稀土修饰的Co/Hβ催化剂催化分解N_2O

以Hβ分子筛为载体,采用浸渍法制备了一系列以钴为主活性组分,稀土元素为助剂的CoM/Hβ（M=La、Ce、Pr、Nd）催化剂,考察了在含氧条件下直接催化分解N2O的性能.采用X射线衍射、热重-质谱联用系统、H2-TPR、NH3-TPD等方法对催化剂进行了表征.XRD结果表明,Co物种主要以Co3O4尖晶石形态存在.NH3-TPD结果表明,催化剂活性与催化剂的酸性有关.活性评价结果显示,稀土助剂的添加使催化剂活性得到改善,其中以Pr为助剂的催化剂活性最好,N2O转化率达到95%时的反应温度为398℃.     

水体中金属(氧化物)纳米颗粒的环境行为与污染控制研究进展

金属(氧化物)纳米材料在生产和使用过程中,可以通过各种途径进入到水环境中,对水生生物、生态环境和人体健康产生威胁.理解纳米颗粒在水体中的环境行为,对于评估纳米材料的归趋及其对环境和人体的健康风险至关重要.本文概述了金属(氧化物)纳米颗粒的性质、来源和毒性危害,汇总了表征纳米颗粒浓度、粒径及形貌的分析方法与技术,分析了它...     

An inventory of N(2)O emissions from agriculture in China using precipitation-rectified emission factor and background emission

Fertilized agricultural soils are a major anthropogenic source of atmospheric N₂O. A credible national inventory of agricultural N₂O emission would benefit its global strength estimate. We compiled a worldwide database of N₂O emissions from fertilized fields that were consecutively measured for more than or close to one year. Both nitrogen input (N) and precipitation (P) were found to be largely responsible for temporal and spatial variabilities in annual N₂O fluxes (N₂O–N). Thus, we established an empirical model (N₂O–N = 1.49 P + 0.0186 P · N), in which both emission factor and background emission for N₂O were rectified by precipitation. In this model, annual N₂O emission consists of a background emission of 1.49 P and a fertilizer-induced emission of 0.0186 P · N. We used this model to develop a spatial inventory at the 10 × 10 km scale of direct N₂O emissions from agriculture in China. N₂O emissions from rice paddies were separately quantified using a cropping-specific emission factor. Annual fertilizer-induced N₂O emissions amounted to 198.89 Gg N₂O–N in 1997, consisting of 18.50 Gg N₂O–N from rice paddies and 180.39 Gg N₂O–N from fertilized uplands. Annual background emissions and total emissions of N₂O from agriculture were estimated to be 92.78 Gg N₂O–N and 291.67 Gg N₂O–N, respectively. The annual direct N₂O emission accounted for 0.92% of the applied N with an uncertainty of 29%. The highest N₂O fluxes occurred in East China as compared with the least fluxes in West China.     

Regional-specific emission inventory for NH3, N2O, and CH4 via animal farming in South, Southeast, and East Asia

Ammonia, nitrous oxide, and methane emission from animal farming of South, Southeast, and East Asia, in 2000, was estimated at about 4.7 Tg NH₃–N, 0.51 Tg N₂O–N, and 29.9 Tg CH₄, respectively, using the FAO database and countries’ statistic databases as activity data, and emission factors taking account of regional characteristics. Most of these atmospheric components, up to 60–80%, were produced in China and India. Pakistan, Bangladesh, and Indonesia, which were large source countries next to China and India, contributed more than a few percent of total emission of each atmospheric component. The largest emission livestock were cattle whose contribution was considerably high in South, Southeast, and East Asia; more than one-fourth of ammonia and nitrous oxide emissions: more than half of methane emission. The other major livestock for nitrous oxide and ammonia emissions were pigs. For methane emission, buffaloes were second source livestock. To provide spatial distributions of these gases, the emissions of county and district level were allocated into each 0.5° grid by means of the weighting by high-resolution land cover datasets. The regions with considerable high emissions of all components were able to be found at the Ganges delta and the Yellow River basin. The spatial distributions for ammonia and nitrous oxide emissions were similar but had a substantial difference from methane distribution.     

生物矿化针铁矿吸附铬的机理探讨

针铁矿在自然界中广泛存在,对重金属离子在地表的迁移和转化有重要影响.利用天然生物矿化针铁矿进行了Cr(Ⅲ)吸附研究,并利用扫描电子显微镜(SEM)和X射线光电子能谱(XPS)等对吸附后的样品进行表征,发现样品中铬的含量随着Al2O3含量的增加而增加,说明表面带负电荷的含高岭土等的粘土较针铁矿对Cr(Ⅲ)有更强的吸附能力.样品的XPS研究表明,NO3-也参与了反应,且促进了Cr(Ⅲ)的氧化.研究还发现,Cr(Ⅲ)在针铁矿上的吸附不均匀,与文献报道的情况不同.     

SIMP钢在高温液态铅铋合金中的腐蚀行为

目的 研究SIMP钢在不同溶解氧浓度的高温液态铅铋合金中长期浸泡后腐蚀产物的变化规律。方法 在550 ℃静态液态铅铋合金(饱和氧状态和贫氧状态)中对SIMP钢进行500、1 000、2 000、3 500、5 000 h的腐蚀试验。通过观察腐蚀后试样的表面和截面形貌,进行物化分析,对比不同时间下腐蚀层厚度以及腐蚀产物结构的变化,得出溶解氧浓度和浸泡时间的变化对腐蚀产物的影响规律。结果 在贫氧环境中,SIMP钢的腐蚀类型主要为氧化腐蚀,氧化腐蚀产物具有双层结构,外层为Fe-Cr尖晶石氧化层,内层为富铬氧化物与基体的混合物层;在饱和氧环境,SIMP钢腐蚀产物则具有3层结构,外层为Fe3O4磁铁矿层,中层为Fe-Cr尖晶石氧化层,最内层为富铬氧化物与基体的混合物层。结论 溶解氧浓度和浸泡时间的变化对腐蚀产物的结构和厚度产生了显著影响,SIMP钢在贫氧环境中呈现出优异的耐腐蚀性能。     

Nb掺杂对CeO2-SnO2催化剂NH3-SCR活性的促进作用

NH₃选择性催化还原 (NH₃-SCR) 是柴油车尾气NO_x净化的主流技术。将Nb引入CeO₂-SnO₂得到了一种新型的CeSnNbO_x金属氧化物催化剂,考察了Nb掺杂对催化剂结构、元素价态、活性位点、氧化还原性能、表面酸性和吸附性能的影响,并结合BET、XRD、XPS、H₂-TPR、NH₃-TPD和in situ DRIFTS等多种表征手段明确了Nb对该催化剂活性的促进作用。结果表明,Ce₁Sn₂Nb₁O_x催化剂表现出最佳活性,在温度为250~500 ℃时,达到接近100%的NO_x转化率。Nb掺杂改善了催化剂的比表面积和总孔体积,合理调控了催化剂表面酸性和氧化还原性能。此外,催化剂表面高度分散的Nb物种可能与Ce物种耦合形成新的Ce-O-Nb活性位点,有助于催化剂NH₃-SCR性能的提升。本研究可为开发高效Ce基氧化物催化剂提供参考。     

金属盐改性活性氧化镁对饮用水中氟离子的去除性能

饮用水中氟含量超标会损害人体的健康,本研究研制了一种改性吸附剂用于去除饮用水中过量的氟离子。本研究采用浸渍,焙烧的方法将金属盐负载到活性氧化镁上,制备改性活性氧化镁,考察了其除氟效果和吸附除氟的主要影响因素。结果表明,经过钙盐,铁盐改性后的活性氧化镁最大吸附容量显著增加,在复杂水体环境中仍有突出的除氟效果;改性吸附剂适宜pH为3~10;金属盐改性活性氧化镁处理水样不会有Mg²⁺和浸渍盐离子溶出,是一种安全可靠的吸附除氟材料。     

纳米金属对污水处理系统中磺胺耐药基因和耐药菌的影响及其机理

细菌耐药性和纳米材料污染为新兴环境问题。细菌耐药性遗传载体——耐药基因 (ARGs) 广泛存在于污水处理系统中,且已被证明与金属纳米材料密切相关。采用实时荧光定量PCR技术,探究了纳米零价铁 (nZVI) 和纳米氧化锌 (nZnO) 对污水处理系统中磺胺类耐药菌 (ARB) 和ARGs的分布特征的影响。结果表明,50 mg·L⁻¹ nZVI和nZnO暴露均有利于削减磺胺ARB浓度数。与对照组相比,nZVI和nZnO暴露后污泥中sul1丰度增加了0.25%~16.21%,而sul2出现明显削减 (1.51%~15.47%) 。此外,50 mg·L⁻¹ nZVI会导致游离态胞外ARGs大幅削减。nZVI和nZnO暴露通过富集污水处理系统中的intI1、改变细胞膜通透性和调节细菌转录能力促进sul1的增殖。本研究结果阐明了典型纳米金属对污水处理系统中ARB和不同形态ARGs消长的影响及其机制,可为制定有效调控和全面削减污水处理系统中耐药污染策略提供参考。     

pH对污水好氧处理过程N2O产生的影响

采用能够同时监测气态和溶解态N2O功能的污水好氧处理过程模拟装置,研究了不同pH条件下氨氧化细菌(AOB)好氧反硝化途径N2O的产生特点、污染物转化过程、胞内聚合物聚羟基脂肪酸酯(PHA)含量的变化以及它们之间的内在联系。结果表明,pH在6.5~8.0范围内,N2O产生量随pH的升高而减小。pH较低时,氧化亚氮还原酶活性受到抑制,导致好氧反硝化过程中产生的N2O大量积累并逸散;随着pH得升高,氧化亚氮还原酶活性增强,N2O产生量随之减少。