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1.
J Colloid Interface Sci ; 675: 935-946, 2024 Jul 02.
Article in English | MEDLINE | ID: mdl-39002243

ABSTRACT

Generally, sulfur poisoning is considered to be one of the main factors contributing to the deactivation of selective catalytic reduction of NOx by CO (CO-SCR) catalysts, while the promotional effect of SO2 on NO reduction over Ir/SiO2 is observed which is an interesting scientific phenomenon. After the introduction of 20 ppm SO2, NOx conversion increased from âˆ¼ 40 % to âˆ¼ 90 % at 275 °C, and N2 selectivity increased from âˆ¼ 80 % to 100 % at 200 âˆ¼ 300 °C. Furthermore, the promoting effect could remain unchanged after 24 h of continuous reaction. However, the temperature point for achieving complete conversion of CO increased from 225 °C to 275 °C after the introduction of SO2. Experimental characterization and theoretical calculation jointly proved that the inhibition of CO oxidation by the generation of sulfate was the main reason for promoting NO reduction. Under the coexistence of O2 and SO2, SO2 was firstly oxidized to SO3 on the iridium surface and generated sulfate species on surface hydroxyl groups of SiO2. Some active sites for O2 adsorption were covered by the generated surface sulfate, and adsorbed CO was hard to react with adsorbed O2, resulting in Langmuir-Hinshelwood (L-H) reaction pathways for CO oxidation being inhibited. Therefore, unoxidized CO reacted with NO adsorbed species and generated N2O to generate N2 and CO2, improving NO reduction. This new insight has implications for understanding the promotional effect of SO2 on NO reduction with CO in the presence of O2.

2.
Sci Total Environ ; 920: 170748, 2024 Apr 10.
Article in English | MEDLINE | ID: mdl-38340848

ABSTRACT

Catalytic oxidation, an end-of-pipe treatment technology for effectively purifying volatile organic compounds (VOCs), has received widespread attention. The crux of catalytic oxidation lies in the development of efficient catalysts, with their optimization necessitating a comprehensive analysis of the catalytic reaction mechanism. Two-dimensional (2D) ultra-thin nanomaterials offer significant advantages in exploring the catalytic oxidation mechanism of VOCs due to their unique structure and properties. This review classifies strategies for regulating catalytic properties and typical applications of 2D materials in VOCs catalytic oxidation, in addition to their characteristics and typical characterization techniques. Furthermore, the possible reaction mechanism of 2D Co-based and Mn-based oxides in the catalytic oxidation of VOCs is analyzed, with a special focus on the synergistic effect between oxygen and metal vacancies. The objective of this review is to provide valuable references for scholars in the field.

3.
ACS Appl Mater Interfaces ; 16(3): 3593-3604, 2024 Jan 24.
Article in English | MEDLINE | ID: mdl-38215440

ABSTRACT

Mining the scientific literature, combined with data-driven methods, may assist in the identification of optimized catalysts. In this paper, we employed interpretable machine learning to discover ternary metal oxides capable of selective catalytic reduction of nitrogen oxides with ammonia (NH3-SCR). Specifically, we devised a machine learning framework utilizing extreme gradient boosting (XGB), identified for its optimal performance, and SHapley Additive exPlanations (SHAP) to evaluate a curated database of 5654 distinct metal oxide composite catalytic systems containing cerium (Ce) element, with records of catalyst composition and preparation and reaction conditions. By virtual screening, this framework precisely pinpointed a CeO2-MoO3-Fe2O3 catalyst with superior NOx conversion, N2 selectivity, and resistance to H2O and SO2, as confirmed by empirical evaluations. Subsequent characterization affirmed its favorable structural, chemical bulk properties and reaction mechanism. Demonstrating the efficacy of combining knowledge-driven techniques with experimental validation and analysis, our strategy charts a course for analogous catalyst discoveries.

4.
Environ Pollut ; 307: 119512, 2022 Aug 15.
Article in English | MEDLINE | ID: mdl-35605835

ABSTRACT

The iron and steel industry (ISI) is one of the most energy-intensive industries in China, which makes a substantial contribution to the emissions of air pollutants. Among the various manufacturing processes, sintering is the major emitting process, which shares over half of the emissions of sulfur dioxide (SO2), nitrogen oxide (NOx) and particulate matter (PM) for the entire industry. In this study we made a comprehensive evaluation of the air pollutant emissions from the sintering process of China's ISI in 2017 based on the Continuous Emission Monitoring System (CEMS) database and estimated the future reduction potentials. We found that there was a general decreasing trend of emission concentrations in the sintering flue gas in response to the strengthened emission control policies, but the mild increase of the oxygen content in the second half of the year flattened the decreasing trend, indicating the necessity for simultaneous control of the oxygen content in the flue gas. Despite the relative high standard-reaching rates of 90% to the emission concentration limits in GB 28662-2012, the standard-reaching rates to the ultra-low emission standards were only 12%, 40% and 27% for NOx, SO2 and PM respectively, with the lowest value mostly occurred in the western provinces. In 2017, the NOx, SO2 and PM emissions from the sintering process were 378.6 kt, 169.0 kt and 51.9 kt, respectively. If the ultra-low emission standards were met, the corresponding NOx, SO2 and PM emissions would decrease by 69.9%, 52.9%, and 56.4% respectively, illustrating large emission reducing potentials by achieving the ultra-low emission standards.


Subject(s)
Air Pollutants , Air Pollution , Air Pollutants/analysis , Air Pollution/analysis , Air Pollution/prevention & control , China , Environmental Monitoring , Iron , Oxygen , Particulate Matter/analysis , Steel
5.
Chemosphere ; 291(Pt 2): 132917, 2022 Mar.
Article in English | MEDLINE | ID: mdl-34793850

ABSTRACT

China is the largest iron and steel producer and consumer in the world. The iron and steel manufacture, especially the sintering process, is energy-intensive, and contributes substantially to air pollutant emissions in China. Compared with other regions, the Fenwei Plain, a coal base, has a heavy industry concentration, and high pollutant emission total amount. In addition, urban air pollution has rebounded, and the pollutants concentrations in many cities have increased rather than decreased. In this study, we investigated the inter-annual trends of particulate matter (PM), sulfur dioxide (SO2) and nitrogen oxide (NOx) from the sintering process of iron and steel industry (ISI) in the Fenwei Plain and the surrounding regions in China from 2014 to 2017 based on the Continuous Emission Monitoring System (CEMS). We found that the oxygen content of the flue gas is the key to judge whether the sintering flue gas air pollutant emission concentration can meet the standard. Therefore, we adopted the converted concentration by the reference oxygen content in the final analysis. Overall, the SO2 and PM emission concentrations exhibit a downward trend from 2014 to 2017, in response to the strengthening of the emission control policies and standards in the ISI, whereas the NOx emission concentration did not change significantly during the same period The emission factors (EFs) of PM, NOx and SO2 obtained in this study are lower than previous estimates. In 2017, the SO2 and PM emissions were 27% and 32% lower than the levels in 2014.While NOx was 22% higher than the level in 2014. Our study confirmed the effectiveness of current emission control policies and standards in the iron and steel sector. However, the levels of NOx emissions were still high until 2017, illustrating the urgent need for more advanced emission control technologies to further reduce NOx emissions from the sintering flue gas in China.


Subject(s)
Air Pollutants , Air Pollution , Air Pollutants/analysis , Air Pollution/analysis , China , Environmental Monitoring , Iron , Metallurgy , Particulate Matter/analysis , Steel
6.
Environ Sci Pollut Res Int ; 28(3): 2549-2571, 2021 Jan.
Article in English | MEDLINE | ID: mdl-33105009

ABSTRACT

Nitric oxides (NOx, which mainly include more than 90% NO) are one of the major air pollutants leading to a series of environmental problems, such as acid rain, haze, photochemical smog, etc. The selective catalytic oxidation of NO to NO2 (NO-SCO) is regarded as a key process for the development of selective catalytic reduction of NOx by ammonia (via fast selective catalytic reduction reaction) and also the simultaneous removal of multipollutant (pre-oxidation and post-absorption). Until now, scholars have developed various types of NO-SCO catalysts, dividing the main groups into noble metals (Pt, Pd, Ru, etc.), metal oxides (Mn-, Co-, Cr-, Ce-based, etc.), perovskite-type oxides (LaMnO3, LaCoO3, LaCeCoO3, etc.), carbon materials (activated carbon, carbon fiber, carbon nanotube, graphene, etc.), and zeolites (ion-exchanged ZSM-5, CHA, SAPO, MCM-41, etc.) in this review. This paper summarizes the recent progress of the above typical catalysts and mostly analyzes the catalytic performance for NO oxidation in terms of the H2O and/or SO2 resistances and also the influencing factors, and their reaction mechanisms are described in detail. Finally, this review points out the key problems and possible solutions of the current researches and presents the application prospects and future development directions of NO-SCO technology using the above typical catalysts.


Subject(s)
Nitric Oxide , Oxygen , Ammonia , Catalysis , Oxidation-Reduction
7.
Ultrason Sonochem ; 32: 336-342, 2016 09.
Article in English | MEDLINE | ID: mdl-27150779

ABSTRACT

Ultrasonic effect in the synthesis of catalysts of NiAl oxides prepared starting from the coprecipitation method of a hydrotalcite structure was evaluated in this work. Removal of carbonyl sulfide (COS) at low temperature over the hydrotalcite-derived oxides was studied. The samples were characterized by X-ray Diffraction (XRD), scanning electron microscope (SEM), N2 adsorption/desorption techniques, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and CO2 temperature-programmed desorption (TPD). It is found that hydrotalcite treated with ultrasonic has smaller average crystallite size and higher particle dispersion compared to hydrotalcite without ultrasonic treatment. As a result, mixed oxides derived from hydrotalcite treated with ultrasonic show more developed pore structure which is good for the physical adsorption of gaseous pollutant. The result of desulfuration test showed that removal efficiency of COS on the NiAl mixed oxides prepared by ultrasonic method (30min) is greater than that on the catalyst prepared without the ultrasonic irradiation assistance with the same aging time. One important reason for the high activity is that when the ultrasonic is used the number of weak basic sites (OH(-) groups) and moderate basic sites (M-O) was increased, whereas the number of strong basic sites (O(2-)) was decreased. Therefore, ultrasonic treatment promoted the COS hydrolysis and suppress the poisoning of the catalyst.

8.
Int J Clin Exp Med ; 8(3): 4328-34, 2015.
Article in English | MEDLINE | ID: mdl-26064349

ABSTRACT

OBJECTIVE: To evaluate the correlation of epicardial adipose tissue volume (EATV) with the coronary artery lesion and its severity. METHODS: Inpatients with suspicious stable angina of coronary heart lesion were recruited. For patients with coronary artery lesions in CTA, further coronary angiography (CAG) was performed to evaluate the coronary artery lesion. Gensini scoring system was employed to assess the severity of coronary artery lesions. RESULTS: Patients were classified as coronary heart disease (CHD) group (n = 160). Results showed the mean EATV was 192.57 ± 30.32 cm(3) in CHD group, which was significantly larger than that in control group (138.56 ± 23.18 cm(3); P < 0.01). The coronary artery stenosis was classified as mild, moderate and severe stenosis according to the extent of coronary artery lesions, and results showed marked difference in the EATV among patients with different severities of coronary artery stenosis (P < 0.005). The Gensini score was positively related to EATV (r = 0.285, P = 0.000). The EATV increased with the increase in the number of affected coronary arteries. Multivariate Logistic regression analysis showed EATV was an independent risk factor of CHD after adjusting other confounding factors (OR = 1.023, P = 0.013). CONCLUSION: EATV is closely related to the severity of coronary artery lesions: the larger the EATV, the more severe the coronary artery lesions. Moreover, EATV is an independent risk factor of CHD.

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