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1.
Chemosphere ; 361: 142517, 2024 Jun 01.
Article in English | MEDLINE | ID: mdl-38830464

ABSTRACT

Indoor volatile formaldehyde is a serious health hazard. The development of low-temperature and efficient nonhomogeneous oxidation catalysts is crucial for protecting human health and the environment but is also quite challenging. Single-atom catalysts (SACs) with active centers and coordination environments that are precisely tunable at the atomic level exhibit excellent catalytic activity in many catalytic fields. Among two-dimensional materials, the nonmagnetic monolayer material g-C3N4 may be a good platform for loading single atoms. In this study, the effect of nitrogen defect formation on the charge distribution of g-C3N4 is discussed in detail using density functional theory (DFT) calculations. The effect of nitrogen defects on the activated molecular oxygen of Pt/C3N4 was systematically revealed by DFT calculations in combination with molecular orbital theory. Two typical reaction mechanisms for the catalytic oxidation of formaldehyde were proposed based on the Eley-Rideal (E-R) mechanism. Pt/C3N4-V3N was more advantageous for path 1, as determined by the activation energy barrier of the rate-determining step and product desorption. Finally, the active centers and chemical structures of Pt/C3N4 and Pt/C3N4-V3N were verified to have good stability at 375 K by determination of the migration energy barriers and ab initio molecular dynamics simulations. Therefore, the formation of N defects can effectively anchor single-atom Pt and provide additional active sites, which in turn activate molecular oxygen to efficiently catalyze the oxidation of formaldehyde. This study provides a better understanding of the mechanism of formaldehyde oxidation by single-atom Pt catalysts and a new idea for the development of Pt as well as other metal-based single-atom oxidation catalysts.

2.
J Hazard Mater ; 474: 134710, 2024 May 23.
Article in English | MEDLINE | ID: mdl-38820758

ABSTRACT

Indoor formaldehyde pollution seriously jeopardizes human health. The development of efficient and stable non-precious metal catalysts for low-temperature catalytic degradation of formaldehyde is a promising approach. In this study, TiO2 {001} and {101} supports were loaded with different ratios of Mn and Ce active components, and the effects of the ratios of the active components on the catalytic activity were investigated. The elemental oxidation states, redox capacities, active oxygen mobilities and acid site distributions of the catalysts were determined using characterization techniques such as XPS, H2-TPR, O2-TPD, and NH3-TPD. In situ infrared spectroscopy was utilized to reveal the differences in the two-step dehydrogenation reactions of dioxymethylene (DOM) in 5Mn1Ce/Ti-NS and 5Mn1Ce/Ti-NP. Density-functional theory was used to investigate the differences in the catalytic steps and maximum energy barriers of Mn-Ce/Ti-NS and Mn-Ce/Ti-NP for HCHO. The differences in catalytic activity due to the influence of the manganese and cerium active components on the {001} and {101} crystal faces of anatase titanium dioxide are comprehensively revealed. Exposure of the supported crystalline surfaces alters the catalytic activity centers and reaction pathways at the molecular level. This study provides experimental and theoretical guidance for the selection of exposed crystalline surfaces for loaded catalysts.

3.
J Hazard Mater ; 470: 134141, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38583201

ABSTRACT

Coal combustion is the major contributor to global toxic selenium (Se) emissions. Inorganic elements in coals significantly affect Se partitioning during combustion. This work confirmed that the calcium (Ca) in ash had a stronger relationship with Se retention at 1300 °C than other major elements. Ca oxide chemically reacted with gaseous Se, and its sintering densification slightly affected Se adsorption capacities (44.45 -1840.71→35.17 -1540.15 mg/kg) at 300 - 1300 °C. Therefore, Ca in coals was identified as having potential for hindering gaseous Se emissions, and coals with increased Ca contents (2.74→5.19 wt%) were used in a 350 MW unit. The decreased Se mass distribution (3.54%→2.63%) in flue gas at air preheater inlet (320 -362 °C) confirmed the effectiveness of increased Ca content on gaseous Se emission reduction. More gaseous Se further condensed and was chemically adsorbed by fly ash when passed through an electrostatic precipitator, resulting in a significant increase in the Se content of fly ash. Additionally, the corresponding Se leaching ratio decreased from 4.88 - 35.74% to 1.87 - 26.31%, indicating enhanced stability of Se enriched in fly ash. This research confirmed the feasibility and environmental safety of sequestration of gaseous Se from flue gas to fly ash by increasing the Ca content in coals.

4.
Chemosphere ; 356: 142024, 2024 May.
Article in English | MEDLINE | ID: mdl-38614396

ABSTRACT

Indoor formaldehyde (HCHO) pollution poses a major risk to human health. Low-temperature catalytic oxidation is an effective method for HCHO removal. The high activity and selectivity of single atomic catalysts provide a possibility for the development of efficient non-precious metal catalysts. In this study, the most stable single-atom catalyst Ti-Ti4C3O2 was screened by density functional theory among many single atomic catalysts with two-dimensional (2D) monolayer Ti4C3O2 as the support. The computational results show that Ti-Ti4C3O2 is highly selective to HCHO and O2 in complex environments. The HCHO oxidation reaction pathways are proposed based on the Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanisms. According to the reaction energy and energy span models, the E-R mechanism has a lower maximum energy barrier and higher catalytic efficiency than the L-H mechanism. In addition, the stability of the Ti-Ti4C3O2 structure and active center was verified by diffusion energy barrier and ab initio molecular dynamics simulations. The above results indicate that Ti-Ti4C3O2 is a promising non-precious metal catalyst. The present study provides detailed theoretical insights into the catalytic oxidation of HCHO by Ti-Ti4C3O2, as well as an idea for the development of efficient non-precious metal catalysts based on 2D materials.


Subject(s)
Density Functional Theory , Formaldehyde , Oxidation-Reduction , Titanium , Formaldehyde/chemistry , Catalysis , Titanium/chemistry , Air Pollution, Indoor , Air Pollutants/chemistry , Molecular Dynamics Simulation
5.
J Hazard Mater ; 465: 133213, 2024 Mar 05.
Article in English | MEDLINE | ID: mdl-38134683

ABSTRACT

After coal combustion, the minerals present in fly ash can adsorb arsenic (As) during flue gas cooling and reduce As emissions. However, a quantitative description of this adsorption behavior is lacking. Herein, the As adsorption characteristics of minerals (Al/Ca/Fe/K/Mg/Na/Si) were investigated, and a model was developed to predict As content in fly ash. Lab-scale experiments and density functional theory calculations were performed to obtain mineral As adsorption potential. Then, the model was established using lab-scale experimental data for 11 individual coals. The model was validated using lab-scale data from ten blended coals and demonstrated acceptable performance, with prediction errors of 2.83-11.45 %. The model was applied to a 350 MW coal-fired power plant (CFPP) with five blended coals, and As concentration in the flue gas was predicted from a mass balance perspective. The experimental and predicted As contents in fly ash were 11.92-16.15 and 9.61-12.55 µg/g, respectively, with a prediction error of 17.39-22.29 %, and those in flue gas were 11.52-16.58 and 5.37-34.04 µg/Nm3. Finally, As distribution in the CFPP was explored: 0.74-1.51 % in bottom ash, 74.05-82.70 % in electrostatic precipitator ash, 0.53-1.19 % in wet flue gas desulfurization liquid, and 0.13-0.73 % in flue gas at the stack inlet.

6.
Environ Pollut ; 337: 122556, 2023 Nov 15.
Article in English | MEDLINE | ID: mdl-37741545

ABSTRACT

Smouldering is a low-energy, low-cost, effective treatment technology for sludge with high moisture. However, combustible gas and pollution in the flue gas limit the low-cost operation. This work proposes a novel method to in-situ reduce gas emissions (CO, NO, VOCs) and absorb heavy metals by regulating inert media with low-cost natural zeolite in self-sustained smouldering of sludge, and the effect of natural zeolite blending ratio on the performance is deeply investigated by fixed-bed and smouldering experiments. Fixed-bed experiments show that adding natural zeolite contributes to the sludge reaction owning to the confined catalysis with porous structure, as observed by the more rapid oxygen consumption, lower CO/NO concentrations. Moreover, smouldering experiments demonstrate that the endothermic dehydroxylation and dehydroxylation processes of the pure natural zeolite decreases the smouldering temperature and the propagation velocity, reduces the pyrolysis layer, but adding natural zeolite significantly reduces the concentrations of CO/NO/VOCs in the flue gas. Furthermore, higher heavy element content in the post-reaction natural zeolite is observed, indicating that the inorganic minerals in natural zeolite can effectively absorb the heavy elements. Taking reaction intensity, CO/NO/VOCs reduction and heavy element absorption into account, adding a small amount of natural zeolite (Sand: Natural-zeolite = 2.90:0.10) may be reasonable with obtaining good performance. Finally, the organic components in condensable liquids of the smouldering flue gas are deeply analyzed, and the main components is 36.7% for amides and 23.41% for nitrogen-containing heterocyclic compounds. This work can provide a possible pathway and useful information for the low-cost application of the sludge smouldring technology.


Subject(s)
Metals, Heavy , Volatile Organic Compounds , Zeolites , Sewage/chemistry , Temperature , Metals, Heavy/chemistry
7.
Waste Manag ; 158: 13-22, 2023 Mar 01.
Article in English | MEDLINE | ID: mdl-36623405

ABSTRACT

Although smouldering of solid waste with high moisture has shown strong promise in laboratory studies, there are fewer reports about the larger-scale device and continuous operation. This work studies a self-sustaining smouldering treatment of food-processing sludge (FPS) with extremely high moisture (over 85 %) in laboratory- and pilot-scale devices. Results from laboratory-scale experiments show that adding auxiliary fuel is necessary to maintain FPS self-sustaining smouldering, Sand: FPS: Sawdust = 25:5:1 is a reasonable mixing ratio. Then, the self-sustaining smouldering is volumetrically scaled up to the pilot-scale. The smouldering asynchrony in the feedstock is observed due to the non-uniform air flux. Compared to the laboratory-scale, the pilot-scale device presents a similar temperature level but a higher smouldering velocity. Furthermore, a continuous process in the pilot-scale device is successfully performed, and the flue gas concentrations are measured: 15.0 âˆ¼ 16.5 % for O2, 4000 âˆ¼ 5500 ppm for CO, 155 âˆ¼ 195 ppm for NOx, 210 âˆ¼ 250 ppm for VOCs, 55 âˆ¼ 70 ppm for SO2, 0.0138 âˆ¼ 0.0317 ngTEQ/m3 (at 11 % O2) for dioxin. These studied results can provide useful information for continuous, low-energy solid waste treatment.


Subject(s)
Polychlorinated Dibenzodioxins , Sewage , Solid Waste , Temperature , Conservation of Natural Resources
8.
J Hazard Mater ; 407: 124742, 2021 Apr 05.
Article in English | MEDLINE | ID: mdl-33333389

ABSTRACT

Mineral oxides are effective in-furnace sorbents used to control lead (Pb) emissions in flue gas at high temperatures. In this paper, the PbO/PbCl2 adsorption characteristics of sorbents were investigated via experimental and density functional theory (DFT) methods. The results show that Si/Al-based compounds can chemically adsorb Pb, and the adsorption is related to the Si-O and Al-O bonds in the sorbents. Exposed Si and O atoms on SiO2 surfaces and exposed Al and O atoms on Al2O3 surfaces are the active sites for Pb adsorption, and PbO is easier to remove than PbCl2. Pb adsorption is promoted in a mixture of SiO2 and Al2O3. Doping Si atoms into Al2O3(100) promotes PbO adsorption, and doped three-coordinate Si atoms have a more obvious promotion effect than doped two-coordinate Si atoms. Doping Al atoms into SiO2(001) has no obvious effect on PbO adsorption. The effect of temperature on Pb adsorption was studied by thermodynamic analysis. The Gibbs free energy difference for PbO adsorption on SiO2(001) increases from -373.04-32.42 kJ/mol as the temperature increases from 300 to 1800 K. High-temperature calcination changes the bond length and bond angle of the system, affecting the stabilities of atomic configurations and decreasing the Pb adsorption capacity.

9.
J Hazard Mater ; 403: 123617, 2021 Feb 05.
Article in English | MEDLINE | ID: mdl-32763637

ABSTRACT

Coal combustion is one of the major pathways by which arsenic enters the ecological environment. An effective method to control arsenic emissions in-furnace is to transform the arsenic from a vapour to fly ash particles using mineral sorbents. However, flue gas components have a significant effect on gas-phase arsenic adsorption, which limits the industrial application of mineral sorbents. In this paper, the effect mechanism of flue gas components (NaCl/HCl/SO2/CO2) on gas-phase arsenic adsorption over different mineral oxide sorbents was investigated. The results demonstrate that the order of arsenic adsorption is CaO > MgO/Fe2O3> NaCl > Al2O3 > SiO2. NaCl promotes the arsenic adsorption of CaO above 800 °C, and the arsenic removal efficiency of CaO with 5 % NaCl is 52.51 % at 900 °C. NaCl inhibits the arsenic adsorption of MgO and Fe2O3, and promotes arsenic adsorption by Al2O3 and SiO2. Acid gases inhibit arsenic adsorption by the sorbents and the order of the inhibition intensity of acid gases at 700 °C is HCl > SO2 > CO2. The active sites (CaO, FeO, or AlO bonds) in the sorbents are the main reaction sites for arsenic adsorption, and captured arsenic is in the form of AsO21- and AsO43-.

10.
Bull World Health Organ ; 95(9): 657-662, 2017 Sep 01.
Article in English | MEDLINE | ID: mdl-28867847

ABSTRACT

PROBLEM: Early detection of syphilis-infected people followed by effective treatment is essential for syphilis prevention and control. APPROACH: Starting in 2010 the local health authority in Yunnan province, China, developed a network of 670 service sites for syphilis testing, diagnosis and treatment or for testing-only with referral for further diagnosis and treatment. Point-of-care tests for syphilis and syphilis interventions were integrated into the existing human immunodeficiency virus (HIV) prevention and control programme. To improve the syphilis services, a pay-for-performance scheme was introduced in which providers were paid for testing and treating patients. LOCAL SETTING: Yunnan province is the region hardest hit by HIV infection and disproportionately burdened with syphilis cases in China. RELEVANT CHANGES: The proportion of attendees at voluntary counselling and testing clinics who were tested for syphilis increased from 46.2% (32 877/71 162) in 2010 to 98.2% (68 012/69 259) in 2015. Syphilis-infected cases treated with the recommended therapy increased from 26.6% (264/993) in 2010 to 82.5% (453/549) in 2015 at designated testing, diagnosis and treatment sites. LESSONS LEARNT: The strategy greatly increased the uptake of syphilis testing and treatment among people at risk. Introduction of point-of-care tests for syphilis increased coverage of the testing services. Introduction of a pay-for-performance scheme seemed to motivate health-care providers to undertake syphilis intervention services.


Subject(s)
Health Promotion/methods , Reimbursement, Incentive , Syphilis Serodiagnosis/statistics & numerical data , Syphilis/diagnosis , Syphilis/economics , Anti-Bacterial Agents/therapeutic use , China , Female , HIV Infections , Health Services Accessibility , Humans , Male , Point-of-Care Systems , Pregnancy , Sentinel Surveillance , Syphilis/drug therapy , Syphilis/epidemiology
12.
Environ Sci Technol ; 49(21): 13040-9, 2015 Nov 03.
Article in English | MEDLINE | ID: mdl-26452156

ABSTRACT

A novel combustion system was applied to a 600 MWe Foster Wheeler (FW) down-fired pulverized-coal utility boiler to solve high NOx emissions, without causing an obvious increase in the carbon content of fly ash. The unit included moving fuel-lean nozzles from the arches to the front/rear walls and rearranging staged air as well as introducing separated overfire air (SOFA). Numerical simulations were carried out under the original and novel combustion systems to evaluate the performance of combustion and NOx emissions in the furnace. The simulated results were found to be in good agreement with the in situ measurements. The novel combustion system enlarged the recirculation zones below the arches, thereby strengthening the combustion stability considerably. The coal/air downward penetration depth was markedly extended, and the pulverized-coal travel path in the lower furnace significantly increased, which contributed to the burnout degree. The introduction of SOFA resulted in a low-oxygen and strong-reducing atmosphere in the lower furnace region to reduce NOx emissions evidently. The industrial measurements showed that NOx emissions at full load decreased significantly by 50%, from 1501 mg/m3 (O2 at 6%) to 751 mg/m3 (O2 at 6%). The carbon content in the fly ash increased only slightly, from 4.13 to 4.30%.


Subject(s)
Air Pollutants/analysis , Coal , Environmental Restoration and Remediation/methods , Nitrates/analysis , Nitrites/analysis , Power Plants/instrumentation , Computer Simulation , Numerical Analysis, Computer-Assisted , Oxygen/analysis , Reproducibility of Results , Temperature
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