Effects of calcination temperature on physicochemical property and activity of CuSO4/TiO2 ammonia-selective catalytic reduction catalysts

CuSO_4/TiO_2 catalysts with high catalytic activity and excellent resistant to SO_2 and H_2 O,were thought to be promising catalysts used in Selective catalytic reduction of nitrogen oxides by NH_3.The performance of catalysts is largely affected by calcination temperature.Here,effects of calcination temperature on physicochemical property and catalytic activity of CuSO_4/TiO_2 catalysts were investigated in depth.Catalyst samples calcined at different temperatures were prepared first and then physicochemical properties of the catalyst were characterized by N2 adsorption-desorption,X-ray diffraction,thermogravimetric analysis,Raman spectra,Fourier-transform infrared spectroscopy,X-ray photoelectron spectroscopy,temperature-pro grammed desorption of NH_3,temperature-programmed reduction of H_2 and in situ diffuse reflectance infrared Fourier transform spectroscopy.Results revealed that high calcination temperature had three main effects on the catalyst.First,sintering and anatase transform into rutile with increase of calcination temperature,causing a decrement of specific surface area.Second,decomposition of CuSO_4 under higher calcination temperature,resulting in disappears of Br(?)nsted acid sites(S-OH),which had an adverse effect on surface acidity.Third,CuO from the decomposition of CuSO_4 changed surface reducibility of the catalyst and favored the process of NH_3 oxidation to nitrogen oxides(NO_x).Thus,catalytic activity of the catalyst calcined under high temperatures(≥600℃) decreased largely.     

Synergistic effects of Cu species and acidity of Cu-ZSM-5 on catalytic performance for selective catalytic oxidation of n-butylamine

In this work, a series of Cu-ZSM-5 catalysts with different SiO₂/Al₂O₃ ratios (25, 50, 100 and 200) were synthesized and investigated in n-butylamine catalytic degradation. The n-butylamine can be completely catalytic degradation at 350°C over all Cu-ZSM-5 catalysts. Moreover, Cu-ZSM-5 (25) exhibited the highest selectivity to N₂, exceeding 90% at 350°C. These samples were investigated in detail by several characterizations to illuminate the dependence of the catalytic performance on redox properties, Cu species, and acidity. The characterization results proved that the redox properties and chemisorption oxygen primarily affect n-butylamine conversion. N₂ selectivity was impacted by the Brønsted acidity and the isolated Cu²⁺ species. Meanwhile, the surface acid sites over Cu-ZSM-5 catalysts could influence the formation of Cu species. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra was adopted to explore the reaction mechanism. The Cu-ZSM-5 catalysts are the most prospective catalysts for nitrogen-containing volatile organic compounds removal, and the results in this study could provide new insights into catalysts design for VOC catalytic oxidation.     

牛粪-化肥配施对水稻田氮磷迁移转化的影响

在控制外源N输入量相同的前提下,通过田间小区实验,探讨有机肥与化肥不同施用量（牛粪施用量：5,10,20t/hm²）对稻田田间土-水界面氮磷迁移转化特征的影响.结果表明：控制稻田水中NH₄⁺-N、NO₃^--N、TN和TP输出的最佳时期分别为施肥后的第5,30,7,20d,且TN和TP浓度随时间变化符合单指数衰减方程（0.7444≤R²≤0.9724;1.1×10^-6≤F≤0.0055）.采用牛粪部分代替化肥的施肥方式,在一定范围内能降低稻田退水中TN、TP输出负荷（41.8%、36.0%、64.3%;20.3%、39.1%、48.9%）,还可以降低稻田水中N/P,降低水体富营养化风险.同时,牛粪的施用可提高土壤中脲酶和磷酸酶的含量,促进氮磷向植物可吸收形态转化.综合经济成本和生态效益核算,采用10t有机肥代替无机肥的处理是相对经济环保的施肥方法,该施肥方式下,氮磷年输出负荷分别为17.70,1.26kg/hm².     

Insights into reactive oxygen species formation induced by water-soluble organic compounds and transition metals using spectroscopic method

Ambient particulate matter (PM) can cause adverse health effects via their ability to produce Reactive Oxygen Species (ROS). Water-Soluble Organic Compounds (WSOCs), a complex mixture of organic compounds which usually coexist with Transition Metals (TMs) in PM, have been found to contribute to ROS formation. However, the interaction between WSOCs and TMs and its effect on ROS generation are still unknown. In this study, we examined the ROS concentrations of V, Zn, Suwannee River Fulvic Acid (SRFA), Suwannee River Humic Acid (SRHA) and the mixtures of V/Zn and SRFA/SRHA by using a cell-free 2′,7′-Dichlorodihydrofluorescein (DCFH) assay. The results showed that V or Zn synergistically promoted ROS generated by SRFA, but had an antagonistic effect on ROS generated by SRHA. Fluorescence quenching experiments indicated that V and Zn were more prone to form stable complexes with aromatic humic acid-like component (C1) and fulvic acid-like component (C3) in SRFA and SRHA. Results suggested that the underlying mechanism involving the fulvic acid-like component in SRFA more tending to complex with TMs to facilitate ROS generation through π electron transfer. Our work showed that the complexing ability and complexing stability of atmospheric PM organics with metals could significantly affect ROS generation. It is recommended that the research deploying multiple analytical methods to quantify the impact of PM components on public health and environment is needed in the future.     

Identification of weather patterns impacting 24-h average fine particulate matter pollution

Methods are presented to extract intra-seasonal meteorological patterns at three scales to explain 24-h fine particulate matter (PM_2.5) pollution events: evolving large-scale meteorological scenarios, synoptic regimes driving diurnal variability near the surface, and localized meteorological triggers. The methods were applied to understand how winter weather conditions impacted PM_2.5 around the San Francisco Bay Area (SFBA). Analyzing data across 12 winters (November–March) ensured robust characterization of the SFBA conditions. SFBA 24-h PM_2.5 exceedances (35 μg m^?3) required several simultaneous characteristics: a ridge of aloft high pressure moving over SFBA, providing weak surface pressure gradients over Central California; persistent easterly flows through SFBA extending vertically to around the 925-hPa pressure level; orographically channeled winds resulting from stability; enhanced nocturnal cooling under clear-sky conditions providing for enhanced drainage flows off the Central California slopes; and at least two consecutive days of these conditions.     

模拟升温对冰川前缘地微生物种群的影响

由于全球变暖影响,冰川处于不断退缩状态.本研究以天山乌鲁木齐河源1号冰川前缘地3个不同退缩年代的土样为研究对象,设置2个温度处理,分别为5℃与15℃,通过150d室内培养实验,探讨升温对冰川前缘地微生物种群的影响.结果表明,在原始样品中,随土壤样品退缩年代的增加,土壤总碳氮含量增加,微生物的数量及α多样性增加. 150d培养实验结果表明:细菌、古菌拷贝数随升温发生变化,但改变未达显著水平.此外,升温改变微生物群落结构,且对不同样点微生物群落结构影响不同.通过对升温后变化显著的优势OTUs进行分析,退缩年代较短的样点对升温响应更为明显,主要表现为Thiobacillus属相对丰度的升高.结果表明,冰川前缘地微生物对变暖响应的土壤异质性,其结果可为高山冰川地区升温下微生物的特征变化提供参考信息.     

Arsenic redox transformation by Pseudomonas sp. HN-2 isolated from arsenic-contaminated soil in Hunan, China

A mesophilic,Gram-negative,arsenite[As(Ⅲ)]-oxidizing and arsenate[As(V)]-reducing bacterial strain,Pseudomonas sp.HN-2,was isolated from an As-contaminated soil.Phylogenetic analysis based on 16 S r RNA gene sequencing indicated that the strain was closely related to Pseudomonas stutzeri.Under aerobic conditions,this strain oxidized 92.0%(61.4 μmol/L) of arsenite to arsenate within 3 hr of incubation.Reduction of As(V) to As(Ⅲ) occurred in anoxic conditions.Pseudomonas sp.HN-2 is among the first soil bacteria shown to be capable of both aerobic As(Ⅲ) oxidation and anoxic As(V) reduction.The strain,as an efficient As(Ⅲ) oxidizer and As(V) reducer in Pseudomonas,has the potential to impact arsenic mobility in both anoxic and aerobic environments,and has potential application in As remediation processes.     

中国粮食作物产量和木本植物生物量与地表臭氧污染的响应关系

当前我国地表臭氧（O₃）污染日趋严重,对植物生产力构成了严重威胁.本文综述了粮食作物产量和木本植物生物量与O₃暴露水平指标M7（7 h平均O₃浓度,09：00~16：00）、SUM06（每小时O₃浓度大于60 nmol·mol^-1的累积值）、W126（每小时O₃浓度在特定时段内用Sigmoidal函数加权求和值）、POD_Y［每小时气孔O₃通量高于阈值Y nmol·（m²·s）^-1的累积吸收通量］和最常用的AOT40（每小时O₃浓度超过40 nmol·mol^-1部分的累积值）之间的响应关系,并计算了相应的损伤阈值.基于AOT40的结果表明,导致水稻、冬小麦、玉米和大豆产量下降5%的O₃风险阈值分别为5.93、2.69、8.67和4.17 μmol·mol^-1·h,说明我国玉米对O₃的耐受性可能要高于其它3种作物;对于木本植物,杨树5个品种的熏蒸实验和17种木本植物的整合分析的结果显示,导致其总生物量减少5%的O₃风险阈值分别为12.20 μmol·mol^-1·h和10.87 μmol·mol^-1·h.此外,提出了未来相关研究应关注建立植物其它重要参数与O₃污染的响应关系与提高O₃区域风险评估精度,同时需要重点考虑如何将影响植物O₃敏感性的重要因子（如土壤氮素和树龄等）耦合到区域评估模型中.     

我国厨余垃圾资源化技术的多维绩效评价

随着我国大力推动生活垃圾分类管理工作,厨余垃圾的资源化利用受到越来越多关注.厨余垃圾资源化技术已有包括厌氧消化处理、好氧生物处理和昆虫饲料转化等类型,但在已有应用案例中存在资源化程度低、环境影响显著和经济效益差等诸多问题,缺乏技术绩效的系统化分析和综合性评价.为此,研究面向厨余垃圾资源化技术应用的全生命周期过程,构建了资源效率、环境影响、经济可行和社会效应的多维绩效评价指标体系(包括21项指标),以我国的14项典型技术应用项目为案例开展定量化综合评价研究.结果表明,厌氧消化和昆虫饲料转化处理技术的得分分别为58.39分和59.65分,高于好氧生物处理(49.16分);按细分技术类型,集中式黑水虻转化和中温湿式厌氧工艺得分较高,分别为67.14分和60.82分.按技术的处理规模和设施分布方式,集中式处理技术在资源效率和经济效益维度上分别比分散式技术高出13%和62%;分散式处理技术在环境影响和社会效应维度上比集中式高出8%和34%.在厨余垃圾资源化实践中,应结合当地的厨余垃圾理化性质、生活垃圾分类收集工作推进情况、财政承担能力和收运距离等多因素综合考量,因地制宜的选择适宜技术路线.     

肠道微生物对土壤中铜、锌、锰生物可给性的影响

为了更全面、准确地评价土壤中金属元素对人体的健康风险,研究土壤中金属元素在结肠阶段的生物可给性具有重要意义。通过采集我国一些地区的6种土壤,利用in vitro方法(PBET和SHIME联用)研究土壤中Cu、Zn、Mn在胃、小肠、结肠阶段的生物可给性。研究显示,土壤中Cu、Zn、Mn在胃阶段的生物可给性分别为23.8%~63.0%、21.2%~64.4%、11.7%~35.6%;从胃阶段到小肠阶段,土壤中Cu的生物可给性提高了0.4%~14.4%,而土壤中Zn在小肠阶段的生物可给性降低了6.7%~38.7%。结肠阶段,土壤中Cu、Zn、Mn的生物可给性分别为2.4%~12.9%、5.7%~18.7%、6.2%~18.9%,与小肠阶段相比,分别降低了21.7%~56.9%、0.4%~36.8%、4.5%~19.1%。结果表明,在肠道微生物存在的情况下,土壤中Cu、Zn、Mn在结肠阶段有较低的人体健康风险。