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.     

Advanced molecular-fingerprinting analysis of dissolved organic sulfur by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry using optimal spray solvent

Molecular level characterization of dissolved organic sulfur (DOS) by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICR MS) is necessary for further understanding of the role of DOS in the environment. Here, ESI spray solvent, a key parameter for ion production during ESI process, was investigated for its effect on the molecular characterization of DOS by ESI-FTICR MS. 100% MeOH as spray solvent was found for the first time to remarkably enhance the ionization efficiency of the majority of CHOS-molecules in NOM, which facilitated a total of 1473 CHOS-molecular formulas with one sulfur atom to be detected. The number of CHOS-molecular formulas obtained using 100%MeOH as spray solvent increased notably over 740 in comparison with those using 50% MeOH aqueous solution (731) or 50% ACN aqueous solution (653). Moreover, due to the enhancement of ionization efficiency of DOS during ESI processes, the tandem mass spectra of the NOM CHOS-molecules could be easily obtained using 100% MeOH as spray solvent, which were hardly obtained using 50% MeOH aqueous solution as spray solvent. The results of the tandem mass spectra suggested the first discovery of organosulfates or sulfonic acids in Suwannee River NOM sample. A simple method based on 100% MeOH as ESI spray solvent for advanced molecular characterization of DOS by ESI-FTICR MS was proposed and applied, and the results revealed more molecular information of DOS in sea DOM samples.     

Metabolomic modulations in a freshwater microbial community exposed to the fungicide azoxystrobin

An effective broad-spectrum fungicide, azoxystrobin (AZ), has been widely detected in aquatic ecosystems, potentially affecting the growth of aquatic microorganisms. In the present study, the eukaryotic alga Monoraphidium sp. and the cyanobacterium Pseudanabaena sp. were exposed to AZ for 7 days. Our results showed that 0.2–0.5 mg/L concentrations of AZ slightly inhibited the growth of Monoraphidium sp. but stimulated Pseudanabaena sp. growth. Meanwhile, AZ treatment effectively increased the secretion of total organic carbon (TOC) in the culture media of the two species, and this phenomenon was also found in a freshwater microcosm experiment (containing the natural microbial community). We attempted to assess the effect of AZ on the function of aquatic microbial communities through metabolomic analysis and further explore the potential risks of this compound. The metabonomic profiles of the microcosm indicated that the most varied metabolites after AZ treatment were related to the citrate cycle (TCA), fatty acid biosynthesis and purine metabolism. We thereby inferred that the microbial community increased extracellular secretions by adjusting metabolic pathways, which might be a stress response to reduce AZ toxicity. Our results provide an important theoretical basis for further study of fungicide stress responses in aquatic microcosm microbial communities, as well as a good start for further explorations of AZ detoxification mechanisms, which will be valuable for the evaluation of AZ environmental risk.     

Analytical methods and environmental processes of nanoplastics

The degradation of plastic debris may result in the generation of nanoplastics (NPs). Their high specific surface area for the sorption of organic pollutions and toxic heavy metals and possible transfer between organisms at different nutrient levels make the study of NPs an urgent priority. However, there is very limited understanding on the occurrence, distribution, abundant, and fate of NPs in the environment, partially due to the lack of suitable techniques for the separation and identification of NPs from complex environmental matrices. In this review, we first overviewed the state-of-the-art methods for the extraction, separation, identification and quantification of NPs in the environment. Some of them have been successfully applied for the field determination of NPs, while some are borrowed from the detection of microplastics or engineered nanomaterials. Then the possible fate and transport of NPs in the environment are thoroughly described. Although great efforts have been made during the recent years, large knowledge gaps still exist, such as the relatively high detection limit of existing method failing to detect ultralow masses of NPs in the environment, and spherical polystyrene NP models failing to represent the various compositions of NPs with different irregular shapes, which needs further investigation.     

UASB启动运行特征及互营丙酸氧化菌定量分析

为揭示升流式厌氧污泥床（UASB）反应器启动运行效能与互营丙酸降解菌群数量之间的关系,以稀释的玉米淀粉生产废水为底物,考察了UASB启动期的运行特征,并采用实时荧光定量PCR技术（qPCR）分析了互营丙酸降解菌群（丙酸氧化菌和产甲烷菌）的演替规律.结果表明,在进水COD 2000mg/L和水力停留时间（HRT）24h条件下,经过38d的连续运行,COD去除率达到了91.9%.当HRT分阶段缩短至8h时,比产甲烷速率达到了315LCH₄/（kg COD·d）,且形成了沉降性能良好的颗粒污泥.qPCR检测结果表明,至少有5种已鉴定的丙酸氧化菌存在于UASB反应器中.Pelotomaculum propionicum为接种污泥中的主要丙酸氧化菌,约占检测到丙酸氧化菌总数的45.7%.它的数量随着HRT缩短不断减少.而Syntrophobacter sulfatireducens和S.wolinii的数量随着HRT缩短不断增加,并在启动完成时达到最大值,分别为1.3×10³,5.5×10³个16S rRNA基因拷贝数/ng DNA,演替成为成熟颗粒污泥中的优势丙酸氧化菌群.Methanobacterium和Methanosarcina为接种污泥中的主要氢营养型产甲烷菌和乙酸营养型产甲烷菌,其数量随着HRT的缩短而逐渐减少,而Methanospirillum和Methanosaeta的数量随HRT的缩短逐渐增加,成为成熟颗粒污泥中的优势产甲烷菌群.     

三江源植被碳利用率动态变化及其对气候响应

本文基于MODIS GPP/NPP数据估算了三江源植被碳利用率（CUE）,结合气象数据和高程数据采用一元线性回归和相关分析法,探讨了2001~2017年三江源植被CUE的时空变化特征及植被CUE对气温、降水量和蒸散量变化的响应.结果表明：（1）三江源植被CUE年内3~10月表现为先增加后降低的变化趋势,其中6月植被CUE最高.（2）三江源年植被碳利用率位于0.73~1,平均水平为0.85;植被CUE空间上呈现北高南低,西高东低的分布特征.（3）整体上,三江源4~10月植被碳利用率与同期气温、降水量和蒸散量分别呈现正相关、负相关和负相关关系,降水量是影响三江源植被CUE变化的主要影响因素,气温为次要因素,蒸散量影响程度最小.     

烟花爆竹燃放对大气污染物及PM2.5组分影响

为了解烟花爆竹燃放对保定市大气污染物和PM_2.5中水溶性离子及有机碳（OC）、元素碳（EC）浓度的影响,对保定市春节期间大气污染物和颗粒物组分的浓度特征进行了分析,并评估了烟花爆竹的贡献.结果表明： 2019年春节期间烟花爆竹集中燃放期PM_2.5、PM₁₀、SO₂、NO₂、CO平均浓度比非集中燃放期分别增加了1.3、1.0、1.1、0.4、0.02倍;保定市春节期间禁燃措施施行后,除夕、初一2d污染物平均浓度、最高浓度和高浓度持续时间均明显下降,集中燃放期烟花爆竹燃放对PM_2.5、PM₁₀和SO₂浓度贡献量从50%左右（2018年、2017年）下降至30%左右（2019年）,其中SO₂贡献量下降幅度超过PM_2.5和PM₁₀;组分分析表明,接待中心站点（主城区）、涿州站点（区县建成区）烟花爆竹燃放期K⁺、Mg²⁺、Cl^-浓度在水溶性离子中的总占比分别为39.3%、51.1%,比非燃放期的占比显著上升;烟花爆竹燃放对PM_2.5中K⁺、Mg²⁺、Cl^-浓度贡献率在50%以上,其中对K⁺贡献占比高达89.0%,涿州站点SO₄^2-、K⁺、Mg²⁺、Cl^-的贡献量分别是接待中心站点的2.2、2.1、1.9、1.8倍,燃放期硫氧化率（SOR）、氮氧化率（NOR）相比于非燃放期均有一定程度的升高;集中燃放期OC、EC浓度较非集中燃放期分别升高了2.5、2.1倍,烟花爆竹燃放对OC影响大于EC.     

Well-to-wheels greenhouse gas and air pollutant emissions from battery electric vehicles in China

Mitigation and Adaptation Strategies for Global Change - Electric vehicles (EVs) play a crucial role in addressing climate change and urban air quality concerns. China has emerged as the global...     

Can a low-carbon development path achieve win-win development: evidence from China’s low-carbon pilot policy

Mitigation and Adaptation Strategies for Global Change - Low-carbon pilot (LCP) policy aims to not only achieve economic development but also address climate change problems in China. With a...     

Evaluating national hydrogen refueling infrastructure requirement and economic competitiveness of fuel cell electric long-haul trucks

This study explored the national hydrogen refueling infrastructure requirement along major United States (US) interstate highway corridors to support the deployment of fuel cell electric trucks (FCETs) for the national long-haul trucking fleet. Given the long-haul trucking shipment demand in 2025 projected by the Freight Analysis Framework, locations and capacities of hydrogen stations were identified for inter-zone freight flows, and the total daily refueling demand was estimated for intra-zone flows for each FAF zone. Based on the infrastructure deployment results, we conducted an economic feasibility analysis of FCETs by evaluating the total ownership cost. We found that when the FCET penetration is relatively high (e.g., 10% penetration), FCETs become more competitive in terms of fuel cost and idling cost and could be economic viable if the incremental vehicle cost is reduced to meet the near-term FCET technology cost targets and the liquefaction cost is reduced to an optimal case. We also observed that the station cost depends on regional factors, particularly regional demand, which is used to determine station capacity. Thus, one possible strategy for station roll-out is to have early investment in target regions where station costs are expected to be relatively low such as the Pacific and West South Central regions.