Ammonia has emerged as a promising hydrogen carrier with applications as an energy source in recent years. However, in addition to being toxic, gaseous ammonia is a precursor of secondary inorganic aerosols. The concentration of ambient fine particulate matter (PM2.5) is intrinsically connected to public health. In this study, PM2.5-related health impacts of utilizing ammonia-hydrogen energy in Kanto Region, Japan, were investigated. It was assumed that 20% of the electricity consumption in Kanto Region, the most populated area in Japan, was supplied by ammonia-hydrogen energy. The PM2.5 resulted from incomplete ammonia decomposition was simulated by a chemical transport model: ADMER-PRO (modified version). Based on the incremental PM2.5 concentration, health impacts on the elderly (individuals over 65 years old) were quantitatively evaluated. The ammonia emission in this scenario increased PM2.5 by 11.7% (0.16 μg·m–3·y–1) in winter and 3.5% (0.08 μg ·m–3·y–1) in summer, resulting in 351 premature deaths per year. This study suggests that costeffective emissions control or treatment and appropriate land planning should be considered to reduce the associated health impacts of this type of energy generation. In addition, further in-depth research, including cost-benefit analysis and security standards, is needed.
A sampling campaign including summer, autumn and winter of 2014 and spring of 2015 was accomplished to obtain the characteristic of chemical components in PM2.5 at three sites of Kunming, a plateau city in South-west China. Nine kinds of water-soluble inorganic ions (WSI), organic and element carbon (OC and EC) in PM2.5 were analyzed by ion chromatography and thermal optical reflectance method, respectively. Results showed that the average concentrations of total WSI, OC and EC were 22.85±10.95 µg·m-3, 17.83±9.57 µg·m-3 and 5.11±4.29 µg·m-3, respectively. They totally accounted for 53.0% of PM2.5. Secondary organic and inorganic aerosols (SOA and SIA) were also assessed by the minimum ratio of OC/EC, nitrogen and sulfur oxidation ratios. The annual average concentrations of SOA and SIA totally accounted for 28.3% of the PM2.5 concentration. The low proportion suggested the primary emission was the main source of PM2.5 in Kunming. However, secondary pollution in the plateau city should also not be ignorable, due to the appropriate temperature and strong solar radiation, which can promote the atmospheric photochemical reactions.
The objective of this paper is to propose a hybrid approach for the source apportionment of primary and secondary species of PM2.5 in the city of Tangshan. The receptor-based PMF (Positive Matrix Factorization) is integrated with the emission inventory (EI) to form the first hybrid method for the source apportionment of the primary species. The hybrid CAMx-PSAT-CP (Comprehensive Air Quality Model with Extensions–Particulate Source Apportionment Technology–Chemical Profile) approach is then proposed and used for the source apportionment of the secondary species. The PM2.5 sources identified for Tangshan included the soil dust, the metallurgical industry, power plants, coalfired boilers, vehicles, cement production, and other sources. It is indicated that the PM2.5 pollution is a regional issue. Among all the identified sources, the metallurgy industry was the biggest contribution source to PM2.5, followed by coal-fired boilers, vehicles and soil dust. The other-source category plays a crucial role for PM2.5, particularly for the formation of secondary species and aerosols, and these other sources include non-specified sources such as agricultural activities, biomass combustion, residential emissions, etc. The source apportionment results could help the local authorities make sound policies and regulations to better protect the citizens from the local and regional PM2.5 pollution. The study also highlights the strength of utilizing the proposed hybrid approaches in the identification of PM2.5 sources. The techniques used in this study show considerable promise for further application to other regions as well as to identify other source categories of PM2.5.
Seasonal pattern of transport pathways and potential sources of PM2.5 in Chengdu during 2012–2013 were investigated based on hourly PM2.5 data, backward trajectories, clustering analysis, potential source contribution function (PSCF), and concentration-weighted trajectory (CWT) method. The annual hourly mean PM2.5 concentration in Chengdu was 97.4 mg·m–3. 5, 5, 5 and 3 mean clusters were generated in four seasons, respectively. Short-distance air masses, which travelled within the Sichuan Basin with no specific source direction and relatively high PM2.5 loadings (>80 mg·m–3) appeared as important pathways in all seasons. These short pathways indicated that emissions from both local and surrounding regions of Chengdu contributed significantly to PM2.5 pollution. The cities in southern Chengdu were major potential sources with PSCF>0.6 and CWT>90 mg·m–3. The northeastern pathway prevailed throughout the year with higher frequency in autumn and winter and lower frequency in spring and summer. In spring, long-range transport from southern Xinjiang was a representative dust invasion path to Chengdu, and the CWT values along the path were 30-60 mg·m–3. Long-range transport was also observed in autumn from southeastern Xinjiang along a northwesterly pathway, and in winter from the Tibetan Plateau along a westerly pathway. In summer, the potential source regions of Chengdu were smaller than those in other seasons, and no long-range transport pathway was observed. Results of PSCF and CWT indicated that regions in Qinghai and Tibet contributed to PM2.5 pollution in Chengdu as well, and their CWT values increased to above 30 mg·m–3 in winter.
Industrial coal-fired boiler is an important air pollutant emission source in China. The chain-grate boiler is the most extensively used type of industrial coal-fired boiler. An electrical low-pressure impactor, and a Dekati® Low Pressure Impactor were applied to determine mass and number size distributions of PM10 at the inlet and the outlet of the particulate emission control devices at six coalfired chain-grate boilers. The mass size distribution of PM10 generated from coal-fired chain-grate boilers generally displays a bimodal distribution that contains a submicron mode and a coarse mode. The PM in the submicron mode for burning with raw coal contributes to 33% ± 10 % of PM10 emissions, much higher than those for pulverized boilers. And the PM in the submicron mode for burning with briquette contributes up to 86 % of PM10 emissions. Multiclones and scrubbers are not efficient for controlling PM10 emission. Their average collection efficiencies for sub-micron particle and super-micron particle are 34% and 78%, respectively. Operating conditions of industrial steam boilers have influence on PM generation. Peak of the submicron mode during normal operation period is larger than the start-up period.
Direct individual analysis using Scanning Electron Microscopy combined with online observation was conducted to examine the S-rich particles in PM2.5 of two typical polluted haze episodes in summer and winter from 2014 to 2015 in Beijing. Four major types of S-rich particles, including secondary CaSO4 particles (mainly observed in summer), S-rich mineral particles (SRM), S-rich water droplets (SRW) and (C, O, S)-rich particles (COS) were identified.We found the different typical morphologies and element distributions of S-rich particles and considered that (C, O, S)-rich particles had two major mixing states in different seasons. On the basis of the S-rich particles’ relative abundances, S concentrations and their relationships with PM2.5 as well as the seasonal comparison, we revealed that the S-participated formation degrees of SRM and SRW would enhance with increasing PM2.5 concentration. Moreover, C-rich matter and sulfate had seasonally different but significant impacts on the formation of COS.
Because the efficiency of biological nutrient removal is always limited by the deficient carbon source for the low carbon/nitrogen (C/N) ratio in real domestic sewage, the denitrifying phosphorus removal (DNPR) was developed as a simple and efficient method to remove nitrogen and phosphorous. In addition, this method has the advantage of saving aeration energy while reducing the sludge production. In this context, a pre-denitrification anaerobic/anoxic/post-aeration + nitrification sequence batch reactor (pre-A2NSBR) system, which could also reduce high ammonia effluent concentration in the traditional two-sludge DNPR process, is proposed in this work. The pre-A2NSBR process was mainly composed of a DNPR SBR and a nitrifying SBR, operating as alternating anaerobic/anoxic/post-aeration + nitrification sequence. Herein, the long-term performance of different nitrate recycling ratios (0–300%) and C/N ratios (2.5–8.8), carbon source type, and functional microbial community were studied. The results showed that the removal efficiency of total inorganic nitrogen (TIN, including NH4+-N, NO2– -N, and NO3– -N) gradually increased with the nitrate recycling ratios, and the system reached the highest DNPR efficiency of 94.45% at the nitrate recycling ratio of 300%. The optimum C/N ratio was around 3.9–7.3 with a nitrogen and phosphorus removal efficiency of 80.15% and 93.57%, respectively. The acetate was proved to be a high-quality carbon source for DNPR process. The results of fluorescence in situ hybridization (FISH) analysis indicated that nitrifiers and phosphorus accumulating organisms (PAOs) were accumulated with a proportion of 19.41% and 26.48%, respectively.
In this study, FeVO4 was prepared and used as Fenton-like catalyst to degrade orange G (OG) dye. The removal of OG in an aqueous solution containing 0.5 g·L–1 FeVO4 and 15 mmol·L–1 hydrogen peroxide at pH 7.0 reached 93.2%. Similar rates were achieved at pH 5.7 (k = 0.0471 min–1), pH 7.0 (k = 0.0438 min–1), and pH 7.7 (k = 0.0434 min–1). The FeVO4 catalyst successfully overcomes the problem faced in the heterogeneous Fenton process, i.e., the narrow working pH range. The data for the removal of OG in FeVO4 systems containing H2O2 conform to the Langmuir–Hinshelwood model (R2 = 0.9988), indicating that adsorption and surface reaction are the two basic mechanisms for OG removal in the FeVO4–H2O2 system. Furthermore, the irradiation of FeVO4 by visible light significantly increases the degradation rate of OG, which is attributed to the enhanced rates of the iron cycles and vanadium cycles.
This work presents an overall introduction to the Station for Observing Regional Processes of the Earth System–SORPES in Nanjing, East China, and gives an overview about main scientific findings in studies of air pollution-weather/climate interactions obtained since 2011. The main results summarized in this paper include overall characteristics of trace gases and aerosols, chemical transformation mechanisms for secondary pollutants like O3, HONO and secondary inorganic aerosols, and the air pollution–weather/climate interactions and feedbacks in mixed air pollution plumes from sources like fossil fuel combustion, biomass burning and dust storms. The future outlook of the development plan on instrumentation, networking and data-sharing for the SORPES station is also discussed.
Effect of different carbon sources on purification performance and change of microbial community structure in a novel A2N-MBR process were investigated. The results showed that when fed with acetate, propionate or acetate and propionate mixed (1:1) as carbon sources, the effluent COD, NH4+-N, TN and TP were lower than 30, 5, 15 and 0.5 mg?L–1, respectively. However, taken glucose as carbon source, the TP concentration of effluent reached 2.6 mg?L–1. Process analysis found that the amount of anaerobic phosphorus release would be the key factor to determine the above effectiveness. The acetate was beneficial to the growth of Candidatus Accumulibacter associated with biological phosphorus removal, which was the main cause of high efficiency phosphorus removal in this system. In addition, it could eliminate the Candidatus Competibacter associated with glycogen-accumulating organisms and guarantee high efficiency phosphorus uptake of phosphorus accumulating organisms in the system with acetate as carbon source.
First-principles calculations were performed to investigate the mechanism of Hg0 adsorption and oxidation on CeO2(111). Surface oxygen activated by the reduction of Ce4+ to Ce3+ was vital to Hg0 adsorption and oxidation processes. Hg0 was fully oxidized by the surface lattice oxygen on CeO2(111), without using any other oxidizing agents. HCl could dissociate and react with the Hg adatom on CeO2(111) to form adsorbed Hg–Cl or Cl–Hg–Cl groups, which promoted the desorption of oxidized Hg and prevented CeO2 catalyst deactivation. In contrast, O–H and H–O–H groups formed during HCl adsorption consumed the active surface oxygen and prohibited Hg oxidation. The consumed surface oxygen was replenished by adding O2 into the flue gas. We proposed that oxidized Hg desorption and maintenance of sufficient active surface oxygen were the rate-determining steps of Hg0 removal on CeO2-based catalysts. We believe that our thorough understanding and new insights into the mechanism of the Hg0 removal process will help provide guidelines for developing novel CeO2-based catalysts and enhance the Hg0 removal efficiency.
To understand the pollution characteristics of particulate matter emitted from outdoor barbecue cooking in eastern China, measurements of the PM2.5 mass concentration, the number concentration of particles with a diameter of 0.01 to 1.0 μm, and the particle size distribution from 0.3 to 25 μm were carried out at seven barbecue restaurants in urban Jinan. The average PM2.5 mass concentration and sub-micron particle number concentrations at a distance of 1 m from the grills were 250 to 1083 μg/m3 and 0.90 × 105 to 2.23 × 105 cm–3, respectively, which were much higher than those in the ambient air of the urban area. Compared to the ambient atmosphere, barbecue cooking emitted very high levels of particles with a larger increase in the concentrations of super-micron particles than that of sub-micron particles. The super-micron particle number concentrations at the barbecue restaurants were 10 to 100 times higher than those observed in the ambient urban atmosphere. The barbecue smoke had a significant effect on the particle concentrations in the surrounding region. Both mass and number concentrations of particles exhibited maximum values immediately near the barbecue grills and often reached a peak at a distance of 10 to 15 m. The removal efficiency of a range hood for the cooking particles was tested in an indoor kitchen. The range hood effectively cleaned the particulate matter pollution caused by cooking with a removal efficiency larger than 80%. Therefore, the use of a range hood is recommended for outdoor barbecue restaurants coupled with a smoke purifier to clean the emitted high concentrations of particles.
The purpose of this work is to study the co-cultivation of Chlorella sp. and wastewater wild algae under different cultivation conditions (i.e. CO2, light intensity, cultivation time, and inoculation ratio) for enhanced algal biomass and lipid productivity in wastewater medium using Response Surface Methodology (RSM). The results show that mixed cultures of Chlorella sp. and wastewater wild algae increase biomass and lipid yield. Additionally, findings indicate that CO2, light intensity and cultivation time significantly affect algal productivity. Furthermore, CO2 concentration and light intensity, and CO2 concentration and algal composition, have an interactive effect on biomass productivity. Under different cultivation conditions, the response of algal biomass, cell count, and lipid productivity ranges from 2.5 to 10.2 mg/mL, 1.1 × 106 to 8.2 × 108 cells/mL, and 1.1 × 1012 to 6.8 × 1012 total fluorescent units/mL, respectively. The optimum conditions for simultaneous biomass and lipid accumulation are 3.6% of CO2 (v/v), 160 µmol/m2/s of light intensity, 1.6/2.4 of inoculation ratio (wastewater-algae/Chlorella), and 8.3 days of cultivation time. The optimal productivity is 9.8 (g/L) for dry biomass, 8.6 E + 08 (cells/mL) for cell count, and 6.8 E + 12 (Total FL units per mL) for lipid yield, achieving up to four times, eight times, and seven times higher productivity compared to nonoptimized conditions. Provided is a supportive methodology to improve mixed algal culture for bioenergy feedstock generation and to optimize cultivation conditions in complex wastewater environments. This work is an important step forward in the development of sustainable large-scale algae cultivation for cost-efficient generation of biofuel.
Porous carbon material facilitates the reaction SO2 + O2 + H2O → H2SO4 in coal-burned flue gas for sulfur resources recovery at mild conditions. It draws a long-term mystery on its heterogeneous catalysis due to the complicated synergic effect between its microstructure and chemical components. To decouple the effects of geometric structure from chemical components, classical molecular dynamics method was used to investigate the static and dynamic characteristics of the reactants (H2O, SO2 and O2) in the confined space truncated by double-layer graphene (DLG). Strong adsorption of SO2 and O2 by the DLG was observed, which results in the filling of the solute molecules into the interior of the DLG and the depletion of H2O. This effect mainly results from the different affinity of the DLG to the species and can be tuned by the separation of the two graphene layers. Such dimension dependence of the static and dynamic properties like distribution profile, molecular cluster, hydrogen bond and diffusion coefficient were also studied. The conclusions drawn in this work could be helpful to the further understanding of the underlying reaction mechanism of desulfurization process in porous carbon materials and other applications of carbon-based catalysts.
Heterogeneous Fenton-like reaction has been extensively investigated to eliminate refractory organic contaminants in wastewater, but it usually shows low catalytic performance due to difficulty in reduction from Fe(III) to Fe(II). In this study, enhanced catalytic efficiency was obtained by employing Cu-doped BiFeO3 as heterogeneous Fenton-like catalysts, which exhibited higher catalytic performance toward the activation of H2O2 for phenol degradation than un-doped BiFeO3. BiFe0.8Cu0.2O3 displayed the best performance, which yielded 91% removal of phenol (10 mg L–1) in 120 min. The pseudo first-order kinetic rate constant of phenol degradation in BiFe0.8Cu0.2O3 catalyzed heterogeneous Fenton-like reaction was 5 times higher than those of traditional heterogeneous Fenton-like catalysts, such as Fe3O4 and goethite. The phenol degradation efficiency could still reach 83% after 4 cycles, which implied the good stability of BiFe0.8Cu0.2O3. The high catalytic activity of BiFe0.8Cu0.2O3 was attributed to the fact that the doping Cu into BiFeO3 could promote the generation of Fe(II) in the catalyst and then facilitate the activation of H2O2 to degrade the organic pollutants.
We implemented the online coupled WRF-Chem model to reproduce the 2013 January haze event in North China, and evaluated simulated meteorological and chemical fields using multiple observations. The comparisons suggest that temperature and relative humidity (RH) were simulated well (mean biases are–0.2K and 2.7%, respectively), but wind speeds were overestimated (mean bias is 0.5 m?s–1). At the Beijing station, sulfur dioxide (SO2) concentrations were overpredicted and sulfate concentrations were largely underpredicted, which may result from uncertainties in SO2 emissions and missing heterogeneous oxidation in current model. We conducted three parallel experiments to examine the impacts of doubling SO2 emissions and incorporating heterogeneous oxidation of dissolved SO2 by nitrogen dioxide (NO2) on sulfate formation during winter haze. The results suggest that doubling SO2 emissions do not significantly affect sulfate concentrations, but adding heterogeneous oxidation of dissolved SO2 by NO2 substantially improve simulations of sulfate and other inorganic aerosols. Although the enhanced SO2 to sulfate conversion in the HetS (heterogeneous oxidation by NO2) case reduces SO2 concentrations, it is still largely overestimated by the model, indicating the overestimations of SO2 concentrations in the North China Plain (NCP) are mostly due to errors in SO2 emission inventory.
A new type of Au/TiO2/reduced graphene oxide (RGO) nanocomposite was fabricated by the hydrothermal synthesis of TiO2 on graphene oxide followed by the photodeposition of Au nanoparticles. Transmission electron microscopy images showed that Au nanoparticles were loaded onto the surface of both TiO2 and RGO. Au/TiO2/RGO had a better photocatalytic activity than Au/ TiO2 for the degradation of phenol. Electrochemical measurements indicated that Au/TiO2/RGO had an improved charge transfer capability. Meanwhile, chemiluminescent analysis and electron spin resonance spectroscopy revealed that Au/TiO2/RGO displayed high production of hydrogen peroxide and hydroxyl radicals in the photocatalytic process. This high photocatalytic performance was achieved via the addition of RGO in Au/TiO2/RGO, where RGO served not only as a catalyst support to provide more sites for the deposition of Au nanoparticles but also as a collector to accept electrons from TiO2 to effectively reduce photogenerated charge recombination.
In this study, a new water treatment system that couples (photo-) electrochemical catalysis (PEC or EC) in a microbial fuel cell (MFC) was configured using a stainless-steel (SS) cathode coated with Fe0/TiO2. We examined the destruction of methylene blue (MB) and tetracycline. Fe0/TiO2 was prepared using a chemical reduction-deposition method and coated onto an SS wire mesh (500 mesh) using a sol technique. The anode generates electricity using microbes (bio-anode). Connected via wire and ohmic resistance, the system requires a short reaction time and operates at a low cost by effectively removing 94% MB (initial concentration 20 mg?L–1) and 83% TOC/TOC0 under visible light illumination (50 W; 1.99 mW?cm–2 for 120 min, MFC-PEC). The removal was similar even without light irradiation (MFC-EC). The EEo of the MFC-PEC system was approximately 0.675 kWh?m–3?order–1, whereas that of the MFC-EC system was zero. The system was able to remove 70% COD in tetracycline solution (initial tetracycline concentration 100 mg?L–1) after 120 min of visible light illumination; without light, the removal was 15% lower. The destruction of MB and tetracycline in both traditional photocatalysis and photoelectrocatalysis systems was notably low. The electron spinresonance spectroscopy (ESR) study demonstrated that ?OH was formed under visible light, and ?O2– was formed without light. The bio-electricity-activated O2 and ROS (reactive oxidizing species) generation by Fe0/TiO2 effectively degraded the pollutants. This cathodic degradation improved the electricity generation by accepting and consuming more electrons from the bio-anode.
The photolysis frequency of NO2, j(NO2), is an important analytical parameter in the study of tropospheric chemistry. A chemical actinometer (CA) was built to measure the ambient j(NO2) based on a high precision NOx instrument with 1 min time resolution. Parallel measurements of the ambient j(NO2) by using the CA and a commercial spectroradiometer (SR) were conducted at a typical urban site (Peking University Urban Environmental Monitoring Station) in Beijing. In general, good agreement was achieved between the CA and SR data with a high linear correlation coefficient (R2 = 0.977) and a regression slope of 1.12. The regression offset was negligible compared to the measured signal level. The j(NO2) data were calculated using the tropospheric ultraviolet visible radiation (TUV) model, which was constrained to observe aerosol optical properties. The calculated j(NO2) was intermediate between the results obtained with CA and SR, demonstrating the consistency of all the parameters observed at this site. The good agreement between the CA and SR data, and the consistency with the TUV model results, demonstrate the good performance of the installed SR instrument. Since a drift of the SR sensitivity is expected by the manufacturer, we propose a regular check of the data acquired via SR against those obtained by CA for long-term delivery of a high quality series of j(NO2) data. Establishing such a time series will be invaluable for analyzing the long-term atmospheric oxidation capacity trends as well as O3 pollution for urban Beijing.
The gene for the catalytic domain of thermostable endo-β-1,3-glucanase (laminarinase) LamA was cloned from Thermotoga maritima MSB8 and heterologously expressed in a bioengineered Synechococcus sp. PCC 7002. The mutant strain was cultured in a photobioreactor to assess biomass yield, recombinant laminarinase activity, and CO2 uptake. The maximum enzyme activity was observed at a pH of 8.0 and a temperature of 70°C. At a CO2 concentration of 5%, we obtained a maximum specific growth rate of 0.083 h–1, a biomass productivity of 0.42 g?L–1?d–1, a biomass concentration of 3.697 g?L–1, and a specific enzyme activity of the mutant strain of 4.325 U?mg–1 dry mass. All parameters decreased as CO2 concentration increased from 5% to 10% and further to 15% CO2, except enzyme activity, which increased from 5% to 10% CO2. However, the mutant culture still grew at 15% CO2 concentration, as reflected by the biomass productivity (0.26 g?L–1?d–1), biomass concentration (2.416 g?L–1), and specific enzyme activity (3.247 U?mg–1 dry mass).
