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1.
Environ Pollut ; 323: 121270, 2023 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-36780978

RESUMEN

Chlorinated organic pollutants (COPs) were widely detected in anaerobic environments while there is limited understanding of their pollution status and potential environmental risks. Here, we applied meta-analysis to identify the occurrence status, pollution sources, and environmental risk of COPs from 246 peer-published literature, including 25 kinds of COPs from 977 sites. The results showed that the median concentrations of COPs were at the ng g-1 level. By the combination of principal component analysis (PCA) and positive matrix factorization (PMF), we established 7 pollution sources for COPs. Environmental risk assessment found 73.3% of selected sites were at a security level but the rest were not, especially for the wetlands. The environmental risk of COPs was usually underestimated by the existing evaluation methods, such as without the consideration of the non-extractable residues (NER) and the multi-process coupling effect. Especially, the synergetic coupling associations between dechlorination and methanogenesis might increase the risk of methane emission that has barely been previously considered in previous risk assessment approaches. Our results expanded the knowledge for the pollution control and remediation of COPs in anaerobic environments.


Asunto(s)
Contaminantes Ambientales , Contaminantes del Suelo , Contaminantes Ambientales/análisis , Suelo/química , Contaminación Ambiental/análisis , Medición de Riesgo , Humedales , Contaminantes del Suelo/análisis , Monitoreo del Ambiente
2.
Angew Chem Int Ed Engl ; 62(15): e202216527, 2023 Apr 03.
Artículo en Inglés | MEDLINE | ID: mdl-36599818

RESUMEN

We reported a strategy of carbon-negative H2 production in which CO2 capture was coupled with H2 evolution at ambient temperature and pressure. For this purpose, carbonate-type Cux Mgy Fez layered double hydroxide (LDH) was preciously constructed, and then a photocatalysis reaction of interlayer CO3 2- reduction with glycerol oxidation was performed as driving force to induce the electron storage on LDH layers. With the participation of pre-stored electrons, CO2 was captured to recover interlayer CO3 2- in presence of H2 O, accompanied with equivalent H2 production. During photocatalysis reaction, Cu0.6 Mg1.4 Fe1 exhibited a decent CO evolution amount of 1.63 mmol g-1 and dihydroxyacetone yield of 3.81 mmol g-1 . In carbon-negative H2 production process, it showed an exciting CO2 capture quantity of 1.61 mmol g-1 and H2 yield of 1.44 mmol g-1 . Besides, this system possessed stable operation capability under simulated flu gas condition with negligible performance loss, exhibiting application prospect.

3.
Angew Chem Int Ed Engl ; 61(50): e202210596, 2022 12 12.
Artículo en Inglés | MEDLINE | ID: mdl-36179068

RESUMEN

The chemical industry is transitioning to more sustainable and biobased processes. One key element of this transition is coupling energy fluxes and feedstock utilization for optimizing processes, routes and efficiencies. Here, we show for the first time the coupling of the Kolbe electrolysis at the anode with a subsequent microbial conversion of the cathodically produced co-product hydrogen. Kolbe electrolysis of valeric acid yields the liquid drop-in fuel additive n-octane. Subsequently, the solvent isopropanol is produced by resting Cupriavidus necator cells using gaseous electrolysis products (esp. CO2 and H2 ). The resting microbial cells show carbon efficiencies of up to 41 % and Coulombic/Faradaic efficiencies of 60 % and 80 % for anodic and cathodic reactions, respectively. The implementation of a paired electrolyser resulted in superior process performances with overall efficiencies of up to 64.4 %.


Asunto(s)
Electrólisis , Hidrógeno , Solventes , Electrólisis/métodos , Electrodos , Dióxido de Carbono
4.
Materials (Basel) ; 13(21)2020 Nov 05.
Artículo en Inglés | MEDLINE | ID: mdl-33167579

RESUMEN

Nickel slags can be produced through ferronickel preparation by the pyrometallurgical processing of laterite nickel ores; however, such techniques are underutilized at present, and serious environmental problems arise from the stockpiling of such nickel ores. In this study, a modification to the process of ferronickel preparation by the direct reduction of carbon bases in laterite nickel ores is proposed. The gangue from the ore is used as a raw material to prepare a cementitious material, with the main components of tricalcium silicate and tricalcium aluminate. By using FactSage software, thermodynamic calculations are performed to analyze the reduction of nickel and iron and the effect of reduction on the formation of tricalcium silicate and tricalcium aluminate. The feasibility of a coupled process to prepare ferronickel and cementitious materials by the direct reduction of laterite nickel ore and gangue calcination, respectively, is discussed under varying thermodynamic conditions. Different warming strategies are applied to experimentally verify the coupled reactions. The coupled preparation of ferronickel and cementitious materials with calcium silicate and calcium aluminate as the main phases in the same experimental process is realized.

5.
J Environ Manage ; 223: 878-887, 2018 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-29990877

RESUMEN

In this work, the electrochemical oxidation of antibiotic ampicillin (AMP) on a boron-doped diamond anode in the presence of sodium persulfate (SPS) was investigated (EO/SPS process). Experiments were conducted at AMP concentrations between 0.8 and 3 mg/L, SPS concentrations between 100 and 500 mg/L, current densities between 5 and 110 mA/cm2, in three water matrices (ultrapure water, bottled water and secondary treated wastewater), using 0.1 M Na2SO4 as the supporting electrolyte. AMP degradation follows a pseudo-first order kinetic expression with the apparent rate constant increasing with (i) increasing SPS concentration (from 0.08 min-1 to 0.36 min-1 at 0 and 500 mg/L SPS, respectively, 1.1 mg/L AMP, 25 mA/cm2), (ii) increasing current (from 0.08 min-1 to 0.6 min-1 at 5 and 110 mA/cm2, respectively, 1.1 mg/L AMP, 250 mg/L SPS), and (iii) decreasing AMP concentration (from 0.16 min-1 to 0.31 min-1 at 3 and 0.8 mg/L, respectively, 250 mg/L SPS, 25 mA/cm2). The presence of various anions (mainly bicarbonates) in bottled water did not impact AMP degradation. The observed kinetic constant decreased by 40% in the presence of 10 mg/L humic acid. On the other hand, process efficiency was enhanced almost 3.5 times in secondary effluent due to the electrogeneration of active chlorine species that promote indirect oxidation reactions in the bulk solution. The efficacy of the EO/SPS process was compared to and found to be considerably greater than a process where SPS was activated by simulated solar irradiation at an intensity of 7.3 × 10-7 E/(L.s) (SLR/SPS process). Coupling the two processes (EO/SLR/SPS) resulted in a cumulative, in terms of AMP degradation, effect. The combined process was tested for AMP degradation, mineralization and inhibition to Vibrio fischeri in wastewater; fast AMP removal was accompanied by low mineralization and incomplete toxicity removal.


Asunto(s)
Ampicilina/química , Compuestos de Sodio , Sulfatos , Contaminantes Químicos del Agua/química , Antibacterianos , Boro , Diamante , Electrodos , Cinética , Oxidación-Reducción
6.
Appl Microbiol Biotechnol ; 101(17): 6575-6586, 2017 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-28766035

RESUMEN

The mixed culture fermentation is an important environmental biotechnology that converts biodegradable organic wastes to valuable chemicals such as hydrogen, methane, acetate, ethanol, propionate, and so on. For the multistep process of hydrolysis, acidogenesis, acetogenesis/homoacetogensis, and methanogenesis, the typical metabolic reactions are firstly summarized. And then, since the final metabolites are always a mixture, the separation and purification processes are necessary to couple with anaerobic fermentation. Therefore, several typical coupling technologies including biogas upgrading, two-stage fermentation, gas stripping, membrane technology of pervaporation, membrane distillation, electrodialysis, bipolar membrane electrodialysis, and microbial fuel cells are summarized to separate the metabolites and recover energy. At last, the novel technologies such as the controlled metabolite production, medium chain carboxylic acid production, and high temperature ethanol recovery in thermophilic mixed culture fermentation are also reviewed. However, the novel concepts are still needed to meet the demands of better overall performances and lower total costs.


Asunto(s)
Reactores Biológicos , Metabolismo Energético , Fermentación , Redes y Vías Metabólicas , Ácido Acético/metabolismo , Anaerobiosis , Biocombustibles , Biotecnología , Etanol/metabolismo , Hidrólisis , Metano/metabolismo
7.
Front Microbiol ; 7: 891, 2016.
Artículo en Inglés | MEDLINE | ID: mdl-27445993

RESUMEN

Synthesis gas (syngas) fermentation using acetogenic bacteria is an approach for production of bulk chemicals like acetate, ethanol, butanol, or 2,3-butandiol avoiding the fuel vs. food debate by using carbon monoxide, carbon dioxide, and hydrogen from gasification of biomass or industrial waste gases. Suffering from energetic limitations, yields of C4-molecules produced by syngas fermentation are quite low compared with ABE fermentation using sugars as a substrate. On the other hand, fungal production of malic acid has high yields of product per gram metabolized substrate but is currently limited to sugar containing substrates. In this study, it was possible to show that Aspergilus oryzae is able to produce malic acid using acetate as sole carbon source which is a main product of acetogenic syngas fermentation. Bioreactor cultivations were conducted in 2.5 L stirred tank reactors. During the syngas fermentation part of the sequential mixed culture, Clostridium ljungdahlii was grown in modified Tanner medium and sparged with 20 mL/min of artificial syngas mimicking a composition of clean syngas from entrained bed gasification of straw (32.5 vol-% CO, 32.5 vol-% H2, 16 vol-% CO2, and 19 vol-% N2) using a microsparger. Syngas consumption was monitored via automated gas chromatographic measurement of the off-gas. For the fungal fermentation part gas sparging was switched to 0.6 L/min of air and a standard sparger. Ammonia content of medium for syngas fermentation was reduced to 0.33 g/L NH4Cl to meet the requirements for fungal production of dicarboxylic acids. Malic acid production performance of A. oryzae in organic acid production medium and syngas medium with acetate as sole carbon source was verified and gave YP∕S values of 0.28 g/g and 0.37 g/g respectively. Growth and acetate formation of C. ljungdahlii during syngas fermentation were not affected by the reduced ammonia content and 66 % of the consumed syngas was converted to acetate. The overall conversion of CO and H2 into malic acid was calculated to be 3.5 g malic acid per mol of consumed syngas or 0.22 g malic acid per gram of syngas.

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