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1.
Environ Sci Technol ; 58(1): 947-959, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38153969

RESUMO

The unavoidable and detrimental formation of silica scale in engineered processes necessitates the urgent development of effective, economic, and sustainable strategies for dissolved silica removal from water. Herein, we demonstrate a rapid, chemical-free, and selective silica removal method using electrosorption. Specifically, we confirm the feasibility of exploiting local pH dynamics at the electrodes in flow-through electrosorption, achieved through a counterintuitive cell configuration design, to induce ionization and concomitant electrosorption of dissolved silica. In addition, to improve the feasibility of silica electrosorption under high-salinity solutions, we developed a silica-selective anode by functionalizing porous activated carbon cloths with aluminum hydroxide nanoparticles (Al(OH)3-p-ACC). The modification markedly enhances silica sorption capacity (2.8 vs 1.1 mgsilica ganode-1) and reduces the specific energy consumption (13.3 vs 19.8 kWh kgsilica-1). Notably, the modified electrode retains remarkable silica sorption capacity even in the presence of high concentrations of co-occurring ions (up to 100 mM NaCl). The mechanisms underlying the superior silica removal stability and selectivity with the Al(OH)3-p-ACC electrode are also elucidated, revealing a synergistic interaction involving outer-sphere and inner-sphere complexation between dissolved silica and Al(OH)3 nanoparticles on the electrodes. Moreover, we find that effective regeneration of the electrodes may be achieved by applying a reverse potential during discharge, although complete regeneration of the modified electrodes may necessitate alternative materials or process optimization. We recommend the adoption of feedwater-specific designs for the development of future silica-selective electrodes in electrosorption capable of meeting silica removal demands across a wide range of engineered systems.


Assuntos
Purificação da Água , Água , Dióxido de Silício , Estudos de Viabilidade , Cloreto de Sódio , Eletrodos
2.
Amino Acids ; 55(2): 173-182, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36588144

RESUMO

L-tryptophan has been used as a feed additive for swine and poultry and as a nutrient supplement for humans. However, some impurities in L-tryptophan have been reported as causative components of eosinophilia-myalgia syndrome. Therefore, from a safety perspective, it is important to analyze meat samples for these impurities. This study aims to develop an analytical method for the simultaneous detection of L-tryptophan impurities in meat products using LC-MS/MS. Among the various impurities, detection methods for (S)-2-amino-3-(5-hydroxy-1H-indol-3-yl)propanoic acid (5-hydroxytryptophan) (HTP), 1-methyl-1,2,3,4-tetrahydro-ß-carboline-3-carboxylic acid (MTCA), 3a-hydroxy-1,2,3,3a,8,8a-hexahydropyrrolo-[2,3-b]-indole-2-carboxylic acid (PIC), and 1,1'-ethylidenebistryptophan (EBT) and 2-(3-indoylmethyl)-L-tryptophan (IMT) were developed. The developed method allowed simultaneous determination of these four impurities in 5 min. No interferences from the matrix were observed, and the method showed good sensitivity to each analyte. The method detection limit and limit of quantification in meat matrices were below 11.2 and 35.7 µg/kg, respectively.


Assuntos
Síndrome de Eosinofilia-Mialgia , Produtos da Carne , Humanos , Animais , Suínos , Triptofano , Cromatografia Líquida , Espectrometria de Massas em Tandem , Cromatografia Líquida de Alta Pressão
3.
Environ Sci Technol ; 57(11): 4578-4590, 2023 03 21.
Artigo em Inglês | MEDLINE | ID: mdl-36893399

RESUMO

Boron removal from aqueous solutions has long persisted as a technological challenge, accounting for a disproportionately large fraction of the chemical and energy usage in seawater desalination and other industrial processes like lithium recovery. Here, we introduce a novel electrosorption-based boron removal technology with the capability to overcome the limitations of current state-of-the-art methods. Specifically, we incorporate a bipolar membrane (BPM) between a pair of porous carbon electrodes, demonstrating a synergized BPM-electrosorption process for the first time. The ion transport and charge transfer mechanisms of the BPM-electrosorption system are thoroughly investigated, confirming that water dissociation in the BPM is highly coupled with electrosorption of anions at the anode. We then demonstrate effective boron removal by the BPM-electrosorption system and verify that the mechanism for boron removal is electrosorption, as opposed to adsorption on the carbon electrodes or in the BPM. The effect of applied voltage on the boron removal performance is then evaluated, revealing that applied potentials above ∼1.0 V result in a decline in process efficiency due to the increased prevalence of detrimental Faradaic reactions at the anode. The BPM-electrosorption system is then directly compared with flow-through electrosorption, highlighting key advantages of the process with regard to boron sorption capacity and energy consumption. Overall, the BPM-electrosorption shows promising boron removal capability, with a sorption capacity >4.5 µmol g-C-1 and a corresponding specific energy consumption of <2.5 kWh g-B-1.


Assuntos
Boro , Purificação da Água , Água , Carbono , Água do Mar , Adsorção , Eletrodos , Purificação da Água/métodos
4.
Environ Sci Technol ; 56(9): 5763-5774, 2022 05 03.
Artigo em Inglês | MEDLINE | ID: mdl-35442651

RESUMO

This study reexamined the mechanisms for oxidative organic degradation by the binary mixture of periodate and H2O2 (PI/H2O2) that was recently identified as a new advanced oxidation process. Our findings conflicted with the previous claims that (i) hydroxyl radical (•OH) and singlet oxygen (1O2) contributed as the primary oxidants, and (ii) •OH production resulted from H2O2 reduction by superoxide radical anion (O2•-). PI/H2O2 exhibited substantial oxidizing capacity at pH < 5, decomposing organics predominantly by •OH. The likelihood of a switch in the major oxidant under varying pH conditions was revealed. IO4- as the major PI form under acidic conditions underwent one-electron reduction by H2O2 to yield radical intermediates, whereas H2I2O104- preferentially occurring at pH > 7 caused 1O2 generation through two-electron oxidation of H2O2. PI reduction by O2•- was suggested to be a key reaction in •OH production, on the basis of the electron paramagnetic resonance detection of methyl radicals in the dimethyl sulfoxide solutions containing PI and KO2, and the absence of deuterated and 18O-labeled hydroxylated intermediates during PI activation using D2O and H218O2. Finally, simple oxyanion mixing subsequent to electrochemical PI and H2O2 production achieved organic oxidation, enabling a potential strategy to minimize the use of chemicals.


Assuntos
Peróxido de Hidrogênio , Oxidantes , Espectroscopia de Ressonância de Spin Eletrônica , Radical Hidroxila , Oxirredução , Ácido Periódico , Superóxidos/metabolismo
5.
Environ Sci Technol ; 54(3): 1867-1877, 2020 02 04.
Artigo em Inglês | MEDLINE | ID: mdl-31934752

RESUMO

This study reports distillation-based salt removal by Ohmic heating in a hybrid process, in which electrochemical oxidation (EO) and direct contact membrane distillation (DCMD) are performed sequentially. In addition to anodically destructing the organics, the hybrid process also separated the sulfate-based electrolytes from treated water through distillation, without consuming external energy, owing to the temperature of the aqueous sulfate solution being elevated to 70 °C via resistive heating. The hybrid process treated organic compounds in a nonselective fashion, whereas DCMD alone did not completely reject (semi)volatile organics. Integrating EO with DCMD made the hybrid process resistant toward the wetting phenomenon; the process exhibited a steady distillate flux and salt rejection as the initial loading of amphiphilic sodium dodecyl sulfate was increased to 0.3 mM. Anodic persulfate formation from the sulfate and Ohmic heating caused an in situ yield of the sulfate radical in the feed solution; this eliminated membrane fouling, according to the observation that the water flux, which was drastically reduced upon adding alginate, was recovered immediately after an electric current was applied. The hybrid process concurrently decomposed spiked organics and removed naturally present inorganic ions in actual flue gas desulfurization wastewater, without an external supply of electrolyte and heat energy.


Assuntos
Destilação , Purificação da Água , Impedância Elétrica , Calefação , Membranas Artificiais
6.
Environ Sci Technol ; 51(18): 10700-10710, 2017 Sep 19.
Artigo em Inglês | MEDLINE | ID: mdl-28792745

RESUMO

A two-stage sequential electro-Fenton (E-Fenton) oxidation followed by electrochemical chlorination (EC) was demonstrated to concomitantly treat high concentrations of organic carbon and ammonium nitrogen (NH4+-N) in real anaerobically digested food wastewater (ADFW). The anodic Fenton process caused the rapid mineralization of phenol as a model substrate through the production of hydroxyl radical as the main oxidant. The electrochemical oxidation of NH4+ by a dimensionally stable anode (DSA) resulted in temporal concentration profiles of combined and free chlorine species that were analogous to those during the conventional breakpoint chlorination of NH4+. Together with the minimal production of nitrate, this confirmed that the conversion of NH4+ to nitrogen gas was electrochemically achievable. The monitoring of treatment performance with varying key parameters (e.g., current density, H2O2 feeding rate, pH, NaCl loading, and DSA type) led to the optimization of two component systems. The comparative evaluation of two sequentially combined systems (i.e., the E-Fenton-EC system versus the EC-E-Fenton system) using the mixture of phenol and NH4+ under the predetermined optimal conditions suggested the superiority of the E-Fenton-EC system in terms of treatment efficiency and energy consumption. Finally, the sequential E-Fenton-EC process effectively mineralized organic carbon and decomposed NH4+-N in the real ADFW without external supply of NaCl.


Assuntos
Compostos Clorados , Técnicas Eletroquímicas , Águas Residuárias , Alimentos , Halogenação , Peróxido de Hidrogênio , Ferro , Oxirredução , Poluentes Químicos da Água , Purificação da Água
7.
Bioresour Technol ; 402: 130792, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38703962

RESUMO

This study evaluates iron particle-integrated anammox granules (IP-IAGs) to enhance wastewater treatment efficiency. The IP-IAGs resulted in notable improvements in settleability and nitrogen removal. The settling velocity of IP-IAGs increased by 17.91 % to 2.92 ± 0.20 cm/s, and the total nitrogen removal efficiency in batch mode improved by 6.82 %. These changes indicate enhanced biological activity for effective treatment. In continuous operation, the IP-IAGs reactor showed no accumulation of nitrite until 40 d, reaching a peak nitrogen removal rate (NRR) of 1.54 kg-N/m3·d and a nitrogen removal efficiency of 82.61 %. Furthermore, a partial nitritation-anammox reactor that treated anaerobic digestion effluent achieved a NRR of 1.41 ± 0.09 kg-N/m3·d, proving the applicability of IP-IAGs in real wastewater conditions. These results underscore the potential of IP-IAGs to enhance the efficiency and stability of anammox-based processes, marking a significant advancement in environmental engineering for wastewater treatment.


Assuntos
Reatores Biológicos , Ferro , Nitrogênio , Águas Residuárias , Ferro/metabolismo , Ferro/química , Águas Residuárias/química , Oxirredução , Anaerobiose , Purificação da Água/métodos , Eliminação de Resíduos Líquidos/métodos , Nitritos/metabolismo
8.
Chemosphere ; 307(Pt 2): 135765, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35870605

RESUMO

This study investigated the potential of a novel fabricated black phosphorus (BP) nanoparticle electrode as an alternative to noble metal-based catalysts for application in electrolysis. The BP electrode was compared with other conventional catalysts (boron-doped diamond (BDD) and a dimensional stable electrode (DSA)) under different electrolyte conditions for the generation of specific oxidants (e.g., OH•, HOCl, OCl-, SO4• -) in the bulk phase during electrolysis. In the presence of sulfate-based electrolyte, results on the electrochemical oxidation showed that the BP not only resulted in an 8-fold increase in the current efficiency compared to DSA, but also reduced energy consumptions by approximately 30-fold. Moreover, electrolysis using certain electrodes (i.e., BDD) under high current densities in the presence of chlorine-based electrolyte has been reported to be hazardous to the water system due to the generation of toxic chlorine oxyanions (i.e., perchlorate), which necessitates the operation of a post-treatment process. Likewise, application of the BDD electrode was confirmed to produce perchlorate under high current densities, while no by-product was generated by electrolysis with the BP electrode. Finally, multiple degradation pathways for selective water treatment was monitored under oxidation with the BP electrode. To the best of our knowledge, this study is the first to apply the novel fabricated BP electrode as the anodic catalyst for the treatment of a water system.


Assuntos
Boro , Poluentes Químicos da Água , Cloro , Diamante , Eletrodos , Eletrólise/métodos , Oxidantes , Oxirredução , Percloratos , Fósforo , Sulfatos
9.
Toxicol Rep ; 9: 1099-1113, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36518375

RESUMO

The subchronic toxicity of oral L-tryptophan produced by fermentation with metabolically engineered Corynebacterium glutamicum was evaluated in Sprague-Dawley rats. Doses of 0, 500, 1000, and 2000 mg/kg/day were administered to groups of 10 male and 10 female rats for 90 days. For the groups administered 0 and 2000 mg/kg/day, an additional 5 male and 5 female rats were tested as a recovery group. No adverse effects associated with the test substance were observed in all rats during the 90-day administration of the product, irrespective of dose, and at 4 weeks of recovery at dosages of 0 and 2000 mg/kg/day. Furthermore, histochemical and immunohistochemical analyses for L-tryptophan-associated eosinophilia-myalgia syndrome (EMS) did not reveal significant changes in both sexes of groups administered 0 or 2000 mg/kg/day. Based on these results, it could be concluded that there were no significant adverse effects related to the test substance in all animals; therefore, dried L-tryptophan fermentation product can be used as feed additive material.

10.
Enzyme Microb Technol ; 115: 9-15, 2018 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-29859607

RESUMO

Escherichia coli has been a primary host for the prokaryotic production of antibody fragments (Fabs) and has contributed to several successes in the pharmaceutical industry. Nevertheless, the requirement of disulfide bonds often results in low-yield fermentation and a lack of cost-effectiveness. Despite the improved production of functional Fabs by fermentation below 30 °C, the limited cellular growth needs further work. To address these issues, we investigated the effect of nitrogen supply on the cellular growth and the Fab productivity. We used the anti-human VEGF-A Fab as a model that exhibited poor expression at 37 °C regardless of the amount of nitrogen supplied during fermentation. In stark contrast, the expression yield of soluble Fab with a gross nitrogen supply of 6.91 g/L of broth throughout the fermentation at 25 °C was 332 mg/L. Furthermore, and increased nitrogen supply of 10.9 g/L significantly improved the yield of active form by 59.7% and the cellular growth rate by 39.3%. These results indicate that overdosing of a nitrogen source at low temperature is critical to Fab productivity in E. coli.


Assuntos
Escherichia coli/metabolismo , Fermentação , Fragmentos de Imunoglobulinas/imunologia , Nitrogênio/metabolismo , Temperatura Baixa , Escherichia coli/genética , Escherichia coli/crescimento & desenvolvimento , Escherichia coli/imunologia , Humanos , Fragmentos de Imunoglobulinas/genética , Fator A de Crescimento do Endotélio Vascular/imunologia
11.
Adv Biochem Eng Biotechnol ; 159: 153-177, 2017.
Artigo em Inglês | MEDLINE | ID: mdl-27872967

RESUMO

L-Methionine has been used in various industrial applications such as the production of feed and food additives and has been used as a raw material for medical supplies and drugs. It functions not only as an essential amino acid but also as a physiological effector, for example, by inhibiting fat accumulation and enhancing immune response. Producing methionine from fermentation is beneficial in that microorganisms can produce L-methionine selectively using eco-sustainable processes. Nevertheless, the fermentative method has not been used on an industrial scale because it is not competitive economically compared with chemical synthesis methods. Presented are efforts to develop suitable strains, engineered enzymes, and alternative process of producing L-methionine that overcomes problems of conventional fermentation methods. One of the alternative processes is a two-step process in which the L-methionine precursor is produced by fermentation and then converted to L-methionine by enzymes. Directed efforts toward strain development and enhanced enzyme engineering will advance industrial production of L-methionine based on fermentation.


Assuntos
Aminoácidos/biossíntese , Fenômenos Fisiológicos Bacterianos , Fermentação/fisiologia , Aditivos Alimentares/metabolismo , Melhoramento Genético/métodos , Metionina/fisiologia , Aminoácidos/genética , Produtos Biológicos/síntese química , Produtos Biológicos/metabolismo , Reatores Biológicos/microbiologia
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