Progress of environmental research in China from 2000 to 2019: Case studies of JES and ES&T

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Relationships between chemical elements of PM2.5 and O3 in Shanghai atmosphere based on the 1-year monitoring observation

Mass level of fine particles(PM_2.5) in main cities in China has decreased significantly in recent years due to implementation of Chinese Clean Air Action Plan since 2013,however,03 pollution is getting worse than before,especially in megacities such as in Shanghai.In this work,O₃ and PM_2.5 were continuously monitored from May 27,2018 to March 31,2019.Our data showed that the annual average concentration of PM_2.5 and O₃(O₃-8 hr,max...     

Distribution and chemical speciation of arsenic in different sized atmospheric particulate matters

The distribution and chemical speciation of arsenic (As) in different sized atmospheric particulate matters (PMs), including total suspended particles (TSP), PM₁₀, and PM_2.5, collected from Baoding, China were analyzed. The average total mass concentrations of As in TSP, PM₁₀, and PM_2.5 were 31.5, 35.3, and 54.1 µg/g, respectively, with an order of PM_2.5 >PM ₁₀ > TSP, revealing that As is prone to accumulate on fine particles. Due to the divergent toxicities of different As species, speciation analysis of As in PMs is further conducted. Most of previous studies mainly focused on inorganic arsenite (iAs^III), inorganic arsenate (iAs^V), monomethylarsonate (MMA), and dimethylarsinate (DMA) in PMs, while the identification and sensitive quantification of trimethylarsine oxide (TMAO) were rarely reported. In this study, a high-performance liquid chromatography coupled to inductively coupled plasma mass spectrometry system was optimized for As speciation including TMAO in PMs. An anion exchange column was used to separate MMA, DMA and iAs^V, while a cation exchange column to separate TMAO and iAs^III. Results showed that iAs^V was the dominate component in all the samples, corresponding to a portion of 79.2% ± 9.3% of the total extractable species, while iAs^III, TMAO and DMA made up the remaining 21%. Our study demonstrated that iAs^III accounted for about 14.4% ± 11.4% of the total extracted species, with an average concentration of 1.7 ± 1.6 ng/m³. It is worth noting that TMAO was widely present in the samples (84 out of 97 samples), which supported the assumption that TMAO was ubiquitous in atmospheric particles.     

Characterization of a new smog chamber for evaluating SAPRC gas-phase chemical mechanism

A new state-of-the-art indoor smog chamber facility(CAPS-ZJU) has been constructed and characterized at Zhejiang University,which is designed for chemical mechanism evaluation under well-controlled conditions.A series of characterization experiments were performed to validate the well-established experimental protocols,including temperature variation pattern,light spectrum and equivalent intensity(J_NO2),injection and mixing performance,as well as gases and particle wall loss.In additi...     

Effects of chemical modification on physicochemical properties and adsorption behavior of sludge-based activated carbon

This study aimed to explore the adsorption performance of sludge-based activated carbon (SBC) towards dissolved organic matters (DOMs) removal from sewage, and investigated the modification effect of different types of chemicals on the structure of synthesized SBC. Waste activated sludge (WAS) was used as a carbon source, and HCl, HNO₃, and NaOH were used as different types of chemicals to modify the SBC. With the aid of chemical activation, the modified SBC showed higher adsorption performances on DOMs removal with maximum adsorption of 29.05 mg/g and second-order constant (k) of 0.1367 (L/mol/sec) due to the surface elution of ash and minerals by chemicals. The surface elemental composition of MSBC suggested that the content of C-C and C-O functional groups on the surface of modified sludge-based activated carbon (MSBC) played an important role on the adsorption capacities of MSBC towards DOMs removal in sewage. Additionally, the residual molecular weight of DOMs in sewage was investigated using a 3-dimension fluorescence excitation-emission matrix (3D-EEM) and high-performance size exclusion chromatography (HP-SEC). Results showed that the chemical modification significantly improved the adsorption capacity of MSBC on humic acids (HA) and aromatic proteins (APN), and both of NaOH-MSBC and HCl-MSBC were effective for a wide range of different AMW DOMs removal from sewage, while the HNO₃-MSBC exhibited poorly on AMW organics of 2,617 Da and 409 Da due to the reducing content of macropore. In brief, this study provides reference values for the impact of the chemicals of the activation stage before the SBCs application.     

Au nanoring arrays as surface enhanced Raman spectroscopy substrate for chemical component study of individual atmospheric aerosol particle

Monolayer-ordered gold nanoring arrays were prepared by ion-sputtering method and used as surface enhanced Raman spectroscopy (SERS) substrates to test the individual atmospheric aerosols particle. Compared to other methods used for testing atmospheric aerosols particles, the collection and subsequent detection in our work is performed directly on the gold nanoring SERS substrate without any treatment of the analyte. The SERS performance can be tuned by changing the depth of the gold nanoring cavity as originating from coupling of dipolar modes at the inner and outer surfaces of the nanorings. The electric field exhibits uniform enhancement and polarization in the ordered Au nanoring substrate, which can improve the accuracy for detecting atmospheric aerosol particles. Combined with Raman mapping, the information about chemical composition of individual atmospheric aerosols particle and distribution of specific components can be presented visually. The results show the potential of SERS in enabling improved analysis of aerosol particle chemical composition, mixing state, and other related physicochemical properties.     

Vertical distribution and temporal evolution of formaldehyde and glyoxal derived from MAX-DOAS observations: The indicative role of VOC sources

Formaldehyde (HCHO) and glyoxal (CHOCHO) are important oxidization intermediates of most volatile organic compounds (VOCs), but their vertical evolution in urban areas is not well understood. Vertical profiles of HCHO, CHOCHO, and nitrogen dioxide (NO₂) were retrieved from ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations in Hefei, China. HCHO and CHOCHO vertical profiles prefer to occur at higher altitudes compared to NO₂, which might be caused by the photochemistry-oxidation of longer-lived VOCs at higher altitudes. Monthly means of HCHO concentrations were higher in summer, while enhanced amounts of NO₂ were mainly observed in winter. CHOCHO exhibited a hump-like seasonal variation, with higher monthly-averaged values not only occurred in warm months (July-August) but also in cold months (November-December). Peak values mainly occurred during noon for HCHO but emerged in the morning for CHOCHO and NO₂, suggesting that HCHO is stronger link to photochemistry than CHOCHO. We further use the glyoxal to formaldehyde ratio (GFR) to investigate the VOC sources at different altitudes. The lowest GFR value is almost found in the altitude from 0.2 to 0.4 km, and then rises rapidly as the altitude increases. The GFR results indicate that the largest contributor of the precursor VOC is biogenic VOCs at lower altitudes, while at higher altitudes is anthropogenic VOCs. Our findings provide a lot more insight into VOC sources at vertical direction, but more verification is recommended to be done in the future.     

An integrated chemical mass balance and source emission inventory model for the source apportionment of PM2.5 in typical coastal areas

The source apportionment of PM_2.5 is essential for pollution prevention.In view of the weaknesses of individual models,we proposed an integrated chemical mass balancesource emission inventory(CMB-SEI) model to acquire more accurate results.First,the SEI of secondary component precursors(SO₂,NO_x,NH₃,and VOCs) was compiled to acquire the emission ratios of these sources for the precursors.Then,a regular CMB simulation was executed to obtain the contribut...     

Fine particle-bound PAHs derivatives at mountain background site (Mount Tai) of the North China: Concentration, source diagnosis and health risk assessment

Ten nitrated polycyclic aromatic hydrocarbons (nPAHs) and 4 oxygenated polycyclic aromatic hydrocarbons (oPAHs) in fine particulate matter (PM_2.5) samples from Mount Tai were analyzed during summer (June to August), 2015. During the observation campaign, the mean concentration of total nPAHs and oPAHs was 31.62 pg/m³ and 0.15 ng/m³, respectively. Two of the monitored compounds, namely 9-nitro-anthracene (9N-ANT) (6.86 pg/m³) and 9-fluorenone (9FO) (0.05 ng/m³) were the predominant compounds of nPAHs and oPAHs, respectively. The potential source and long-range transportation of nPAHs and oPAHs were investigated by the positive matrix factorization (PMF) method and the potential source contribution function (PSCF) methods. The results revealed that biomass/coal burning, gasoline vehicle emission, diesel vehicle emission and secondary formation were the dominant sources of nPAHs and oPAHs, which were mainly from Henan province and Beijing-Tianjin-Hebei region and Bohai sea. The incremental life cancer risk (ILCR) values were calculated to evaluate the exposure risk of nPAHs and oPAHs for three group people (infant, children and adult), and the values of ILCR were 7.02 × 10^?10, 3.49 × 10^?9 and 1.41 × 10^?8 for infant, children and adults, respectively. All these values were lower than the standard of EPA (Environmental Protection Agency) (<10^?6), indicating acceptable health risk of nPAHs and oPAHs.     

Potential dissemination mechanism of the tetC gene in Aeromonas media from the aerobic biofilm reactor under oxytetracycline stresses

The tetC gene has been found to be one of the most widely distributed tetracycline resistance (tet) genes in various environmental niches, but the detailed dissemination mechanisms are still largely unknown. In the present study, 11 tetC-containing Aeromonas media strains were isolated from an aerobic biofilm reactor under oxytetracycline stresses, and the genome of one strain was sequenced using the PacBio RSII sequencing approach to reveal the genetic environment of tetC. The tetC gene was carried by an IS26 composite transposon, named Tn6434. The tetC-carrying Tn6434 structure was detected in all of the A. media strains either in a novel plasmid pAeme2 (n=9) or other DNA molecules (n=2) by PCR screening. The NCBI database searching result shows that this structure was also present in the plasmids or chromosomes of other 13 genera, indicating the transferability of Tn6434. Inverse PCR and sequencing confirmed that Tn6434 can form a circular intermediate and is able to incorporate into a preexisting IS26 element, suggesting that Tn6434 might be responsible for the dissemination of tetC between different DNA molecules. This study will be helpful in uncovering the spread mechanism of tet genes in water environments.     

Formation control of bromate and trihalomethanes during ozonation of bromide-containing water with chemical addition: Hydrogen peroxide or ammonia?

To ensure the safety of drinking water, ozone (O₃) has been extensively applied in drinking water treatment plants to further remove natural organic matter (NOM). However, the surface water and groundwater near the coastal areas often contain high concentrations of bromide ion (Br^?). Considering the risk of bromate (BrO₃^?) formation in ozonation of the sand-filtered water, the inhibitory efficiencies of hydrogen peroxide (H₂O₂) and ammonia (NH₃) on BrO₃^? formation during ozonation process were compared. The addition of H₂O₂ effectively inhibited BrO₃^? formation at an initial Br^? concentration amended to 350 µg/L. The inhibition efficiencies reached 59.6 and 100% when the mass ratio of H₂O₂/O₃ was 0.25 and > 0.5, respectively. The UV₂₅₄ and total organic carbon (TOC) also decreased after adding H₂O₂, while the formation potential of trihalomethanes (THMsFP) increased especially in subsequent chlorination process at a low dose of H₂O₂. To control the formation of both BrO₃^? and THMs, a relatively large dose of O₃ and a high ratio of H₂O₂/O₃were generally needed. NH₃ addition inhibited BrO₃^? formation when the background ammonia nitrogen (NH₃N) concentration was low. There was no significant correlation between BrO₃^? inhibition efficiency and NH₃ dose, and a small amount of NH₃N (0.2 mg/L) could obviously inhibit BrO₃^? formation. The oxidation of NOM seemed unaffected by NH₃ addition, and the structure of NOM reflected by synchronous fluorescence (SF) scanning remained almost unchanged before and after adding NH₃. Considering the formation of BrO₃^? and THMs, the optimal dose of NH₃ was suggested to be 0.5 mg/L.     

Key strategies for the restoration of Dongting Lake in Middle Yangtze, China

The Yangtze River Economic Belt(YREB)has been estab-lished since 2015 by the Chinese Government as a strat-egy in regional economic development.Approximately 40...     

The role of extracellular organic matter on the cyanobacteria ultrafiltration process

The membrane fouling caused by extracellular organic matter (EOM) and algal cells and organic matter removal of two typical cyanobacteria (M. aeruginosa and Pseudoanabaena sp.) during ultrafiltration (UF) process were studied in this work. The results showed that EOM had a broad molecular weight (Mw) distribution and the irreversible membrane fouling was basically caused by EOM. Moreover, humic acid and microbial metabolites were major components of EOM of two typical cyanobacteria. Since EOM could fill the voids of cake layers formed by the algal cells, EOM and algal cells played synergistic roles in membrane fouling. Fourier transform infrared spectroscopy analysis indicated that the CH₂ and CH₃ chemical bonds may play an important role in membrane fouling caused by EOM. Interestingly, the cake layer formed by the algal cells could trap the organic matter produced by algae and alleviate some irreversible membrane fouling. The results also showed that although the cake layer formed by the algal cells cause severe permeate flux decline, it could play a double interception role with UF membrane and increase organic matter removal efficiency. Therefore, when using UF to treat algae-laden water, the balance of membrane fouling and organic matter removal should be considered to meet the needs of practical applications.     

Impact of meteorological condition changes on air quality and particulate chemical composition during the COVID-19 lockdown

Stringent quarantine measures during the Coronavirus Disease 2019 (COVID-19) lockdown period (January 23, 2020 to March 15, 2020) have resulted in a distinct decrease in anthropogenic source emissions in North China Plain compared to the paralleled period of 2019. Particularly, 22.7% decrease in NO₂ and 3.0% increase of O₃ was observed in Tianjin, nonlinear relationship between O₃ generation and NO₂ implied that synergetic control of NO_x and VOCs is needed. Deteriorating meteorological condition during the COVID-19 lockdown obscured the actual PM_2.5 reduction. Fireworks transport in 2020 Spring Festival (SF) triggered regional haze pollution. PM_2.5 during the COVID-19 lockdown only reduced by 5.6% in Tianjin. Here we used the dispersion coefficient to normalize the measured PM_2.5 (DN-PM_2.5), aiming to eliminate the adverse meteorological impact and roughly estimate the actual PM_2.5 reduction, which reduced by 17.7% during the COVID-19 lockdown. In terms of PM_2.5 chemical composition, significant NO₃^? increase was observed during the COVID-19 lockdown. However, as a tracer of atmospheric oxidation capacity, odd oxygen (O_x = NO₂ + O₃) was observed to reduce during the COVID-19 lockdown, whereas relative humidity (RH), specific humidity and aerosol liquid water content (ALWC) were observed with noticeable enhancement. Nitrogen oxidation rate (NOR) was observed to increase at higher specific humidity and ALWC, especially in the haze episode occurred during 2020SF, high air humidity and obvious nitrate generation was observed. Anomalously enhanced air humidity may response for the nitrate increase during the COVID-19 lockdown period.     

Response of PM2.5-bound elemental species to emission variations and associated health risk assessment during the COVID-19 pandemic in a coastal megacity

The coronavirus (COVID-19) pandemic is disrupting the world from many aspects. In this study, the impact of emission variations on PM_2.5-bound elemental species and health risks associated to inhalation exposure has been analyzed based on real-time measurements at a remote coastal site in Shanghai during the pandemic. Most trace elemental species decreased significantly and displayed almost no diel peaks during the lockdown. After the lockdown, they rebounded rapidly, of which V and Ni even exceeded the levels before the lockdown, suggesting the recovery of both inland and shipping activities. Five sources were identified based on receptor modeling. Coal combustion accounted for more than 70% of the measured elemental concentrations before and during the lockdown. Shipping emissions, fugitive/mineral dust, and waste incineration all showed elevated contributions after the lockdown. The total non-carcinogenic risk (HQ) for the target elements exceeded the risk threshold for both children and adults with chloride as the predominant species contributing to HQ. Whereas, the total carcinogenic risk (TR) for adults was above the acceptable level and much higher than that for children. Waste incineration was the largest contributor to HQ, while manufacture processing and coal combustion were the main sources of TR. Lockdown control measures were beneficial for lowering the carcinogenic risk while unexpectedly increased the non-carcinogenic risk. From the perspective of health effects, priorities of control measures should be given to waste incineration, manufacture processing, and coal combustion. A balanced way should be reached between both lowering the levels of air pollutants and their health risks.     

Technology development and cost analysis of multiple pollutant abatement for ultra-low emission coal-fired power plants in China

The implementation of ultra-low emission (ULE) limits (SO₂: 35 mg/m³, NOx: 50 mg/m³, PM: 10 mg/m³) promoted the development of flue gas treatment technologies in China. Pollutant control technology development for Chinese coal-fired power plants was summarized and an analysis of the applicability and cost of pollutant control technologies was conducted. Detailed data were collected from 30 ultra-low emission coal-fired units across China. Based on a cost analysis model, the average unit power generation incremental costs were 0.0144 and 0.0095 CNY/(kW·hr) for SO₂ and NOx control technologies, respectively. The unit power generation incremental cost of twin spray tower technology was 7.2% higher than that of dual-loop spray tower technology. The effect of key parameters on operating cost was analyzed. The unit power generation incremental cost increased because of increments in the electricity price for SO₂ control technology and the price of the reductant in NOx control technology. With high sulfur content or NOx concentration, the unit power generation incremental cost caused by pollutant control increased, whereas the unit pollutant abatement cost decreased. However, the annual operating hours or load increased, thereby leading to a decline in unit power generation incremental cost and unit pollutant abatement cost.     

Coastal mudflats as reservoirs of extracellular antibiotic resistance genes: Studies in Eastern China

Despite coastal mudflats serving as essential ecological zones interconnecting terrestrial/freshwater and marine systems, little is known about the profiles of antibiotic resistance genes (ARGs) in this area. In this study, characteristics of typical ARGs, involving both intracellular (iARGs) and extracellular ARGs (eARGs) at different physical states, were explored in over 1000 km of coastal mudflats in Eastern China. Results indicated the presence of iARGs and eARGs at states of both freely present or attached by particles. The abundance of eARGs was significantly higher than that of iARGs (87.3% vs 12.7%), and their dominance was more significant than those in other habitats (52.7%-76.3%). ARG abundance, especially for eARGs, showed an increasing trend (p < 0.05) from southern (Nantong) to northern (Lianyungang) coastal mudflats. Higher salinity facilitated the transformation from iARGs to eARGs, and smaller soil particle size was conducive to the persistence of eARGs in northern coastal mudflats. This study addresses the neglected function of coastal mudflats as eARGs reservoirs.     

Sources and health risks of PM2.5-bound polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) in a North China rural area

Polychlorinated biphenyls(PCBs) and organochlorine pesticides(OCPs) are typical persistent organic pollutants(POPs),which have high toxicity,bioaccumulation and long-distance transfer capability.Daily variation,sources of PcBs and OcPs in PM_2.5 are rarely explored in polluted rural area.Here,the sources and health risks of the PcBs and OcPs were evaluated for 48 PM_2.5 samples collected in winter 2017 in Wangdu,a heavy polluted rural area in the North China Plain.The average...     

Human health risk assessment of groundwater nitrate at a two geomorphic units transition zone in northern China

To assess groundwater nitrate contamination and its human health risks, 489 unconfined groundwater samples were collected and analyzed from Zhangjiakou, northern China. The spatial distribution of principle hydrogeochemical results showed that the average concentrations of ions in descend order was HCO₃^?, SO₄^2?, Na⁺, Ca²⁺, Cl^?, NO₃^?, Mg²⁺ and K⁺, among which the NO₃^? concentrations were between 0.25 and 536.73 mg/L with an average of 29.72 mg/L. In total, 167 out of 489 samples (~ 34%) exceeded the recommended concentration of 20 mg/L in Quality Standard for Groundwater of China. The high NO₃^? concentration groundwater mainly located in the northern part and near the boundary of the two geomorphic units. As revealed by statistical analysis, the groundwater chemistry was more significantly affected by anthropogenic sources than by the geogenic sources. Moreover, human health risks of groundwater nitrate through oral and dermal exposure pathways were assessed by model, the results showed that about 60%, 50%, 32% and 26% of the area exceeded the acceptable level (total health index>1) for infants, children, adult males and females, respectively. The health risks for different groups of people varied significantly, ranked: infants> children> adult males>adult females, suggesting that younger people are more susceptible to nitrate contamination, while females are more resistant to nitrate contamination than males. To ensure the drinking water safety in Zhangjiakou and its downstream areas, proper management and treatment of groundwater will be necessary to avoid the health risks associated with nitrate contamination.