Density functional theory (DFT) studies of vanadium-titanium based selective catalytic reduction (SCR) catalysts

Based on density functional theory (DFT) and basic structure models, the chemical reactions on the surface of vanadium-titanium based selective catalytic reduction (SCR) denitrification catalysts were summarized. Reasonable structural models (non-periodic and periodic structural models) are the basis of density functional calculations. A periodic structure model was more appropriate to represent the catalyst surface, and its theoretical calculation results were more comparable with the experimental results than a non-periodic model. It is generally believed that the SCR mechanism where NH₃ and NO react to produce N₂ and H₂O follows an Eley-Rideal type mechanism. NH₂NO was found to be an important intermediate in the SCR reaction, with multiple production routes. Simultaneously, the effects of H₂O, SO₂ and metal on SCR catalysts were also summarized.     

Recent advances in catalytic decomposition of ozone

Ozone (O₃), as a harmful air pollutant, has been of wide concern. Safe, efficient, and economical O₃ removal methods urgently need to be developed. Catalytic decomposition is the most promising method for O₃ removal, especially at room temperature or even subzero temperatures. Great efforts have been made to develop high-efficiency catalysts for O₃ decomposition that can operate at low temperatures, high space velocity and high humidity. First, this review describes the general reaction mechanism of O₃ decomposition on noble metal and transition metal oxide catalysts. Then, progress on the O₃ decomposition performance of various catalysts in the past 30 years is summarized in detail. The main focus is the O₃ decomposition performance of manganese oxides, which are divided into supported manganese oxides and non-supported manganese oxides. Methods to improve the activity, stability, and humidity resistance of manganese oxide catalysts for O₃ decomposition are also summarized. The deactivation mechanisms of manganese oxides under dry and humid conditions are discussed. The O₃ decomposition performance of monolithic catalysts is also summarized from the perspective of industrial applications. Finally, the future development directions and prospects of O₃ catalytic decomposition technology are put forward.     

基于边介数的省域生态廊道构建方法优化

我国城市建设和生态保护工作均对土地资源有大量需求,二者之间的矛盾在经济优先发展区表现尤为明显.为了有效地改善生态环境,管控土地利用并引导其变化发展,需要建设具备不可替代特征的省域生态廊道.最小累积阻力模型（minimum cumulative resistance,MCR）是识别生态廊道最常用、有效的模型,但在应用于省域尺度时,MCR模型识别的潜在廊道路由存在冗余的问题.因此,通过引入网络科学中的边介数指数（edge-betweenness）对MCR模型进行优化,计算潜在廊道路由的边介数指数值,选取出其中最为重要和简明的结构来连通生态源地,即提取潜在路由中的骨干路由（backbone route）和关键战略点（key strategic point）作为不可替代的结构来指导省域生态廊道建设.将优化后的MCR模型应用于广东省,构建了全长5 493 km的省域生态廊道,其中包含生态源地20处,关键战略点11个,骨干生态廊道29条.骨干路由与关键战略点构成的不可替代省域生态廊道（irreplaceable provincial corridor）能够实现"廊道数量和占地面积最少、连通性基本不变"的目标.研究显示,边介数能够对潜在路由进行优化筛选,识别出维护省域生态安全的关键结构;不可替代生态廊道能够指导省域生态规划和土地空间的发展利用,并为更高水平的生态安全环境提供了演进的基础;同时也为土地资源紧张的地区提供了建设生态廊道的参考与依据.      

Coupling mechanism of activated carbon mixed with dust for flue gas desulfurization and denitrification

To clarify the effect of coking dust, sintering dust and fly ash on the activity of activated carbon for various industrial flue gas desulfurization and denitrification, the coupling mechanism of the mixed activated carbon and dust was investigated to provide theoretical reference for the stable operation. The results show that coking dust had 34% desulfurization efficiency and 10% denitrification efficiency; correspondingly, sintering dust and fly ash had no obvious desulfurization and denitrification activities. For the mixture of activated carbon and dust, the coking dust reduced the desulfurization and denitrification efficiencies by blocking the pores of activated carbon, and its inhibiting effect on activated carbon was larger than its own desulfurization and denitrification activity. The sintering dust also reduced the desulfurization efficiency on the activated carbon while enhancing the denitrification efficiency. Fly ash blocked the pores of activated carbon and reduced its reaction activity. The reaction activity of coking dust mainly came from the surface functional groups, similar to that of activated carbon. The reaction activity of sintering dust mainly came from the oxidative property of Fe₂O₃, which oxidized NO to NO₂ and promoted the fast selectively catalytic reduction (SCR) of NO to form N₂. Sintering dust was activated by the joint action of activated carbon, and both had a coupling function. Sintering dust enhanced the adsorption and oxidation of NO, and activated carbon further promoted the reduction of NO_x by NH₃; thus, the denitrification efficiency increased by 5%-7% on the activated carbon.     

Chemical characteristics of road dust PM2.5 fraction in oasis cities at the margin of Tarim Basin

In order to understand the compositions characteristics of particulate matter with aerodynamic diameter less than 2.5 μm (PM_2.5) fraction in road dust (RD_2.5) of oasis cities on the edge of Tarim Basin, 30 road dust (RD) samples were collected in Kashi, Cele, and Yutian in the spring, 2018, and RD_2.5 was collected using the resuspension approach. Eight water-soluble ions, 39 trace elements and 8 fractions of carbon-containing species in PM_2.5 were analyzed. Ca²⁺ and Ca were the most abundant ions and elements in RD_2.5 (7.1% and 9.5%). Cl^- in RD_2.5 was affected not only by attributed to saline-alkali soils in oasis cities of the Tarim Basin and dust from Taklimakan Desert but also by human activities. Moreover, the organic carbon/elemental carbon (OC/EC) ratio indicated that carbon components in RD_2.5 in Cele town mainly come from fossil fuel combustion, while those in Yutian and Kashi mainly come from biomass combustion. It is noteworthy that high Ca in RD_2.5 was seriously affected by anthropogenic emissions, and high Na and K contents in RD_2.5 could be derived from soil and desert dust. It was estimated that Cd, Tl, Sn and Cr were emitted from anthropogenic emissions using the enrichment factor. The coefficients of divergence (COD) result indicated that the influence of local emission on road dust emission is greater than that of long-distance transmission. This study is the first time to comprehensively analyze the chemical characteristics of road dust in oasis cities, and the results provides the sources of road dust at the margin of Tarim Basin.     

外加氮源影响下铁铝氧化物在土壤氮素转化中的作用

土壤中铁铝氧化物在团聚体稳定性和有机碳吸附方面具有重要作用,而氮添加对土壤氮循环影响的变化也可能与其有关,但是目前尚缺乏在氮循环方面的研究.为了探究铁铝氧化物在土壤氮素转化中的作用,选择福建省建瓯罗浮栲森林土壤为研究对象,采用选择性溶提技术准备不同的土壤——未经处理（T1）的土壤和去除游离态铁铝氧化物（T2）土壤、去除非晶质铁铝氧化物（T3）土壤、去除络合态铁铝氧化物（T4）土壤,在这些土壤中添加不同形态氮（40 mg/kg）——丙氨酸（氨基酸态氮,AA）、硫酸铵（铵态氮,AN）、硝酸钠（硝态氮,NAN）和亚硝酸钠（亚硝态氮,NIN）,进行室内培养试验,分析氮含量变化和氮素转化情况.结果表明:①与CK处理相比,AA和AN处理均增加了T1土壤中w（NH₄+-N）,NAN处理增加了w（NO₃--N）,但低于添加量,表明添加氨基酸和铵态氮均会促进氮矿化,添加硝态氮会增加NO₃--N的固定且抑制其硝化.②在CK处理下,与T1土壤相比,T2和T4土壤中w（NH₄+-N）、w（NO₃--N）和w（氨基酸）均降低,但T3土壤中w（NH₄+-N）和w（氨基酸）增加、w（NO₃--N）降低,表明土壤中游离态氧化铁铝和络合态氧化铁铝的存在有助于氮素矿化,非晶质氧化铁铝有助于硝化.③在不同氮处理下,各土壤的氮含量及其转化速率与CK处理规律相似.与CK处理相比,各氮处理均未显著增加T2和T4土壤中w（NH₄+-N）,且AA和AN处理均未影响T2、T3和T4土壤中w（NO₃--N）和w（氨基酸）.结果显示,氮添加并没有改变铁铝氧化物的作用,其中,矿化和氨化作用均表现为游离氧化铁铝>络合氧化铁铝>非晶质氧化铁铝,硝化作用表现为非晶质氧化铁铝>游离氧化铁铝>络合态氧化铁铝.因此,土壤铁铝氧化物的不同存在状态应该是调节氮素转化的重要土壤条件.      

餐厨垃圾生物有机肥对贫瘠黄褐土改良的研究

为了阐明餐厨垃圾生物有机肥改良贫瘠土壤的作用机制,以贫瘠黄褐土为研究对象,通过不施肥、长期（>5 a）施用化肥、中长期（5 a）施用少量餐厨垃圾生物有机肥和短期（1 a）施用大量餐厨垃圾生物有机肥4种施肥方式,分别记为CK组、CF组、LOF-5组和MOF-1组,对比分析不同施肥方式对土壤OM（有机质）、活性有机碳、营养元素和团聚体等的影响.结果表明:①施用餐厨垃圾生物有机肥可显著提高土壤OM、活性有机碳含量,其中,MOF-1组提高效果最显著,与CK组相比,w（OM）可提高173.29%,w（ROC）（ROC为易氧化有机碳）增加了39.17%,w（POC）（POC为颗粒有机碳）和w（DOC）（DOC为可溶性有机碳）分别是CK组的13.85和10.32倍.②中长期（5 a）施用少量餐厨垃圾生物有机肥可增加土壤中较大粒径团聚体的占比,且更有利于提高土壤团粒结构的稳定性,LOF-5组>2 mm粒级的团聚体占比是CK组的4.68倍;与CK组相比,LOF-5组MWD（平均重量直径）增加了100.00%,GMD（几何平均直径）增加了82.98%,>0.25 mm水稳定性团聚体质量占比（DR_0.25）增加了27.20%.③中长期（5 a）施用少量餐厨垃圾生物有机肥可增加土壤中w（TN）（TN为全氮）和w（AN）（AN为速效氮）,与CK组相比,LOF-5组w（TN）和w（AN）分别增加了77.42%和20.82%.施用餐厨垃圾有机肥也可同时增加土壤中w（AP）（AP为速效磷）和w（AK）（AK为速效钾）,MOF-1组增加效果较佳,w（AP）和w（AK）分别是CK组的9.43和3.39倍.研究显示,中长期（5 a）施用少量餐厨垃圾生物有机肥可提升土壤固碳能力,提高土壤养分利用的有效性,从而提升耕地土壤质量,减少化肥施用量,是我国贫瘠黄褐土改良的有效施肥模式.      

国内外饮用水余氯限值及监测方法的研究进展

新型冠状病毒肺炎疫情期间大规模使用含氯消毒剂,其残留可能对水环境及人体健康造成影响.我国饮用水水源地质量标准并未设置余氯项目及其浓度限值,且缺乏统一的余氯现场快速分析方法标准.为公共卫生事件发生期间的水质余氯监测与评价提供参考,对国内外饮用水标准余氯限值、实验室标准分析方法、现场快速分析方法等进行汇总分析,结果表明:①不同国家和地区以及WHO（World Health Organization,世界卫生组织）在饮用水标准中分别设置了出厂水中余氯限值（范围为0.1~2.0 mg/L）、管网末梢水中余氯限值（范围为0.1~1.8 mg/L）及饮用水中余氯最大允许浓度（范围为4~5 mg/L）.②比色法、容量法因其具有反应迅速且稳定、准确度及精密度较高等优点而成为国内外实验室主要标准或推荐分析方法,高效液相色谱法检出限最低,灵敏度最高,可用于余氯痕量分析.③余氯现场快速分析方法多以比色法为主,在线监测方法多为电化学方法,但缺乏统一的标准方法.研究显示,国外饮用水标准中余氯最大允许浓度为5 mg/L,WHO推荐高风险环境下的管网末梢余氯浓度最低为0.5 mg/L,建议尽快开展水质余氯现场监测方法标准化研究.      

新冠肺炎疫情期间我国居民洗手行为研究

直接接触和飞沫传播等方式是新型冠状病毒传播的主要途径,合理的洗手行为是切断暴露途径和降低病毒感染风险的有效防控措施,对于新型冠状病毒肺炎（COVID-19,简称“新冠肺炎”）疫情的防控具有重要的作用.该研究于2020年2月25日—3月14日,采用电子问卷的方式调查了覆盖我国31个省（自治区、直辖市）1 728个县（区）18岁及以上的居民,收集共计8 330名成人的洗手情形及洗手时长等信息,分析不同暴露情景下的洗手行为及其影响因素.结果表明:女性、城市地区居民在洗手比例和洗手时长上均分别高于男性、农村地区居民.人群在一般暴露情景下的洗手比例较高,而对于病毒感染风险较高的暴露情景（如咳嗽或打喷嚏后、接触他人后等）的洗手率（分别为73.6%和83.9%）排名靠后,说明人群对病毒的传播途径和防护措施有待深入理解;在洗手时间上,根据WHO规定的洗手时长标准（20 s）,仅有41.7%的人群洗手时长合格（大于20 s）,城区居民洗手时长的合格率（42.0%）显著高于农村地区（39.7%）;总体上,具有外出经历的人群洗手比例较未曾外出的人群高,新冠肺炎疫情期间居住地是否存在新冠肺炎疑似和确诊病例显著影响居民的洗手行为,但是疫情最严重的地区居民的洗手时长合格率（37.2%）最低,反而疫情最轻的地区居民的洗手时长合格率（43.6%）最高,说明居民的洗手行为可能受疫情等多方面的影响.研究显示,相比于非疫情期间而言,疫情期间我国居民洗手行为发生率提高,洗手时长合格率提高,但是仍然水平偏低.应提高居民洗手行为意识,科学地执行洗手这一防护措施,相关政策制定以及个人防护应当进一步关注和重视洗手行为的防疫作用.      

闽江河口养虾塘养殖期和非养殖期CO2通量变化特征

为揭示河口区陆基养虾塘从养殖期到非养殖期一年间的CO₂通量变化,以福建省闽江河口鳝鱼滩陆基养虾塘为研究对象,于2016年5月-2017年3月采用悬浮箱/静态箱-气相色谱法对养虾塘养殖期水-大气界面和非养殖期沉积物-大气界面白天CO₂垂直通量进行原位观测.结果表明:①养虾塘在整个研究期间CO₂通量变化范围为-62.87~162.81 mg/（m2·h）,平均值为（42.66±18.12）mg/（m2·h）,总体上表现为大气CO₂的释放源,且呈非养殖期CO₂通量平均值[（78.51±16.61）mg/（m2·h）]显著高于养殖期[（17.98±18.26）mg/（m2·h）]的特征.②养殖期间,养虾塘CO₂通量呈"排放-吸收"交替变化的特征,而非养殖期养虾塘一直是大气CO₂的净排放源.③养虾塘养殖期CO₂通量时间变化特征主要受到ρ（DOC）（DOC为总溶解有机碳）、ρ（SO₄2-）、ρ（Cl-）、盐度、pH、ρ（Chla）（Chla为叶绿素a）的影响,其中,pH和ρ（SO₄2-）是其主要影响因子,而ρ（TDN）（TDN为总溶解氮）、ρ（TDP）（TDP为总溶解磷）、ρ（SO₄2-）对非养殖期CO₂通量时间变化影响较大.研究显示,滨海陆基养殖塘是大气CO₂的重要来源,其排放通量多低于河流、水库等水生生态系统,但高于湖泊生态系统;养殖塘CO₂通量受人为影响明显,其较高的变异性与养殖生物、饲料投放以及浮游藻类有关.