稻田NO3-还原耦合As(III)氧化过程及微生物群落特征

以华南稻田土壤为研究对象通过构建微宇宙体系,研究了淹水稻田自养硝酸盐还原耦合As（III）氧化过程及其微生物群落结构组成.结果表明,NO₃^-的添加促进了稻田土壤中As（III）的氧化,在未添加NO₃^-的处理（Soil+As（III））以及灭菌处理（Sterilized soil+As（III）+NO₃^-）中As（III）未发生明显的氧化;在Soil+As（III）+NO₃^-处理中,NO₃^-有少量被还原,而在Soil+NO₃^-处理中,NO₃^-没有被还原.通过16S rRNA高通量分析在NO₃^-还原耦合As（III）氧化体系中微生物群落结构特征,在Soil+As（III）+NO₃^-处理中shannon指数相对较低为8.19,土壤微生物群落多样性降低,其中在门水平上主要优势菌群为变形菌门Proteobacteria（33%）、绿弯菌门Chloroflexi（11%）、浮霉菌门Planctomycetes（12%）;在属水平上主要的优势菌属为Gemmatimonas（7.4%）以及少量的Singulisphaera、Thermomonas、Bacillus.NO₃^-的添加能够促进稻田土壤中自养As（III）氧化,并且影响着稻田土壤中微生物群落组成.     

Role of glycine on sulfuric acid-ammonia clusters formation: Transporter or participator

Glycine(Gly) is ubiquitous in the atmosphere and plays a vital role in new particle formation(NPF).However,the potential mechanism of its on sulfuric acid(SA)-ammonia(A)clusters formation under various atmospheric conditions is still ambiguous.Herein,a(Gly)_x·(SA)_y·(A)_z(z≤x+y≤3) multicomponent system was investigated by using density functional theory(DFT) combined with Atmospheric Cluster Dynamics Code(ACDC) at different temperatures and precursor concentrations.The results show that Gly,with one carboxyl(-COOH) and one amine(-NH_2) group,can interact strongly with SA and A in two directions through hydrogen bonds or proton transfer.Within the relevant range of atmospheric concentrations,Gly can enhance the formation rate of SA-A-based clusters,especially at low temperature,low [SA],and median [A].The enhancement(R) of Gly on NPF can be up to 340 at T=218.15 K,[SA]=10~4,[A]=10~9,and [Gly]=10~7 molecules/cm~3.In addition,the main growth paths of clusters show that Gly molecules participate into cluster formation in the initial stage and eventually leave the cluster by evaporation in subsequent cluster growth at low [Gly],it acts as an important "transporter" to connect the smaller and larger cluster.With the increase of [Gly],it acts as a "participator" directly participating in NPF.     

Effects of SO2 and H2O on low-temperature NO conversion over F-V2O5-WO3/TiO2 catalysts

F-V_2 O_5-WO3/Ti02 catalysts were prepared by the impregnation method.As the content of F ions increased from 0.00 to 0.35 wt.%,the NO conversion of F-V_2 O_5-WO_3/TiO_2 catalysts initially increased and then decreased.The 0.2 F-V_2 O_5-WO_3/TiO_2 catalyst(0.2 wt.% F ion)exhibited the best denitration(De-NOx) performance,with more than 95% NO conversion in the temperature range 160-360℃,and 99.0% N2 selectivity between 110 and 280℃.The addition of an appropriate amount of F ions eroded the surface morphology of the catalyst and reduced its grain size,thus enhancing the NO conversion at low temperature as well as the sulfur and water resistance of the V_2 O_5-WO3/Ti02 catalyst.After selective catalytic reduction(SCR) reaction in a gas flow containing SO_2 and H_2 O,the number of NH3 adsorption sites,active component content,specific surface area and pore volume decreased to different degrees.Ammonium sulfate species deposited on the catalyst surface,which blocked part of the active sites and reduced the NO conversion performance of the catalyst.On-line thermal regeneration could not completely recover the catalyst activity,although it prolonged the cumulative life of the catalyst.In addition,a mechanism for the effects of S02 and H_2 O on catalyst NO conversion was proposed.     

Dynamic nano-Ag colloids cytotoxicity to and accumulation by Escherichia coli: Effects of Fe3+, ionic strength and humic acid

Released Ag ions or/and Ag particles are believed to contribute to the cytotoxicity of Ag nanomaterials, and thus, the cytotoxicity and mechanism of Ag nanomaterials should be dynamic in water due to unfixed Ag particle:Ag⁺ ratios. Our recent research found that the cytotoxicity of PVP-Ag nanoparticles is attributable to Ag particles alone in 3 hr bioassays, and shifts to both Ag particles and released Ag⁺ in 48 hr bioassays. Herein, as a continued study, the cytotoxicity and accumulation of 50 and 100 nm Ag colloids in Escherichia coli were determined dynamically. The cytotoxicity and mechanisms of nano-Ag colloids are dynamic throughout exposure and are derived from both Ag ions and particles. Ag accumulation by E. coli is derived mainly from extracellular Ag particles during the initial 12 hr of exposure, and thereafter mainly from intracellular Ag ions. Fe³⁺ accelerates the oxidative dissolution of nano-Ag colloids, which results in decreasing amounts of Ag particles and particle-related toxicity. Na⁺ stabilizes nano-Ag colloids, thereby decreasing the bioavailability of Ag particles and particle-related toxicity. Humic acid (HA) binds Ag⁺ to form Ag⁺-HA, decreasing ion-related toxicity and binding to the E. coli surface, decreasing particle-related toxicity. HA in complex conditions showed a stronger relative contribution to toxicity and accumulation than Na⁺ or Fe³⁺. The results highlighted the cytotoxicity and mechanism of nano-Ag colloids are dynamic and affected by environmental factors, and therefore exposure duration and water chemistry should be seriously considered in environmental and health risk assessments.     

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.     

Effect of substituents in hydroxyl radical-mediated degradation of azo pyridone dyes: Theoretical approaches on the reaction mechanism

Understanding the degradation behavior of azo dyes in photocatalytic wastewater treatment is of fundamental and practical importance for their application in textile-processing and other coloration industries. In this study, quantum chemistry, as density functional theory, was used to elucidate different degradation pathways of azo pyridone dyes in a hydroxyl radical (HO^?)-initiated photocatalytic system. A series of substituted azo pyridone dyes were synthesized by changing the substituent group in the para position of the benzene moiety, ranging from strong electron-donating to strong electron-withdrawing groups. The effect of dye molecular structure on the photocatalytic degradation reaction mechanism was analyzed and quantification of substituent effects on the thermodynamic and kinetics parameters was performed. Potential energy surface analysis revealed the most susceptible reaction site for the HO^? attack. The calculated reaction barriers are found to be strongly affected by the nature of substituent group with a good correlation using Hammett σ_p constants and experimentally determined reaction rates. The stability of pre-reaction complexes and transition state complexes were analyzed applying the distortion-interaction model. The increased stability of the transition state complexes with the distancing from the substituent group has been established.     

2019年10~12月京津冀及周边“2+26”城市重污染减排效果评估

为评估京津冀及周边区域重污染过程期间应急减排措施的效果,基于情景模拟的方法,采用NAQPMS模式和多种观测资料,分析了2019年10~12月期间京津冀及周边区域环境空气质量、重污染过程和气象条件概况,评估了模式24、72和144 h的PM_2.5预报效果,并对应急减排措施的效果和不确定性进行了讨论.结果表明,2019年10~12月京津冀及周边"2+26"城市PM_2.5平均浓度64 μg ·m^-3,同比降低了10 μg ·m^-3;区域性重污染过程4次,受影响城市重污染过程期间PM_2.5平均浓度156 μg ·m^-3."2+26"城市PM_2.5气象条件评估指数（EMI）变化值范围为-15.6%~16.8%,EMI显示北京、天津和石家庄等12个城市气象条件与同期相比变差,变差程度范围为3.2%~16.8%.减排情景模拟分析显示应急减排措施有效减少了区域性重污染过程的发生,污染物峰值浓度降幅明显,未出现区域性严重污染过程.典型重污染期间,北京、石家庄、保定和唐山等城市PM_2.5日均浓度削减2%~9%.区域应急减排措施促使"2+26"城市PM_2.5季度均值分别降低1~3 μg ·m^-3左右,区域性减排效果明显.     

德州市夏季臭氧敏感性特征及减排方案

近年来德州市臭氧污染频发,2018年夏季（6~8月）,德州市发生了严重臭氧污染事件,臭氧日最大8 h浓度值超标天数达60 d,超标率65%,3个月平均值为176 μg ·m^-3,最高达262 μg ·m^-3.本研究利用WRF-CAMx耦合的HDDM模块,分析期间德州臭氧敏感性特征及减排方案.结果表明,在空间上,德州市中心城区为VOCs控制区,而郊区为NO_x与VOCs协同控制区.在时间上,VOCs敏感值每日为正值,但dO₃_V₅₀在6月（城区18.7 μg ·m^-3,郊区19.7 μg ·m^-3）和8月（城区15.3 μg ·m^-3,郊区16.4 μg ·m^-3）高于7月（城区13.0 μg ·m^-3,郊区11.8 μg ·m^-3）,NO_x敏感值城区呈正负交错,郊区大部分为正值,并与VOCs敏感值接近.对于城区减排方案应考虑以仅VOCs削减为优先,而郊区由于NO_x和VOCs对臭氧减排效果相当,建议以NO_x：VOCs=1：1为优.     

汶川地震重灾区泥石流灾损土地利用及生态修复模式——以北川县都坝河小流域为例

汶川地震诱发了大量泥石流灾害,灾损土地利用和生态修复是灾区产业重建面临的重要课题。以北川县都坝河小流域为研究对象,通过调查灾损土地禀赋、灾害特征、土地需求,采取多因素耦合和关键因子限制分析法,探讨灾害胁迫条件下的经济活动与生态修复之间的互馈作用,结果表明：（1）流域新增土地供给源主要为泥石流灾损土地,土地资源化利用受灾害、聚落和产业结构控制;（2）灾损土地根据成因划分为沟口堆积型、沟道冲淤型以及岸坡侵蚀型,三者的肥力、安全性及交通条件等特征具有显著差异;（3）基于“因灾分区、耕地优先、产业共建、美居造景”的原则,建立了灾损土地的利用方式和生态修复模式,并选取杨家沟进行验证,沟域灾损土地利用方式为生态林地、产业林地及优质耕地,分别占比28.5%、56.3%、15.2%,生态修复措施主要为提高土地安全度、提升植被覆盖率和增强水保功能。该研究建立的震区土地利用和生态修复模式可有力协调人地矛盾、发展绿色经济和提升人居环境。