RESUMEN
Coal gasification fine slag (CGFS), as a difficult-to-dispose solid waste in the coal chemical industry, consists of minerals and residual carbon. Due to the aggregate structure of minerals blocking pores and encapsulating active substances, the high-value utilization of CGFS still remains a challenge. Based on the intrinsic characteristics of CGFS, this study synthesized Fe-N doped porous carbon/silicate composites (Fe-NC) by alkali activation and pyrolysis for electrocatalytic degradation of phenolic wastewater. Meanwhile, minerals were utilized to regulate the surface chemical and pore structure, turning their disadvantages into advantages, which caused a sharp increase in m-cresol mineralization. The positive effect of minerals on composite properties was investigated by characterization techniques, electrochemical analyses and density functional theory (DFT) calculations. It was found that the mesoporous structure of the mineral-regulated composites was further developed, with more carbon defects and reactive substances on its surface. Most importantly, silicate mediated iron conversion through strong interaction with H2O2, high work function gradient with electroactive iron, and excellent superoxide radical (â¢O2-) production capacity. It effectively improved the reversibility and kinetics of the entire electrocatalytic reaction. Within the Fe-NC311 electrocatalytic system, the m-cresol removal rate reached 99.55 ± 1.24%, surpassing most reported Fe-N-doped electrocatalysts. In addition, the adsorption and electrooxidation experiment confirmed that the synergistic effect of Fe-N doped porous carbon and silicate simultaneously promoted the capture of pollutants and the transformation of electroactive molecules, and hence effectively shortened the diffusion path of short-lived radicals, which was further supported by molecular dynamics simulation. Therefore, this research provides new insights into the problem of mineral limitations and opens an innovative approach for CGFS recycling and environmental remediation.
Asunto(s)
Carbono , Hierro , Fenoles , Silicatos , Aguas Residuales , Contaminantes Químicos del Agua , Silicatos/química , Aguas Residuales/química , Carbono/química , Porosidad , Hierro/química , Contaminantes Químicos del Agua/química , Fenoles/química , Catálisis , Carbón Mineral , Minerales/química , Nitrógeno/química , Eliminación de Residuos Líquidos/métodos , Técnicas Electroquímicas/métodos , Residuos Industriales/análisisRESUMEN
Landfill is the major waste disposal method of high-moisture coal gasification fine slag (GFS) which causes the pollution of soil and water and brings the waste of resources. GFS efficient dewatering is an urgent problem to be solved, which is beneficial to realize its resource utilization. In this paper, mechanical pressure and vacuum coupling energy fields are applied to carry out the dewatering processes of GFS. The pressure field provides strong power for water migration, which makes water leave the particle system, while the vacuum field provides traction for water removal from system. The fine slag produced from Coal-to-methanol (named JC) with larger size particles tends to form "bridging" frameworks among particles, which provides water occurrence space and increases the moisture migration resistance. The mechanical dewatering process has an energy advantage interval, when the sample moisture is reduced to a certain degree, the mechanical force field is mainly used for particle friction and breakage but not for moisture migration. Through dewatering process energy optimization, high moisture gasification fine slag can be removed about 15% water within 30s and energy consumption of efficient dewatering is 2.63 kJ/g which is much lower than that of drying. Efficient dewatering is benefit to the GFS recycling which reduces hazardous materials release to environment. The potential effects of high efficiency dewatering process on GFS resource utilization and the possible eco-design framework for products recycled from the waste GFS were proposed. The research results will provide theoretical guidance for the gasification fine slag efficient dewatering and is benefit to the environment.
Asunto(s)
Carbón Mineral , Eliminación de Residuos , Reciclaje , Eliminación de Residuos/métodos , Vacio , AguaRESUMEN
Using bamboo powder biochar as raw material, high-quality meso/microporous controlled hierarchical porous carbon was prepared-through the catalysis of Fe3+ ions loading, in addition to a chemical activation method-and then used to adsorb copper ions in an aqueous solution. The preparation process mainly included two steps: load-alkali leaching and chemical activation. The porosity characteristics (specific surface area and mesopore ratio) were controlled by changing the K2CO3 impregnation ratio, activation temperature, and Fe3+ ions loading during the activation process. Additionally, three FBPC samples with different pore structures and characteristics were studied for copper adsorption. The results indicate that the adsorption performance of the bamboo powder biochar FBPC material was greatly affected by the meso/micropore ratio. FBPC 2.5-900-2%, impregnated at a K2CO3: biochar ratio of 2.5 and a Fe3+: biochar mass ratio of 2%, and activated at 900 °C for 2 h in N2 atmosphere, has a very high specific surface area of 1996 m2 g-1 with a 58.1% mesoporous ratio. Moreover, it exhibits an excellent adsorption capacity of 256 mg g-1 and rapid adsorption kinetics for copper ions. The experimental results show that it is feasible to control the hierarchical pore structure of bamboo biochar-derived carbons as a high-performance adsorbent to remove copper ions from water.
Asunto(s)
Carbono/química , Cloruros/química , Cobre/química , Compuestos Férricos/química , Sasa/química , Absorción Fisicoquímica , Carbón Orgánico/química , Polvos/química , Espectrofotometría Atómica/instrumentación , Espectrofotometría Atómica/métodos , Purificación del Agua/métodosRESUMEN
A large amount of coal gasification slag is produced every year in China. However, most of the current disposal is into landfills, which causes serious harm to the environment. In this research, coal gasification fine slag residual carbon porous material (GFSA) was prepared using gasification fine slag foam flotation obtained carbon residue (GFSF) as raw material and an adsorbent to carry out an adsorption test on waste liquid containing methylene blue (MB). The effects of activation parameters (GFSF/KOH ratio mass ratio, activation temperature, and activation time) on the cation exchange capacity (CEC) of GFSA were investigated. The total specific surface area and pore volume of GSFA with the highest CEC were 574.02 m2/g and 0.467 cm3/g, respectively. The degree of pore formation had an important effect on CEC. The maximum adsorption capacity of GFSA on MB was 19.18 mg/g in the MB adsorption test. The effects of pH, adsorption time, amount of adsorbent, and initial MB concentration on adsorption efficiency were studied. Langmuir isotherm and quasi second-order kinetic model have a good fitting effect on the adsorption isotherm and kinetic model of MB.
RESUMEN
The entrained-flow gasifier has a better adaptability to various coals. The composition of coal ash is an important factor affecting the high-temperature flow characteristics of molten slag. Based on the SiO2-Al2O3-CaO/Na2O ternary phase diagram, the high-temperature molten flow characteristics of slag located in the main phase regions of feldspar, melilite, diopside, and mullite were investigated by experiments and thermodynamic software calculations. The results indicate that the melting process of ash in the three phase zones is influenced by different factors. It was discovered by infrared spectroscopy analysis that the slag was dominated by Si2O52- ion clusters in the feldspar region. The slag in the diopside region had a slightly higher proportion of simple silicate ion clusters than the slag in the feldspar region, resulting in better fluidity. This is significant for revealing the mechanism of coal ash melting and flowing and guiding industrial coal blending.
RESUMEN
In recent years, the coal gasification industry has rapidly developed, becoming one of the most promising technologies in the advanced and clean coal chemical industry. As a result, the annual emission of coal gasification fine slag (CGFS) has continuously increased. The present situation of CGFS is regarded as a notorious waste in gasification plants and is rudely landfilled or deposited in slag yards, which leads to a large waste of land resources, the release of dangerous elements, and numerous pollution problems. Although CGFS is classified as industrial solid waste, its unique physical and chemical properties make it a valuable resource that cannot be overlooked. This paper focuses on the resource utilization technology and environmental impact of CGFS. The resource utilization of different components of CGFS has realized the evolution from waste to valuable substances. Moreover, during the disposal and utilization of CGFS, its environmental effects cannot be ignored. The main problems and future research directions are also further proposed. Efforts should be focused on the challenges of the technology, cost, and environmental protection in the application process to achieve industrial application, and ultimately committed to sustainable and green development goals, and promote the sustainable management and conservation of resources.
Asunto(s)
Carbón Mineral , Metales Pesados , Carbón Mineral/análisis , Residuos Industriales , Conservación de los Recursos Naturales , ClimaRESUMEN
The abundant coal powder generated as a waste by-product during the lignite upgrading process is harmful to the environment. Lignite briquetting offers a practical solution for lignite usage. Altering the process parameters of briquetting can significantly improve briquette quality. In this paper, the characteristics of lignite briquettes, including drop strength and compressive strength were investigated. A combination of quadratic orthogonal rotation combination designs and regression equations established the best process parameters to be 40% weight of #2 upgraded coal, 20% weight of briquetting moisture, 25 MPa of briquetting pressure, and 12 h of drying time. The low error variance of the drop strength and compressive strength, at 0.01% and 1.83% respectively, verified the feasibility of the model. The analysis by scanning electron microscope (SEM) showed that the surface morphology of briquette was denser than that of raw coal. Finally, the combustion test of briquettes revealed that the particulate matter emission (PM2.5) of briquette was 16.7% lower than that of raw coal. In summary, these data provide a theoretical reference for realizing the reasonable utilization potential of waste products derived from industrial processes.
Asunto(s)
Contaminantes Atmosféricos , Carbón Mineral , Contaminantes Atmosféricos/análisis , Material Particulado/análisis , ResiduosRESUMEN
From the perspective of environmental protection and resource utilization, the feasibility of treating m-cresol wastewater with coal gasification fine slag (GFS) as particle electrodes in an electrocatalytic system was evaluated to achieve the purpose of treating waste with waste. Characterization by scanning electron microscope (SEM), Brunauer-Emmett-Teller (BET), Raman, and fourier transform infrared spectroscopy (FTIR) confirmed that the GFS featured a diverse inorganic framework, large specific surface area (as large as above 155 m2 g-1), hierarchical porous structure, and plenty of catalytic sites. The Venn diagram method was used to systematically propose the following distribution modes of residual carbon (RC) and ash in GFS: discrete distribution, embedded distribution, crosslinked distribution, and association and bonding. Only 8 g L-1 of GFS particle electrodes prevented the formation of a yellow sticky passivation film on the anode. Compared to the two-dimensional electrocatalytic system (47.89%), the wastewater treatment efficiency was increased by 108.81%. Zero-order kinetic results showed that the reaction rate constant was the highest (2.1106 mg L-1·min-1) when the secondary flotation RC was adopted as particle electrodes. It was indicated that GFS in discrete mode played either no role or at most a minor role. Last but not least, the synergy of RC and ash was revealed from a molecular perspective. The RC exhibited hierarchical microporous/mesoporous/macroporous structure, which facilitated the entry of H2O2 into the catalytic sites of ash. Abundant catalytic sites in ash accelerated adsorption and oxidation processes on RC surfaces.
Asunto(s)
Carbono , Carbón Mineral , Ceniza del Carbón/química , Electrodos , Estudios de Factibilidad , Peróxido de HidrógenoRESUMEN
The coal gasification fine slag (CGFS) from the entrained-flow coal gasification unit faces the challenge of safe disposal and clean utilization in the Ningdong region, China. This study aims to provide complete and thorough understanding of the distribution features, chemical speciation, environmental impact, and leaching behavior of typical heavy metals (i.e., V, Cr, Mn, Ni, Cu, Zn, Ba, and Pb) in the CGFS with different size fractions. The results show that the distribution of selected heavy metals in the CGFS has evident particle size dependence. Except for Zn, the other heavy metals in different size fractions mainly exist in chemical speciation of residual form with the ratio of 50.11-86.69 wt%. Moreover, it is found that the heavy metals in the different-sized CGFS show different RAC (risk assessment code) environmental risk levels and TCLP (Toxicity Characteristic Leaching Procedure) leaching concentrations. Especially, Zn in SGFS-C and SGFS-D posed a high-risk level to the environment, while the heavy metal elements of Cr, Mn, Ni, Zn, and Ba in other size fractions are classified as a medium environmental risk. In addition, the TCLP test results indicate that the leaching concentration of Cr, Mn, Ni, Zn, Ba, and Pb exceeds the groundwater-related regulatory limit in China. The pH-dependent leaching experiments suggest that Pb shows the amphoteric behavior, while the leaching mode of other heavy metals seems to be the cationic pattern. Furthermore, the leachability of the selected heavy metals in small-size fractions of the CGFS should be given more consideration at both acid and alkaline pH ranges. The leaching kinetic results demonstrate that the most effective mechanism to describe the leaching process of Cr, Ni, Zn, and Pb in different CGFS size fractions is the diffusion-controlled theory, which is supported by the different morphological traits of spherical mineral particles and carbon particles in the CGFS.
Asunto(s)
Medicamentos Herbarios Chinos , Metales Pesados , China , Carbón Mineral , Plomo , Metales Pesados/análisisRESUMEN
In this study, a novel three-dimensional photoelectric system was designed and constructed for the degradation of methylene blue (MB) via photocatalysis, electrocatalysis, and photoelectric catalysis. To this end, a Ti/RuO2-IrO2-SnO2-CeO2 electrode was prepared via a thermal oxidation coating method and used as a dimensionally-stable anode (DSA). The cathode was made of a titanium sheet with Fe3+-doped TiO2 loaded on coal gasification slag (CGS) (Fe3+-TiO2@CGS) as a photocatalyst. The factors affecting the degradation efficiency, such as the supporting electrolyte, current density, and initial pH were systematically investigated. The results revealed Fe3+-TiO2@CGS three-dimensional photoelectric system exhibiting efficient synergistic performance of photocatalysis and electrocatalysis with a synergistic factor of 1.11. Photo-generated holes (h+) were generated by light irradiation and direct anodic oxidation. Furthermore, hydroxyl radicals (HO·) radicals were induced via other pathways. Such active species showed highly-oxidizing abilities, beneficial to the degradation of methylene blue (MB). The representative Fe3+-TiO2@CGS three-dimensional photoelectric system showed super high degradation efficiency at pH 11 and current density of 18.76 mA cm-2. Using NaCl as a supporting electrolyte, the degradation yield reached 99.98% after 60 min of photoelectrical treatment. Overall, the novel Fe3+-TiO2@CGS three-dimensional photoelectrical system looks very promising for the highly efficient catalytic degradation of organic contaminants.
RESUMEN
An accurate and quantitative description of the pore structure of gasification-coke using fractal geometry could be of great significance to its industrial utilization. In this study, gasification-coke was prepared with low-quality coal blending at different high-temperature residence times to investigate the variation in the pore structure, fractal dimensions, reactivities, and their relationship. The pore structure parameters (e.g., specific surface area, pore volume, and average pore diameter) of gasification-coke were investigated by low-temperature N2 adsorption/desorption and mercury intrusion porosimetry. Fractal dimensions D 1 and D 2 (at relative pressures of 0-0.5 and 0.5-1, respectively) were calculated using the fractal Frenkel-Halsey-Hill model, and the fractal dimension D 3 was obtained using the Menger sponge model. The results show that the pore structure systems of gasification-coke prepared at different high-temperature residence times are continuous and complete, which contributes to the gasification reaction. The variation trend of the macropore structure parameters is more complex than that of micropore and mesopore with the extension of the high-temperature residence time. It is found that D 1 is linearly correlated with the micropore specific surface area, indicating that D 1 is more suitable for reflecting the roughness of the micropore surface; D 2 is linearly correlated with the mesopore volume and can describe the volumetric roughness of the mesopore; and D 3 reflects the irregularities and surface roughness of the macropores. Gasification reactivity is closely related to the D 2 value, and the reactivity of the gasification-coke may be improved if the number of mesopores is increased by controlling the high-temperature residence time or other pyrolysis conditions. The research results will provide theoretical reference for controlling the gasification reaction of gasification-coke and gasifier design.