Changes in source composition of wet nitrate deposition after air pollution control in a typical area of Southeast China.

In recent years, China has adopted numerous policies and regulations to control NOx emissions to further alleviate the adverse impacts of NO3--N deposition. However, the variation in wet NO3--N deposition under such policies is not clear. In this study, the southeastern area, with highly developed industries and traditional agriculture, was selected to explore the variation in NO3--N deposition and its sources changes after such air pollution control through field observation and isotope tracing. Results showed that the annual mean concentrations of NO3--N in precipitation were 0.67 mg L-1 and 0.54 mg L-1 in 2014-2015 and 2021-2022, respectively. The average wet NO3--N depositions in 2014-2015 and 2021-2022 was 7.76 kg N ha-1 yr-1 and 5.03 kg N ha-1 yr-1, respectively, indicating a 35% decrease. The δ15N-NO3- and δ18O-NO3- values were lower in warm seasons and higher in cold seasons, and both showed a lower trend in 2021-2022 compared with 2014-2015. The Bayesian model results showed that the NOx emitted from coal-powered plants contributed 53.6% to wet NO3--N deposition, followed by vehicle exhaust (22.9%), other sources (17.1%), and soil emissions (6.4%) during 2014-2015. However, the contribution of vehicle exhaust (33.3%) overpassed the coal combustion (32.3%) and followed by other sources (25.4%) and soil emissions (9.0%) in 2021-2022. Apart from the control of air pollution, meteorological factors such as temperature, precipitation, and solar radiation are closely related to the changes in atmospheric N transformation and deposition. The results suggest phased achievements in air pollution control and that more attention should be paid to the control of motor vehicle exhaust pollution in the future, at the same time maintaining current actions and supervision of coal-powered plants.

Simultaneous removal of naphthalene and NOx over V-Ce/Ti catalyst: Design of separated active sites for naphthalene degradation and SCR reaction.

V-Ce/Ti catalysts were prepared for the removal of naphthalene and NOx in the flue gas. The adverse effects of NH3 and NO on the naphthalene degradation were weakened on V-Ce/Ti, resulting in a decrease of only 2.5 % in COx selectivity. The formation of high molecular weight byproducts was also reduced. Besides the acid sites on the catalysts, Ce introduced new Brønsted basic sites, which could also adsorb and degrade naphthalene into naphthol effectively. With the separated active sites for naphthalene degradation and NO removal, the reaction between NH3 and the intermediates during the naphthalene degradation was also inhibited, decreasing the formation and accumulation of phthalimide. The oxidation of the intermediates was promoted by active V5+ introduced by Ce, inhibiting the transformation of the intermediates to higher molecular weight byproducts. Nearly 100 % conversion of naphthalene and NO, as well as 40.1 % of the COx selectivity were obtained on V-Ce/Ti.

Hydrothermal-enhanced pyrolysis for efficient NOX reduction and biochar valorization from food waste digestate.

Pyrolysis has emerged as a promising technology for valorizing digestate resulting from the anaerobic digestion of food waste. However, the high NOX emissions during pyrolysis limit its application. This study proposed a hydrothermal coupled pyrolysis process to control the element transfer in digestate during biochar production. The efficient reduction of NOX emissions and the improvement of biochar adsorbability were realized. The hydrothermal process reduced the nitrogen content in solid digestate by 49.10 %-81.79 %, thus reducing the NOX precursors in syngas and the N-containing substances in bio-oil. Additionally, the specific surface area and the total pore volume of biochar were enhanced from 25 m2/g to 60-73 m2/g and 0.06 cm3/g to 0.12-0.14 cm3/g, respectively. More defects, oxygen-containing functional groups, and doped Ca on the biochar resulted in a high phosphate removal efficiency of 94 %. The proposed technology provides an efficient and environmentally friendly way to utilize the digestate.

Experimental assessment of pollutant emissions from residential fuel cells and comparative benchmark analysis.

Energy transition currently brings focus on fuel cell micro-combined heat and power (mCHP) systems for residential uses. The two main technologies already commercialized are the Proton Exchange Membrane Fuel Cells (PEMFCs) and Solid Oxide Fuel Cells (SOFCs). The pollutant emissions of one system of each technology have been tested with a portable probe both in laboratory and field-test configurations. In this paper, the nitrogen oxides (NOx), sulphur dioxide (SO2), and carbon monoxide (CO) emission levels are compared to other combustion technologies such as a recent Euro 6 diesel automotive vehicle, a classical gas condensing boiler, and a gas absorption heat pump. At last, a method of converting the concentration of pollutants (in ppm) measured by the sensors into pollutant intensity per unit of energy (in mg/kWh) is documented and reported. This allows for comparing the pollutant emissions levels with relevant literature, especially other studies conducted with other measuring sensors. Both tested residential fuel cell technologies fed by natural gas can be considered clean regarding SO2 and NOx emissions. The CO emissions can be considered quite low for the tested SOFC and even nil for the tested PEMFC. The biggest issue of natural gas fuel cell technologies still lies in the carbon dioxide (CO2) emissions associated with the fossil fuel they consume. The gas absorption heat pump however shows worse NOx and CO levels than the classical gas condensing boiler. At last, this study illustrates that the high level of hybridization between a fuel cell and a gas boiler may be responsible for unexpected ON/OFF cycling behaviours and therefore prevent both sub-systems from operating as optimally and reliably as they would have as standalone units.

Preparation of Mn/TiO2 catalysts using recovered manganese from spent alkaline batteries for low-temperature NH3-SCR.

Black mass (BM) from spent alkaline Zn-MnO2 batteries was used for the first time as a Mn source in the preparation of Mn/TiO2 catalysts for low-temperature NH3-selective catalytic reduction (SCR) of NOx. To recover Mn species and eliminate alkali and Zn species, BM powder underwent DI-water washing, followed by carbothermal reduction. The resulting slags were further dissolved in HNO3, loaded onto TiO2 particles with ball milling, and then subjected to calcination. Nearly 100% of Zn species were removed from the BM via carbothermal reduction at 950 °C for 4 h with 5.0 wt% activated carbon. The resulting catalyst, derived from the treated BM, achieved similar NOx conversion (97%) as the catalyst prepared using a reagent-grade Mn chemical at 160 °C but a higher NOx-to-N2 conversion rate at 78%. The promoted N2 selectivity was attributed to a high Mn4+/Ti ratio and the presence of impurities from BM, such as Fe3+ ions, which enhanced oxidation ability of the catalyst. Conversely, insufficient removal of Zn or carbon additives in the slags led to a decreased Mn concentration, an increased proportion of Mn2+/Mn3+ species, increased surface OH groups, and reduced oxidation ability on the surface, thus reducing NOx conversion and N2 selectivity.

Dual-course dielectric barrier discharge with a novel hollow micro-holes electrode to efficiently mitigate NOx.

The effect of a novel hollow annular micro-hole electrode on the DBD de-NOx performance was investigated. The experimental results show that the hollow electrode allows the feed gas to take full advantage of the redundant heat of the electrode, thus reducing the energy consumption of the system. Subsequently, the micro-hole structure can improve the uniformity of feed gas in the plasma channel and prolong the residence time of the feed gas in the plasma channel. The reactor can also raise the temperature of the feed gas and enhance the plasma electric field. The optimum NOx removal efficiency of about 82.6% is achieved at 16 annular micro-holes. Compared to the rod electrode reactor, the novel electrode reactor shows 19.7% reduction in energy consumption and 13.2% enhancement in de-NOx efficiency. The calculations of de-NOx mechanism show that the NO2 concentration decays significantly as the feed gas residence time increases, accompanied by a slight increase in N2O concentration. The NO2 concentration marginally increases while N2O concentration slightly decreases as the increase of feed gas temperature. DBD de-NOx presents the mode of accelerated reduction of NO, essential removal of NO2, and gradual consumption of N2O with the reduced electric field increases.

Deseasonalized trend of ground-level ozone and its precursors in an industrial city Kaohsiung, Taiwan.

Mitigating ground-level ozone (GLO) remains challenging due to its highly nonlinear formation process. Thus, understanding GLO pollution trends is crucial for developing effective control strategies, especially Kaohsiung industrial city, Taiwan. Based on the long-term monitoring data set of 2011-2022, temporal analysis reveals that monthly mean GLO peaks in autumn (40.66 ± 5.10 ppb), carbon monoxide (CO) and major precursors such as nitrogen oxides (NOx), nonmethane hydrocarbons (NMHC) reach their highest levels in winter. The distinct seasonal variation of air pollutants in Kaohsiung is primarily influenced by the unique blocking effect of the mountainous area under the northeasterly wind, as the city is situated downwind, causing high GLO levels during autumn due to the accumulation of stagnant air hindering the dispersion of pollutants. Over the 12 years (2011-2022), the deseasonalized trend analysis was conducted with p < 0.001, revealing a stabilization trend of GLO (+0.04 ppb/yr) from a previous sharp increase. The observed improvement is credited to a drastic decrease in total oxidants (Ox) at -0.63 ppb/yr due to significantly reducing their precursors. Furthermore, the effectiveness of precursor reduction is also supported by GLO daily maximum profile changes. While high GLO events (>120 ppb) decrease, days within midrange (60-80 ppb) rise from 24.4% to 33.3%. A notable difference emerges when comparing daytime and nighttime GLO. While daytime GLO decreased at -0.22 ppb/yr, nighttime GLO increased at +0.34 ppb/yr. Weakened nocturnal titration effects accounted for the nighttime increase. The distinct spatial variations in GLO trends on a citywide scale underscore that areas with complicated industrial activities may not benefit from a continuing reduction of precursors compared to less-polluted areas. The findings of this study hold significant implications for improving GLO control strategies in heavily industrialized city and provide valuable information to the general public about the current state of GLO pollution.

Identification of NOx emissions and source characteristics by TROPOMI observations - A case study in north-central Henan, China.

With the development of industries, air pollution in north-central Henan is becoming increasingly severe. The TROPOspheric Monitoring Instrument (TROPOMI) provides nitrogen dioxide (NO2) column densities with high spatial resolution. Based on TROPOMI, in this study, the nitrogen oxides (NOx) emissions in north-central Henan are derived and the emission hotspots are identified with the flux divergence method (FDM) from May to September 2021. The results indicate that Zhengzhou has the highest NOx emissions in north-central Henan. The most prominent hotspots are in Guancheng Huizu District (Zhengzhou) and Yindu District (Anyang), with emissions of 448.4 g/s and 300.3 g/s, respectively. The Gaussian Mixture Model (GMM) is applied to quantify the characteristics of emission hotspots, including the diameter, eccentricity, and tilt angle, among which the tilt angle provides a novel metric for identifying the spatial distribution of pollution sources. Furthermore, the results are compared with the CAMS global anthropogenic emissions (CAMS-GLOB-ANT) and Multi-resolution Emission Inventory model for Climate and air pollution research (MEIC), and they are generally in good agreement. However, some point sources, such as power plants, may be missed by both inventories. It is also found that for emission hotspots near transportation hubs, CAMS-GLOB-ANT may not have fully considered the actual traffic flow, leading to an underestimation of transportation emissions. These findings provide key information for the accurate implementation of pollution prevention and control measures, as well as references for future optimization of emission inventories. Consequently, deriving NOx emissions from space, quantifying the characteristics of emission hotspots, and combining them with bottom-up inventories can provide valuable insights for targeted emission control.

Synergistic catalytic removal of NOx and chlorinated organics through the cooperation of different active sites.

The synergistic removal of NOx and chlorinated volatile organic compounds (CVOCs) has become the hot topic in the field of environmental catalysis. However, due to the trade-off effects between catalytic reduction of NOx and catalytic oxidation of CVOCs, it is indispensable to achieve well-matched redox property and acidity. Herein, synergistic catalytic removal of NOx and chlorobenzene (CB, as the model of CVOCs) has been originally demonstrated over a Co-doped SmMn2O5 mullite catalyst. Two kinds of Mn-Mn sites existed in Mn-O-Mn-Mn and Co-O-Mn-Mn sites were constructed, which owned gradient redox ability. It has been demonstrated that the cooperation of different active sites can achieve the balanced redox and acidic property of the SmMn2O5 catalyst. It is interesting that the d band center of Mn-Mn sites in two different sites was decreased by the introduction of Co, which inhibited the nitrate species deposition and significantly improved the N2 selectivity. The Co-O-Mn-Mn sites were beneficial to the oxidation of CB and it cooperates with Mn-O-Mn-Mn to promote the synergistic catalytic performance. This work paves the way for synergistic removal of NOx and CVOCs over cooperative active sites in catalysts.

A machine learning-based ensemble model for estimating diurnal variations of nitrogen oxide concentrations in Taiwan.

Air pollution is inextricable from human activity patterns. This is especially true for nitrogen oxide (NOx), a pollutant that exists naturally and also as a result of anthropogenic factors. Assessing exposure by considering diurnal variation is a challenge that has not been widely studied. Incorporating 27 years of data, we attempted to estimate diurnal variations in NOx across Taiwan. We developed a machine learning-based ensemble model that integrated hybrid kriging-LUR, machine-learning, and an ensemble learning approach. Hybrid kriging-LUR was performed to select the most influential predictors, and machine-learning algorithms were applied to improve model performance. The three best machine-learning algorithms were suited and reassessed to develop ensemble learning that was designed to improve model performance. Our ensemble model resulted in estimates of daytime, nighttime, and daily NOx with high explanatory powers (Adj-R2) of 0.93, 0.98, and 0.94, respectively. These explanatory powers increased from the initial model that used only hybrid kriging-LUR. Additionally, the results depicted the temporal variation of NOx, with concentrations higher during the daytime than the nighttime. Regarding spatial variation, the highest NOx concentrations were identified in northern and western Taiwan. Model evaluations confirmed the reliability of the models. This study could serve as a reference for regional planning supporting emission control for environmental and human health.

Gd-modified Mn-Co oxides derived from layered double hydroxides for improved catalytic activity and H2O/SO2 tolerance in NH3-SCR of NOx reaction.

Metal oxides derived from layered double hydroxides (LDHs) are expected to obtain low-temperature denitrification (de-NOx) catalysts with high catalytic activity and H2O/SO2 tolerance in the selective catalytic reduction (SCR) of NOx with NH3. In current work, we successfully prepared Gd-modified Mn-Co metal oxides derived from Gd-modified Mn-Co LDHs. The resultant Gd-modified Mn-Co metal oxides exhibit excellent catalytic activity and high H2O/SO2 tolerance in the NH3-SCR de-NOx reaction. The reasons for the enhancement can be ascribed to the unique surface physicochemical properties inherited from LDHs and the modification of Gd, which increase the specific surface area, improve the relative content of Mn4+ and Co3+ on the surface, enhance the number of acidic sites, strengthen the reducibility of catalyst, resulting in the enhanced catalytic activity and H2O/SO2 tolerance. Additionally, it is demonstrated that the NH3-SCR de-NOx reaction occurred on the surface of Gd-modified Mn-Co oxides followed both Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanisms. This study provides us with a design approach to promote catalytic activity and H2O/SO2 tolerance through morphology control and rare earth modification.

Spatial and temporal variations of surface background ozone in China analyzed with the grid-stretching capability of GEOS-Chem High Performance.

Surface background ozone, defined as the ozone in the absence of domestic anthropogenic emissions, is important for developing emission reduction strategies. Here we apply the recently developed GEOS-Chem High Performance (GCHP) global atmospheric chemistry model with ∼0.5° stretched resolution over China to understand the sources of Chinese background ozone (CNB) in the metric of daily maximum 8 h average (MDA8) and to identify the drivers of its interannual variability (IAV) from 2015 to 2019. The GCHP ozone simulations over China are evaluated with an ensemble of surface and aircraft measurements. The five-year national-mean CNB ozone is estimated as 37.9 ppbv, with a spatially west-to-southeast downward gradient (55 to 25 ppbv) and a summer peak (42.5 ppbv). High background levels in western China are due to abundant transport from the free troposphere and adjacent foreign regions, while in eastern China, domestic formation from surface natural precursors is also important. We find greater importance of soil nitric oxides (NOx) than biogenic volatile organic compound emissions to CNB ozone in summer (6.4 vs. 3.9 ppbv), as ozone formation becomes increasingly NOx-sensitive when suppressing anthropogenic emissions. The percentage of daily CNB ozone to total surface ozone generally decreases with increasing daily total ozone, indicating an increased contribution of domestic anthropogenic emissions on polluted days. CNB ozone shows the largest IAV in summer, with standard deviations (seasonal means) of ∼5 ppbv over Qinghai-Tibet Plateau (QTP) and >3.5 ppbv in eastern China. CNB values in QTP are strongly correlated with horizontal circulation anomalies in the middle troposphere, while soil NOx emissions largely drive the IAV in the east. El Nino can inhibit CNB ozone formation in Southeast China by increased precipitation and lower temperature locally in spring, but enhance CNB in Southwest China through increased biomass burning emissions in Southeast Asia.

Characteristics of NOX and NH3 emissions from in-use heavy-duty diesel vehicles with various aftertreatment technologies in China.

Some in-use China IV and China V heavy-duty diesel vehicles (HDDVs) with selective catalytic reduction (SCR) systems probably fail to mitigate nitrogen oxide (NOX) emissions as expected. Meanwhile, these SCR-equipped HDDVs might emit excessive ammonia (NH3). To better understand the NOX and NH3 emissions from typical HDDVs in China, seventeen in-use vehicles with various emission-control technologies were tested by using laboratory chassis dynamometers. The results indicated that individual NOX and NH3 emissions from HDDV fleets widely varied owing to differences in aftertreatment performance. China V and VI HDDVs with effectively functioning SCRs could substantially control their NOX emissions to be below the corresponding emission limits (i.e., 4.0 and 0.69 g/kWh for China V and China VI vehicles, respectively) but with a potential risk of high NH3 emissions caused by diesel exhaust fluid (DEF) overdosing. Furthermore, higher vehicle speed and payload resulted in lower NOX emissions and possibly higher NH3 emissions from HDDVs with effectively functioning SCRs, while higher NOX emissions from tampered- and non-SCR HDDVs. NOX emissions from China VI HDDVs were more sensitive to cold starts compared to China V and earlier vehicles, but there was no significant discrepancy in NH3 emissions between cold- and hot-start tests.

Strong metal oxide-zeolite interactions during selective catalytic reduction of nitrogen oxides.

In response to the stricter EU VII emission standards and the "150 â„ƒ challenge", selective catalytic reduction by ammonia (NH3-SCR) catalysts for motor vehicles are required to achieve high NO conversion below 200 °C. Compounding metal oxides with zeolites is an important strategy to design the low-temperature SCR catalysts. Here, we original prepared Cu-SSZ-13 @ MnGdOx (Cu-Z @ MGO), which achieved over 90% NO conversion and 95% N2 selectivity at 150 â„ƒ. It has been demonstrated that a uniform mesoporous loaded layer of MGO grows on Cu-Z, and a recrystallization zone appears at the MGO-Cu-Z interface. We discover that the excellent low-temperature SCR activity derives from the strong metal oxide-zeolite interaction (SMZI) effects. The SMZI effects cause the anchor and high dispersion of MGO on the surface of Cu-Z. Driven by the SMZI effects, the Mn3+/Mn4+ redox cycle ensures the low and medium temperature-SCR activity and the Cu2+/Cu+ redox cycle guarantees the medium and high temperature-SCR activity. The introduction of MGO improves the reaction activity of -NH2 species adsorbed at Mn sites at 150 â„ƒ, achieving a cycle of reduction and oxidation reactions at low temperatures. This strategy of inducing SMZI effects of metal oxides and zeolites paves a way for development of high-performance catalysts.

Catalytic removal of gaseous pollutant NO using CO: Catalyst structure and reaction mechanism.

Carbon monoxide (CO) has recently been considered an ideal reducing agent to replace NH3 in selective catalytic reduction of NOx (NH3-SCR). This shift is particularly relevant in diesel engines, coal-fired industry, the iron and steel industry, of which generate substantial amounts of CO due to incomplete combustion. Developing high-performance catalysts remain a critical challenge for commercializing this technology. The active sites on catalyst surface play a crucial role in the various microscopic reaction steps of this reaction. This work provides a comprehensive overview and insights into the reaction mechanism of active sites on transition metal- and noble metal-based catalysts, including the types of intermediates and active sites, as well as the conversion mechanism of active molecules or atoms. In addition, the effects of factors such as O2, SO2, and alkali metals, on NO reduction by CO were discussed, and the prospects for catalyst design are proposed. It is hoped to provide theoretical guidance for the rational design of efficient CO selective catalytic denitration materials based on the structure-activity relations.

Redox mediators boost NOx reduction via trade-off electron charges using a cube-shaped (cMn@rGO) catalyst; mechanism and electrochemical study.

Gaseous pollutants like sulfur dioxide and nitrogen oxide(s) (SO2, NOx) have been increasing exponentially for the last two decades, which have had adverse effects on human health, aquatic life, and the environment. Recently, for air pollution taming, manganese/oxide (Mn/MnO) has become a very promising heterogeneous catalyst due to its environment-friendly, low-price, and remarkable catalytic abilities for toxic gases. In this work, cube-shaped Mn nanoparticles (cMn NPs) were decorated on the surface of reduced graphene oxide (rGO) by the solvothermal method. The resulting cMn@rGO composite was employed for electrochemical NOx reduction. However, the microscopic (TEM/HRTEM) and structural analysis were utilised to investigate the morphology and characteristics of the cMn@rGO composite. This electrochemical-based treatment for NOx reduction is employed by using electron shuttle or redox mediators. Here, four distinct redox mediators are used to address electrochemical obstacles, which effectively facilitate electron transportation and promoted NOx reduction on the electrode surface. These mediators not only significantly enhanced the NOx conversion into valuable products, i.e., N2 and N2O, but also made the process smooth with high performance. Among these mediators, neutral red (N.R) exhibited extraordinary potential in enhancing NOx reduction. The obtained results indicated that the remarkable catalytic performance (∼93%) of the cMn@rGO can be attributed to several factors, including the catalyst's three-dimensional architecture structure and abundant active sites. The designed catalyst (cMn@rGO) is not only cost-effective and sustainable but also exhibits excellent potential in effectively reducing NOx, which could be beneficial for large-scale NOx abatement.

Clay mineral as catalysis for controlling the nitrogen containing pollutants during sewage sludge pyrolysis.

Pyrolysis technology is considered one of the most promising processes for the environmentally friendly disposal of sewage sludge (SS), as it can neutralize pathogens, reduce hazardous substances, and promote the immobilization of heavy metals. However, nitrogen-containing gases produced in SS pyrolysis can be converted to nitrogen oxides, causing serious environmental pollution. In this study, we investigated the evolution of the nitrogen (N) element in rapid pyrolysis of SS and explored the effect of clay minerals (attapulgite, montmorillonite, and kaolin) in regulating N conversion. The results showed that the higher temperature (800 °C) could promote the conversion of pyrroles/pyridines and NOx precursors in char to N2 (the conversion rate was 32.76 %), and clay minerals catalyzed the cleavage of N-containing macromolecules in the bio-oil, reducing the N content in bio-oil from 28.70 % to 6.23 %, and was conducted to realize the denitrification of bio-oil. Notably, the attapulgite (ATP) on N migration was more effective and could reduce the yield of NOx precursors from 23.80 % to 10.55 % by capturing NH4* and inhibiting the secondary reaction, while catalyzing the removal of N2 from pyridine/pyrrole (N2 production increased to 34.38 %). MgO and CaO in the clays played a major role in facilitating the conversion of char-N to N2, and clay structures loading on the biochar surface promoted the catalysis of N-containing volatiles to N2 by metal oxides. This study provides a viable and harmless approach to SS minimization.

Effects of impregnation sequence on the NH3-SCR activity and hydrothermal stability of a Ce-Nb/SnO2 catalyst.

Hydrothermal stability is crucial for the practical application of deNOx catalyst on diesel vehicles, for the selective catalytic reduction of NOx with NH3 (NH3-SCR). SnO2-based materials possess superior hydrothermal stability, which is attractive for the development of NH3-SCR catalyst. In this work, a series of Ce-Nb/SnO2 catalysts, with Ce and Nb loading on SnO2 support, were prepared by impregnation method. It was found that, the NH3-SCR activities and hydrothermal stabilities of the Ce-Nb/SnO2 catalysts significantly varied with the impregnation sequences, and the Ce-Nb(f)/SnO2 catalyst that firstly impregnated Nb and then impregnated Ce exhibited the best performance. The characterization results revealed that Ce-Nb(f)/SnO2 possessed appropriate acidity and redox capability. Furthermore, the strong synergistic effect between Nb and Sn species stabilized the structure and maintained the dispersion of acid sites. This study may provide a new understanding for the effect of impregnation sequence on activity and hydrothermal stability and a new environmental-friendly NH3-SCR catalyst with potential applications for NOx removal from diesel and hydrogen-fueled engines.

Research on ozone formation sensitivity based on observational methods: Development history, methodology, and application and prospects in China.

Observation-based method for O3 formation sensitivity research is an important tool to analyze the causes of ground-level O3 pollution, which has broad application potentials in determining the O3 pollution formation mechanism and developing prevention and control strategies. This paper outlined the development history of research on O3 formation sensitivity based on observational methods, described the principle and applicability of the methodology, summarized the relative application results in China and provided recommendations on the prevention and control of O3 pollution in China based on relevant study results, and finally pointed out the shortcomings and future development prospects in this field in China. The overview study showed that the O3 formation sensitivity in some urban areas in China in recent years presented a gradual shifting tendency from the VOC-limited regime to the transition regime or the NOx-limited regime due to the implementation of the O3 precursors emission reduction policies; O3 pollution control strategies and precursor control countermeasures should be formulated based on local conditions and the dynamic control capability of O3 pollution control measures should be improved. There are still some current deficiencies in the study field in China. Therefore, it is recommended that a stereoscopic monitoring network for atmospheric photochemical components should be further constructed and improved; the atmospheric chemical mechanisms should be vigorously developed, and standardized methods for determining the O3 formation sensitivity should be established in China in the near future.

Design of Ca-type todorokite catalysts with highly active for the selective reduction of NOx by NH3 at low temperatures.

Ca-type todorokite catalysts were designed and prepared by a simple redox method and applied to the selective reduction of NOx by NH3 (NH3-SCR) for the first time. Compared with the Na-type manjiroite prepared by the same method, the todorokite catalysts with different Mn/Ca ratios showed greatly improved catalytic activity for NOx reduction. Among them, Mn8Ca4 catalyst exhibited the best NH3-SCR performance, achieving 90% NOx conversion within temperature range of 70-275°C and having a high sulphur resistance. Compared to the Na-type manjiroite sample, Ca-type todorokite catalysts possessed an increased size of tunnel, resulting in a larger specific surface area. As increased the amounts of Ca doping, the Na content in Ca-type todorokite catalysts significantly decreased, providing larger amounts of Brønsted acid sites for NH3 adsorption to produce NH4+. The NH4+ species were highly active for reaction with NO + O2, playing a determining role in NH3-SCR process at low temperatures. Meanwhile, larger amounts of surface adsorbed oxygen contained over the Ca-doping samples than that over Na-type manjiroite, promoting the oxidation of NO and fast SCR processes. Over the Ca-type todorokite catalysts, furthermore, nitrates produced during the flow of NO + O2, were more active for reaction with NH3 than that over Na-type manjiroite, benefiting the occurrence of NH3-SCR process. This study provides novel insights into the design of NH3-SCR catalysts with high performance.