pore channels of Albite. The Cu in the Albite was immobilized by forming Chrysocolla finally.     

硒和生物炭联合施用降低稻米甲基汞累积的研究

汞矿区土壤汞污染是造成水稻及其他作物中汞累积的主要原因,尤其是稻米中甲基汞的累积已成为当地居民甲基汞暴露的重要途径之一。本文针对含汞废水排放所造成的稻田汞污染情形,分别进行了模拟实验和盆栽试验,探究无机硒、生物炭、硒和生物炭联合施用对降低稻米甲基汞累积的作用效果。结果表明,无论向土壤中添加无机硒,还是生物炭,抑或是两者的组合均能有效降低土壤中甲基汞含量,且随着硒添加量的增加,其相应处理组土壤甲基汞含量不断降低。盆栽试验表明稻米中甲基汞含量因硒或生物炭的添加降低62%～73%（硒处理）、88%（生物炭处理）和90%～91%（硒+生物炭处理）,表明了硒和生物炭共同施用的作用效果要好于单独施用硒的作用效果。这种效果可能与生物炭降低了土壤中甲基汞的生物可利用性有关。总之,本研究为原位修复控制稻田汞污染风险提供了可能途径。     

Low nutrient levels as drinking water conditions can reduce the fitness cost of efflux pump-mediated ciprofloxacin resistance in Pseudomonas aeruginosa

The long-term persistence of antibiotic resistance in the environment, especially in drinking water, is a public health concern. Expression of an efflux pump, an important mechanism of resistance to antibiotics, usually confers a fitness cost in bacteria. In this study, we aimed to determine why antibiotic resistance conferred by overexpression of an efflux pump persisted in low-nutrient environments(TOC 10 mg/L) such as drinking and source water in which antibiotic selective pressure might be very low or even absent.Competition experiments between wild-type Pseudomonas aeruginosa and ciprofloxacinresistant mutants revealed that the fitness cost of ciprofloxacin resistance significantly decreased(p 0.05) under low-nutrient(0.5 mg/L total organic carbon(TOC)) relative to high-nutrient(500 mg/L TOC) conditions. Mechanisms underlying this fitness cost were analyzed. The mexD gene expression in resistant bacteria(cip_3 strain) was significantly lower(p 0.05) in low-nutrient conditions, with 10 mg/L TOC((8.01 ± 0.82)-fold), than in high-nutrient conditions, with 500 mg/L TOC((48.89 ± 4.16)-fold). Moreover, rpoS gene expression in resistant bacteria((1.36 ± 0.13)-fold) was significantly lower(p 0.05) than that in the wild-type strain((2.78 ± 0.29)-fold) under low-nutrient conditions(10 mg/L TOC),suggesting a growth advantage. Furthermore, the difference in metabolic activity between the two competing strains was significantly smaller(p 0.05) in low-nutrient conditions(5 and 0.5 mg/L TOC). These results suggest that nutrient levels are a key factor in determining the persistence of antibiotic resistance conferred by efflux pumps in the natural environment with trace amounts or no antibiotics.     

Novel chitosan–ethylene glycol hydrogel for the removal of aqueous perfluorooctanoic acid

It is urgent to explore an effective removal method for perfluorooctanoic acid (PFOA) due to its recalcitrant nature. In this study, a novel chitosan-based hydrogel (CEGH) was prepared with a simple method using chitosan and ethylene glycol through a repeated freezing–thawing procedure. The adsorption of PFOA anions to CEGH agreed well to the Freundlich–Langmuir model with a maximum adsorption capacity as high as 1275.9?mg/g, which is higher than reported values of most adsorbents for PFOA. The adsorption was influenced by experimental conditions. Experimental results showed that the main removal mechanism was the ionic hydrogen bond interaction between carbonyl groups (COO^?) of PFOA and protonated amine (NH⁺) of the CEGH adsorbent. Therefore, CEGH is a very attractive adsorbent that can be used to remove PFOA from water in the future.     

Preparation of Ti species coating hydrotalcite by chemical vapor deposition for photodegradation of azo dye

TiO_2 in anatase crystal phase is a very effective catalyst in the photocatalytic oxidation of organic compounds in water. To improve its photocatalytic activity, the Ti-coating Mg Al hydrotalcite(Ti–Mg Al–LDH) was prepared by chemical vapor deposition(CVD) method.Response surface method(RSM) was employed to evaluate the effect of Ti species coating parameters on the photocatalytic activity, which was found to be affected by the furnace temperature, N2 flow rate and influx time of precursor gas. Application of RSM successfully increased the photocatalytic efficiency of the Ti–Mg Al–LDH in methylene blue photodegradation under UV irradiation, leading to improved economy of the process.According to the results from X-ray diffraction, scanning electron microscopy, Brunner–Emmet–Teller and Barrett–Joyner–Hallender, thermogravimetric and differential thermal analysis, UV–vis diffuse reflectance spectra analyses, the Ti species(TiO_2or/and Ti~(4+)) were successfully coated on the Mg Al–LDH matrix. The Ti species on the surface of the Ti–Mg Al–LDH lead to a higher photocatalytic performance than commercial TiO_2-P25. The results suggested that CVD method provided a new approach for the industrial preparation of Ti-coating Mg Al–LDH material with good photocatalytic performances.     

基于复合软电离源飞行时间质谱的小型化大气非甲烷烃在线快速监测系统的设计与应用

针对大气非甲烷烃(NMHCs)的时空分布监测需求,并弥补现有监测技术时间分辨率低、体积和功耗较大的不足,本研究自主研发出一套高性能、小型化的大气非甲烷烃在线快速测量系统.该方法基于串联吸附剂在特定温度下对目标物质的富集与解吸,采用单光子/化学复合软电离源飞行时间质谱(SPI/CI-TOFMS)作为分离和检测手段,实现对C_2～C_(10)挥发性有机物的快速分离和检测.通过对标准样品的测量表明:在SPI/CI模式下,C_2～C_(10)物种工作曲线(0～10×10~(-9))拟合优度R~20.99,大部分物种方法检出限为1×10~(-12)～80×10~(-12),仪器检出限为1×10~(-12)～35×10~(-12),RSD(n≥10)小于10%.将仪器初步应用于北京大学站点进行定点观测,测量结果与商业化仪器TH-300B离线分析结果吻合.本系统样品分析时间5～12 min可调,整机重量低于40 kg,整机尺寸小于50 cm×50 cm×80 cm,功率低于500 W,可满足大气非甲烷烃的快速监测需求,为提供高分辨率大气NMHCs时空分布数据提供技术支持.