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In response to the need for improvement in the utilization of ammonium-rich solutions after the electrochemical reduction of nitrate (NO3--RR), this study combined phosphorus-containing wastewater and adopted the electrochemical precipitation method for the preparation of struvite (MAP) to simultaneously recover nitrogen and phosphorus resources. At a current density of 5 mA·cm-2 and an initial solution pH of 7.0, the recovery efficiencies for nitrogen and phosphorus can reach 47.15% and 88.66%, respectively. Under various experimental conditions, the generated struvite (MgNH4PO4·6H2O) exhibits a typical long prismatic structure. In solutions containing nitrate and nitrite, the coexisting ions have no significant effect on the final product, struvite. Finally, the characterization of the precipitate product by X-ray diffraction (XRD) revealed that its main component is struvite, with a high purity reaching 93.24%. Overall, this system can effectively recover ammonium nitrogen from the NO3--RR solution system after nitrate reduction, with certain application prospects for the recovery of ammonium nitrogen and phosphate.
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With the rapid development of industry, the discharge of heavy metal-containing wastewater poses a significant threat to aquatic and terrestrial environments as well as human health. This paper provides a brief introduction to the basic principles of ion-imprinted polymer preparation and focuses on the interaction between template ions and functional monomers. We summarized the current research status on typical heavy metal ions, such as Cu(II), Ni(II), Cd(II), Hg(II), Pb(II), and Cr(VI), as well as metalloid metal ions of the As and Sb classes. Furthermore, it discusses recent advances in multi-ion-imprinted polymers. Finally, the paper addresses the challenges faced by ion-imprinted technology and explores its prospects for application.
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In the context of carbon capture, utilization, and storage, the high-value utilization of carbon storage presents a significant challenge. To address this challenge, this study employed the bipolar membrane electrodialysis integrated with carbon utilization technology to prepare Na2CO3 products using simulated seawater concentrate, achieving simultaneous saline wastewater utilization, carbon storage and high-value production of Na2CO3. The effects of various factors, including concentration of simulated seawater concentrate, current density, CO2 aeration rate, and circulating flow rate of alkali chamber, on the quality of Na2CO3 product, carbon sequestration rate, and energy consumption were investigated. Under the optimal condition, the CO32- concentration in the alkaline chamber reached a maximum of 0.817 mol/L with 98 mol% purity. The resulting carbon fixation rate was 70.50%, with energy consumption for carbon sequestration and product production of 5.7 kWhr/m3 CO2 and 1237.8 kWhr/ton Na2CO3, respectively. This coupling design provides a triple-win outcome promoting waste reduction and efficient utilization of resources.
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Dióxido de Carbono , Carbono , Carbonatos , Agua de Mar , SodioRESUMEN
Electrochemical reduction of nitrate has broad application prospects. However, in traditional electrochemical reduction of nitrate, the low value of oxygen produced by the anodic oxygen evolution reaction and the high overpotential limit its application. Seeking a more valuable and faster anodic reaction to form a cathode-anode integrated system with nitrate reaction can effectively accelerate the reaction rate of the cathode and anode, and improve the utilization of electrical energy. Sulfite, as a pollutant after wet desulfurization, has faster reaction kinetics in its oxidation reaction compared to the oxygen evolution reaction. Therefore, this study proposes an integrated cathodic nitrate reduction and anodic sulfite oxidation system. The effect of operating parameters (cathode potential, initial NO3--N concentration, and initial SO32--S concentration) on the integrated system was studied. Under the optimal operating parameters, the nitrate reduction rate in the integrated system reached 93.26% within 1 h, and the sulfite oxidation rate reached 94.64%. Compared with the nitrate reduction rate (91.26%) and sulfite oxidation rate (53.33%) in the separate system, the integrated system had a significant synergistic effect. This work provides a reference for solving nitrate and sulfite pollution, and promotes the application and development of electrochemical cathode-anode integrated technology.
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Selective electrodialysis is a promising approach to recovering K+ from complex coexisting ionic systems. In this study, the effects of current density, the concentration of K+ and Mg2+, as well as the operating temperature on the separation process of K+ and Mg2+ were explored to investigate the competitive migration of mono- and multivalent ions, offering a guide for the design of selective electrodialysis process, and therefore obtain the desired aqueous solutions containing K+ and Mg2+. The results show that ion concentration played a critical role in determining the selectivity of separation between K+ and Mg2+. High concentrations of K+ and Mg2+ led to a decrease in selectivity but the effect of concentration of K+ on selectivity was more pronounced. Although higher current density increased the flux of ions, their impact on separation selectivity was minimal. Furthermore, higher temperature increased the flux of ions but resulted in a decrease of K+ proportion in the solution. Overall, this study provides good guidance for studying the competitive migration of mono- and multivalent ions and the high-value recycling of potassium resources.
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The microstructure of a mixed KCl and K2SO4 aqueous solution was studied using X-ray scattering (XRS), Raman spectroscopy, and molecular dynamics simulation (MD). Reduced structure functions [F(Q)], reduced pair distribution functions [G(r)], Raman spectrum, and pair distribution functions (PDF) were obtained. The XRS results show that the main peak (r = 2.81 Å) of G(r) shifted to the right of the axis (r = 3.15 Å) with increased KCl and decreased K2SO4. The main peak was at r = 3.15 Å when the KCl concentration was 26.00% and the K2SO4 concentration was 0.00%. It is speculated that this phenomenon was caused by the main interaction changing, from K-OW (r = 2.80 Å) and OW-OW (r = 2.80 Å), to Cl−-OW (r = 3.14 Å) and K+-Cl− (r = 3.15 Å). According to the trend of the hydrogen bond structure in the Raman spectrum, when the concentration of KCl was high and K2SO4 was low, the destruction of the tetrahedral hydrogen bond network in the solution was more serious. This shows that the destruction strength of the anion to the hydrogen bond network structure in solution was Cl− > SO42−. In the MD simulations, the coordination number of OW-OW decreased with increasing KCl concentration, indicating that the tetrahedral hydrogen bond network was severely disrupted, which confirmed the results of the Raman spectroscopy. The hydration radius and coordination number of SO42− in the mixed solution were larger than Cl−, thus revealing the reason why the solubility of KCl in water was greater than that of K2SO4 at room temperature.
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Simulación de Dinámica Molecular , Espectrometría Raman , Espectrometría Raman/métodos , Sulfatos , Agua/química , Rayos XRESUMEN
In the previous study, greenhouse gas CO2 was successfully used as the precipitator to realize its carbonation by calcium ions in seawater with the help of magnesium oxide. In this study, the reaction process was firstly analyzed by a proposed reaction mechanism, and then the dynamic simulation of the gas-liquid-solid system was carried out via kinetic Monte Carlo simulation. Based on the reaction mechanism, the continuous experimental study was realized in a bubble column. The effects of air flow rate, carbon dioxide flow rate and temperature on the effectiveness evaluation indexes of decalcification efficiency, total mass transfer coefficient and carbon sequestration rate were studied. Finally, a bonnet tower with a diameter of 1 m and a height of 8 m was built to carry out the pilot test. In the laboratory experiments, the calcium removal rate reached 94%, the carbon sequestration rate reached 63.6%, and pure micron calcium carbonate products were obtained. The decalcification rate reached 95% in the pilot test, which is consistent with the results of the laboratory experiment.
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Dióxido de Carbono , Secuestro de Carbono , Carbonato de Calcio , Carbonatos , Agua de MarRESUMEN
Sulfite oxidation is critical for the stable operation of desulfurization process and the treatment & recovery of desulfurization by-products. The Fe and Co oxides modified super hydrophobic layer was prepared on tubular ceramic membranes using hydrothermal synthesis and surface modifications to realize the combination of the membrane catalysis and membrane aeration. These two oxides were approximately two-layer distributed on the membrane surface, among which the Fe2O3 located in the bottom layer and the Co3O4 located in the upper layer. The catalytic rate of the bifunctional membrane was about 5.8 times than that of the original ceramic membrane, which was decreased with the increasing of Fe/Co ratio and declined after an initial rise with the increase of urea and cetyltrimethylammonium bromide. The conjoint effect of Fe and Co could improve the catalytic performance and reduce the dissolution loss of catalyzer. The oxidation rate tended to be constant after a 15 % decrease in 7 times experiments.
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Achieving separation of lithium and magnesium with similar radii is crucial for the current lithium extraction technology from salt lakes, which usually possess a high lithium-to-magnesium ratio. Herein, we proposed the facile sequential interfacial polymerization (SIP) approach to construct electronanofiltration membranes (ENFMs) with a bilayer charged structure consisting of a high positively charged surface and a negatively charged sublayer. The trimesoyl chloride (TMC) concentration was adjusted to enhance the -COOH content and negative charge of the polyamide sublayer to promote Li+ migration, and then the quaternized polyethylenimine was introduced to the membrane surface by the SIP process to increase the positive charge density on the surface of the ENFMs, which would block the migration of Mg2+ and enhance the Li+/Mg2+ selectivity of the ENFMs. The optimal quaternary-modified ENFMs achieved outstanding selectivity for Li+/Mg2+ (49.85) and high Li+ flux (4.10 × 10-8 mol cm-2 s-1) at a current density of 10 mA cm-2. Moreover, in simulated brines with low lithium concentration and high Mg2+/Li+ ratio, the optimal ENFMs also displayed elevated Li+/Mg2+ selectivity (>45), highlighting the substantial promise of the membranes for practical applications.
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Aqueous solutions of magnesium chloride (MgCl2(aq)) are often used to test advances in the theory of electrolyte solutions because they are considered an ideal strong 2:1 electrolyte. However, there is evidence that some ion association occurs in these solutions, even at low concentrations. Even a small ion-pairing constant can have a significant impact on the chemical speciation of ions, so it is important to determine whether ion pairing actually occurs. In this study, MgCl2(aq) with concentrations ranging from 1 to 35% was studied using three methods: X-ray scattering (XRS) with the Shanghai Synchrotron Radiation Facility (SSRF) and silver-anode laboratory sources, Raman spectroscopy, and molecular dynamics (MD) simulations with the COMPASS-II and Madrid force fields. XRS results were analyzed in the framework of PDF theory to obtain the reduced structure function F(Q) and the reduced pair distribution function G(r). The F(Q) values from synchrotron radiation and laboratory sources both showed that the tetrahedral hydrogen bonds in bulk water were destroyed with the increased MgCl2 concentration. The results of G(r) indicated that the main peaks centered at 2.05 and 2.80 Å can be ascribed to the interactions of Mg-O and O-O, respectively. The peak at 3.10 Å is attributed to the combined effect of O-O and Cl-O. By comparing the structural information on MgCl2 solution obtained from the two light sources, it was found that both SSRF and silver-anode laboratory sources can reflect the above-mentioned structural information on MgCl2 solution. The radial distribution function (RDF) obtained from MD simulations of MgCl2 solutions assigned the peaks at 2.0, 2.8, and 3.2 Å to the Mg-O, O-O, and Cl-O interatomic pairs, respectively. The decrease in the O-O coordination number confirms that the hydrogen-bonding network of water is disrupted by increasing MgCl2 observed by X-ray scattering. The proportion of Mg-Cl contact ion pairs gradually increases with MgCl2 concentration as does the coordination number. Raman spectroscopy results show that the bond type changes from double donor double acceptor (DDAA) to single donor-single acceptor (DA) with increasing concentration, providing explicit details of the hydrogen-bond evolution in the aqueous solution.
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Carbon dioxide (CO2) capture coupled with further mineralization in high value-added form is a great challenge for carbon capture utilization and storage (CCUS) processes. In this work, a bipolar membrane electrodialysis (BMED) technique integrated with crystallization chamber was proposed to utilize CO2-derived carbonates and the residual magnesium resource from seawater to produce functional nesquehonite. To ensure the stable CO2 storage and magnesium extraction by BMED process, the metastable zone during nesquehonite crystallizing was first measured to modulate crystallization rate, obtain high-quality crystal products and inhibit membrane fouling states. Subsequently, the effects of current density, temperature, and CO2 flow rate during the whole BMED-crystallization process were further investigated. The increase in current density and temperature was conducive for the extraction of magnesium while the enlarged gas flow rate induced higher absorption of CO2. Under the current density at 22 A/m2, CO2 flow rate at 50 mL/min and temperature at 30 °C, the optimal carbon absorption ratio and the magnesium extraction ratio reached 50.85% and 56.71%, respectively. Under this condition, the explosion nucleation of the nesquehonite was effectively avoided to inhibit membrane fouling and the generation of magnesium hydroxide was depressed to obtain the target product nesquehonite. This study on simultaneous carbon capture and magnesium utilization provides theoretical guidance for the industrial green storage of CO2 and development of valuable magnesium products.
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Dióxido de Carbono , Magnesio , Dióxido de Carbono/química , Carbonatos , Magnesio/química , Agua de Mar/química , TemperaturaRESUMEN
The performance of the cathode significantly affects the ability of the electro-Fenton (EF) process to degrade chemicals. In this study, a simple method to modify the graphite felt (GF) cathode was proposed, i.e. oxidizing GF by hydrothermal treatment in nitric acid. The surface physical and electrochemical properties of modified graphite felt were characterized by several techniques: scanning electron microscope (SEM), water contact angle, X-ray photoelectron spectroscopy (XPS), Raman spectroscopy and linear scanning voltammetry (LSV). Compared with an unmodified GF (GF-0), the oxygen reduction reaction (ORR) activity of a modified GF was significantly improved due to the introduction of more oxygen-containing functional groups (OGs). Furthermore, the results showed that GF was optimally modified after 9 h (GF-9) of treatment. As an example, the H2O2 generation by GF-9 was 2.26 times higher than that of GF-0. After optimizing the process parameters, which include the initial Fe2+ concentration and current density, the apparent degradation rate constant of levofloxacin (LEV) could reach as high as 0.40 min-1. Moreover, the total organic carbon (TOC) removal rate and mineralization current efficiency (MCE) of the modified cathode were much higher than that of the GF-0. Conclusively, GF-9 is a promising cathode for the future development in organic pollutant removal via EF.
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Grafito , Contaminantes Químicos del Agua , Electrodos , Peróxido de Hidrógeno , Hierro , Levofloxacino , Oxidación-Reducción , Aguas ResidualesRESUMEN
Cell apoptosis induced by endoplasmic reticulum (ER) stress appears to be one of the main causes of myocardial necrosis following myocardial ischemia/reperfusion (MI/R). The C/EBP homologous protein (CHOP) pathway is the main pathway through which apoptosis is induced during ER stress. Glucose-regulated protein 78 (GRP78) is an important protein involved in the CHOP pathway. The present study investigated the hypothesis that MI/R activates the CHOP pathway through signaling via a pathway involving PKR-like ER kinase (PERK), α-subunit of eukaryotic initiation factor 2 (eIF2α) and activating transcription factor 2 (ATF2). Immunohistochemical staining of the heart tissues from spontaneously hypersensitive rats indicated that MI/R injury increases CHOP and GPR78 protein expression levels. To further analyze the mechanism by which MI/R injury induces apoptosis by ER stress, the expression levels of five marker proteins involved in the hypothetical PERK-eIF2α-ATF2 pathway were detected, namely PERK, phosphorylated PERK (P-PERK), eIF2α, phosphorylated eIF2α (P-eIF2α) and ATF2. An increase in the collective expression levels of these proteins would indicate that apoptosis was induced by this signaling pathway. In addition, the study also explored whether hypertension affects the signaling pathway of MI/R-induced myocardial apoptosis by treating spontaneously hypertensive rats (SHRs) with captopril (an effective drug used to treat hypertension). Rats treated with captopril experienced a reduction in blood pressure to normal levels, but no marked differences in the expression levels of the tested proteins or in MI/R injury severity compared with those in untreated rats. These results suggest that MI/R activates the CHOP pathway during ER stress by activating the PERK-eIF2α-ATF2 pathway and that hypertension does not affect this signaling pathway.