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1.
Environ Res ; 247: 118359, 2024 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-38320717

RESUMEN

In this work, the Mn, Co, Ce co-doped corn cob biochar (MCCBC) as catalytic particle electrodes in a three-dimensional heterogeneous electro-Fenton-like (3D-HEFL) system for the efficient degradation of coking wastewater was investigated. Various characterization methods such as SEM, EDS, XRD, XPS and electrochemical analysis were employed for the prepared materials. The results showed that the MCCBC particle electrodes had excellent electrochemical degradation performances of COD in coking wastewater, and the COD removal and degradation rates of the 3D/HEFL system were 85.35% and 0.0563 min-1 respectively. RSM optimized conditions revealed higher COD removal rate at 89.23% after 31.6 min of electrolysis. The efficient degradability and wide adaptability of the 3D/HEFL system were due to its beneficial coupling mechanism, including the synergistic effect between the system factors (3D and HEFL) as well as the synergistic interactions between the ROS (dominated by •OH and supplemented by O2•-) in the system. Moreover, the COD removal rate of MCCBC could still remain at 81.41% after 5 cycles with a lower ion leaching and a specific energy consumption of 11.28 kWh kg-1 COD. The superior performance of MCCBC, as catalytic particle electrodes showed a great potential for engineering applications for the advanced treatment of coking wastewater.


Asunto(s)
Carbón Orgánico , Cocaína , Coque , Contaminantes Químicos del Agua , Aguas Residuales , Eliminación de Residuos Líquidos/métodos , Coque/análisis , Oxidación-Reducción , Electrodos , Cocaína/análisis , Contaminantes Químicos del Agua/análisis
2.
J Environ Manage ; 359: 120986, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38696849

RESUMEN

The efficient, safe and eco-friendly disposal of the chromium-containing sludge (CCS) has attracted an increasing concern. In this study, Co-processing of CCS was developed via employing sintering and ironmaking combined technology for its harmless disposal and resource utilization. Crystalline phase and valence state transformation of chromium (Cr), technical feasibility assessment, leaching risk, characteristics of sintered products, and pollutant release during CCS co-processing were investigated through a series of laboratory-scale sintering pot experiments and large scale industrial trials. The results showed that the content of Cr(VI) in sintered products first increased then decreased with increasing temperature ranges of 300 °C-800 °C, and reached a maximum of 2189.64 mg/kg at 500 °C. 99.99% of Cr(VI) can be reduced to Cr(III) at above 1000 °C, which was attributed to the transformation of the Cr(VI)-containing crystalline phases (such as, MgCrO4 and CaCrO4) to the (Mg, Fe2+)(Cr, Al, Fe3+)2O4. The industrial trial results showed that adding 0.5 wt‰ CCS to sintering feed did not have adverse effects on the properties of the sintered ore and the plant's operating stability. The tumbler index of sinter was above 78% and the leaching concentrations of TCr (0.069 mg/L) was significantly lower than the Chinese National Standard of 1.0 mg/L (GB5085.3-2007). The TCr contents of sintering dust and blast furnace gas (BFG) scrubbing water were less than 0.19 wt‰ and 0.11 mg/L, respectively, which was far below the regulatory limit (1.5 mg/L, GB13456-2012). The mass balance evaluation results indicated that at least 89.9% of the Cr in the CCS migrated into the molten iron in the blast furnace (BF), which became a useful supplement to the molten iron. This study provided a new perspective strategy for the safe disposal and resource utilization of CCS in iron and steel industry.


Asunto(s)
Cromo , Aguas del Alcantarillado , Cromo/química , Aguas del Alcantarillado/química , Hierro/química
3.
Molecules ; 29(1)2024 Jan 04.
Artículo en Inglés | MEDLINE | ID: mdl-38202858

RESUMEN

A novel Mn/TiO2 catalyst, prepared through modification with the rare-earth metal Dy, has been employed for low-temperature selective catalytic reduction (SCR) denitrification. Anatase TiO2, with its large specific surface area, serves as the carrier. The active component MnOx on the TiO2 carrier is modified using Dy. DyxMn/TiO2, prepared via the impregnation method, exhibited remarkable catalytic performance in the SCR of NO with NH3 as the reducing agent at low temperatures. Experiments and characterization revealed that the introduction of a suitable amount of the rare-earth metal Dy can effectively enhance the catalyst's specific surface area and the gas-solid contact area in catalytic reactions. It also significantly increases the concentration of Mn4+, chemisorbed oxygen, and weak acid sites on the catalyst surface. This leads to a notable improvement in the reduction performance of the DyMn/TiO2 catalyst, ultimately contributing to the improvement of the NH3-SCR denitrification performance at low temperatures. At 100 °C and a space velocity of 24,000 h-1, the Dy0.1Mn/TiO2 catalyst can achieve a 98% conversion rate of NOx. Furthermore, its active temperature point decreases by 60 °C after the modification, highlighting exceptional catalytic efficacy at low temperatures. By doubling the space velocity, the NOx conversion rate of the catalyst can still reach 96% at 130 °C, indicating significant operational flexibility. The selectivity of N2 remained stable at over 95% before reaching 240 °C.

4.
Molecules ; 29(15)2024 Jul 24.
Artículo en Inglés | MEDLINE | ID: mdl-39124872

RESUMEN

Mn/TiO2 catalysts with varying solid contents were innovatively prepared by the sol-gel method and were used for selective catalytic reduction of NO at low temperatures using NH3 (NH3-SCR) as the reducing agent. Surprisingly, it was found that as the solid content of the sol increased, the catalytic activity of the developed Mn/TiO2 catalyst gradually increased, showing excellent catalytic performance. Notably, the Mn/TiO2 (50%) catalyst demonstrates outstanding denitration performance, achieving a 96% NO conversion rate at 100 °C under a volume hourly space velocity (VHSV) of 24,000 h-1, while maintaining high N2 selectivity and stability. It was discovered that as the solid content increased, the catalyst's specific surface area (SSA), surface Mn4+ concentration, chemisorbed oxygen, chemisorption of NH3, and catalytic reducibility all improved, thereby enhancing the catalytic efficiency of NH3-SCR in degrading NO. Moreover, NH3 at the Lewis acidic sites and NH4+ at the Bronsted acidic sites of the catalyst were capable of reacting with NO. Conversely, NO and NO2 adsorbed on the catalyst, along with bidentate and monodentate nitrates, were unable to react with NH3 at low temperatures. Consequently, the developed catalyst's low-temperature catalytic reaction mechanism aligns with the E-R mechanism.

5.
Molecules ; 28(6)2023 Mar 09.
Artículo en Inglés | MEDLINE | ID: mdl-36985479

RESUMEN

In this study, high-performance modified biochar/alginate composite bead (MCB/ALG) adsorbents were prepared from recycled agricultural waste corncobs by a high-temperature pyrolysis and KOH/FeCl3 activation process. The prepared MCB/ALG beads were tested for the adsorption of methylene blue (MB) dye from wastewater. A variety of analytical methods, such as SEM, BET, FTIR and XRD, were used to investigate the structure and properties of the as-prepared adsorbents. The effects of solution pH, time, initial MB concentration and adsorption temperature on the adsorption performance of MCB/ALG beads were discussed in detail. The results showed that the adsorption equilibrium of MB dye was consistent with the Langmuir isothermal model and the pseudo-second-order kinetic model. The maximum adsorption capacity of MCB/ALG-1 could reach 1373.49 mg/g at 303 K. The thermodynamic studies implied endothermic and spontaneous properties of the adsorption system. This high adsorption performance of MCB/ALG was mainly attributed to pore filling, hydrogen bonding and electrostatic interactions. The regeneration experiments showed that the removal rate of MB could still reach 85% even after five cycles of experiments, indicating that MCB/ALG had good reusability and stability. These results suggested that a win-win strategy of applying agricultural waste to water remediation was feasible.

6.
Molecules ; 28(8)2023 Apr 13.
Artículo en Inglés | MEDLINE | ID: mdl-37110678

RESUMEN

A novel pyridine-modified chitosan (PYCS) adsorbent was prepared in a multistep procedure including the successive grafting of 2-(chloromethyl) pyridine hydrochloride and crosslinking with glutaraldehyde. Then, the as-prepared materials were used as adsorbents for the removal of metal ions from acidic wastewater. Batch adsorption experiments were carried out to study the impact of various factors such as solution pH value, contact time, temperature, and Fe (III) concentration. The results showed that the absorbent exhibited a high capacity of Fe (III) and the maximum adsorption capacity was up to 66.20 mg/g under optimal experimental conditions (the adsorption time = 12 h, pH = 2.5, and T = 303 K). Adsorption kinetics and isotherm data were accurately described by the pseudo-second-order kinetic model and Sips model, respectively. Thermodynamic studies confirmed that the adsorption was a spontaneous endothermic process. Moreover, the adsorption mechanism was investigated using Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results revealed the pyridine group forms a stable chelate with iron (III) ions. Therefore, this acid-resistant adsorbent exhibited excellent adsorption performance for heavy metal ions from acidic wastewater compared to the conventional adsorbents, helping realize direct decontamination and secondary utilization.

7.
Carbohydr Polym ; 332: 121935, 2024 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-38431402

RESUMEN

A novel cellulose composite (denoted as PEI@MMA-1) with porous interconnected structure was prepared by adsorbing methyl cellulose (MC) onto microcrystalline cellulose (MCC) and cross-linking polyethyleneimine (PEI) with MCC by the action of epichlorohydrin, which had the excellent adsorption property, wettability and elasticity. The performances of PEI@MMA-1 composite for removing tetracycline (TC), Cu2+ and coexistent pollutant (TC and Cu2+ mixture) were systematically explored. For single TC or Cu2+ contaminant, the maximum adsorption capacities were 75.53 and 562.23 mg/g at 30 °C, respectively, while in the dual contaminant system, they would form complexes and Cu2+ could play a "bridge" role to remarkably promote the adsorption of TC with the maximum adsorption capacities of 281.66 and 253.58 mg/g for TC and Cu2+. In addition, the adsorption kinetics, isotherms and adsorption mechanisms of single-pollutant and dual-pollutant systems have been thoroughly investigated. Theoretical calculations indicated that the amide group of TC molecule with the assistance of Cu2+ interacted with the hydroxyl group of PEI@MMA-1 composite to enhance the TC adsorption capacity. Cycle regeneration and fixed bed column experiments revealed that the PEI@MMA-1 possessed the excellent stability and utility. Current PEI@MMA-1 cellulose composite exhibited a promising application for remediation of heavy metals and antibiotics coexistence wastewater.


Asunto(s)
Celulosa/análogos & derivados , Cobre , Polietileneimina/análogos & derivados , Contaminantes Químicos del Agua , Cobre/química , Adsorción , Contaminantes Químicos del Agua/química , Tetraciclina/química , Antibacterianos , Iones , Cinética
8.
Int J Biol Macromol ; 269(Pt 1): 132005, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38777686

RESUMEN

To enhance the mechanics performance, sensitivity and response range of multi-responsive photonic films, herein, a facile method for fabricating multi-responsive films is demonstrated using the evaporative self-assembly of a mixture of grape skin red (GSR), cellulose nanocrystal (CNC), polyvinyl alcohol (PVA) and deep eutectic solvent (DES). The prepared materials exhibited excellent thermal stability, strain properties, solvent resistance, ultraviolet (UV) resistance and antioxidant activity. Compared to a pure PVA film, the presence of GSR strengthened the antioxidant property of the film by 240.1 % and provided excellent UV barrier capability. The additional cross-linking of DES and CNC promoted more efficient phase fusion, yielding a film strain of 41.5 %. The addition of hydrophilic compound GSR, wetting and swelling due to the DES and the surface inhomogeneity of the films rendered the multi-responsive films high sensitivity, wide response range and multi-cyclic stability in environments with varying pH and humidity. A sample application showed that a PVA/CNC/DES film has the potential to differentiate between fresh, sub-fresh and fully spoiled shrimps. The above results help in designing intelligent thin film materials that integrate antioxidant properties, which help in monitoring the changes in food freshness and food packaging.


Asunto(s)
Antioxidantes , Celulosa , Nanopartículas , Alcohol Polivinílico , Alcohol Polivinílico/química , Celulosa/química , Nanopartículas/química , Antioxidantes/química , Disolventes Eutécticos Profundos/química , Embalaje de Alimentos/métodos , Vitis/química , Análisis de los Alimentos/métodos , Concentración de Iones de Hidrógeno
9.
Int J Biol Macromol ; 264(Pt 1): 130410, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38417751

RESUMEN

In this study, magnetic DTPA-modified chitosan composite microspheres (MDCM) were prepared by reverse emulsion-double crosslinking method (carbodiimide followed by glutaraldehyde) for removal of Pb(II) from aqueous solution. The obtained magnetic adsorbents were characterized by FTIR, SEM, XRD, VSM, BET, and 13C NMR. The effects of the pH, contact time, initial concentration, and competitive metal cations (Na(I), Ca(II), or Mg(II)) on Pb(II) adsorption were investigated. The results revealed that MDCM exhibited high removal performance over a wide pH range and in the presence of competitive metal cations. The maximum adsorption capacity of MDCM for Pb(II) is 214.63 mg g-1 at pH 3, which is higher than most recently reported magnetic adsorbents. Adsorption kinetics and isotherms can be described by the pseudo-second-order model and Langmuir model, respectively. In addition, MDCM is easy to regenerate and can be reused five cycles with high adsorption capacity. Finally, the adsorption mechanism was further revealed by FTIR and XPS analysis. Overall, MDCM has practical application potential in removing Pb(II) from contaminated wastewater due to its high adsorption efficiency, good reusability, and convenient magnetic separation.


Asunto(s)
Quitosano , Contaminantes Químicos del Agua , Adsorción , Quitosano/química , Plomo , Microesferas , Contaminantes Químicos del Agua/química , Concentración de Iones de Hidrógeno , Agua/química , Cinética , Fenómenos Magnéticos , Cationes , Ácido Pentético
10.
RSC Adv ; 14(12): 8556-8566, 2024 Mar 06.
Artículo en Inglés | MEDLINE | ID: mdl-38482063

RESUMEN

Polyimide aerogels (PIAs) not only possess excellent thermodynamic properties but also have a high porosity structure, making them an exceptional protective and thermal insulation material, and further broadening their application scope in aerospace and other cutting-edge fields. In this work, a series of anisotropic polyimide aerogels (3,3',4,4'-biphenyltetracarboxylic dianhydride (S-BPDA), p-phenylenediamine (PDA), 4,4'-diaminodiphenyl ether (ODA)) with excellent properties were prepared. These PIAs were obtained by unidirectional freeze-drying and thermal amination of two different precursor solutions mixed in proportion. These PIAs possess an irregularly oval tubular structure, exhibiting pronounced anisotropy. (PIA-2 exhibits outstanding flexible resilience in the radial direction. It can still regain its original form after half an hour of compression by a universal testing machine, yet it cannot do so in the axial direction. The thermal diffusivity of PIA-5 in the radial direction at room temperature is as low as 0.067 mm2 s-1, and even at 200 °C, the thermal diffusivity is as low as 0.057 mm2 s-1. Meanwhile, the thermal diffusivity in the axial direction at room temperature is 0.11 mm2 s-1, surpassing the value of 0.106 mm2 s-1 of aerogels prepared from monomeric raw materials and dried under supercritical conditions). PIAs exhibit outstanding thermal stability (the axial strength and modulus retention of PIA-8 at 200 °C are as high as 52.63% and 44.82%), and its weight loss temperature of 5% is as high as 603 °C and it has a glass softening temperature of 387 °C. PIAs also demonstrate exceptional flame retardancy in imitation flame retardant experiments and exhibit outstanding thermal insulation performance when heated on a 150 °C heating plate for 10 minutes (the radial surface temperature of PIA-5 was only 49.9 °C). These anisotropic PIAs materials exhibit outstanding flexible resilience, and thermal protection performance, holding significant importance for their widespread adoption as thermal insulation materials in aerospace, high-precision electronic components, and other domains.

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