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1.
Chemosphere ; 289: 133119, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34864014

RESUMO

Organic amines are regarded as high toxic, refractory chemicals due to the great damage on human body, and ecosystem. The treatment of organic amine wastewater involves the removal of total nitrogen and toxic organics simultaneously, which is one of the biggest difficulties in wastewater treatment. In this study, hazardous organic amine wastewater was purified by a photocatalytic fuel cell (PFC) with efficient nitrogen removal and organic degradation, and its chemical energy was recovered simultaneously based on hydroxyl radical (HO·) and chlorine radical (Cl·) reaction in a novel TiO2/WO3 and 3D Cu nanowires modified Cu foam (CuNWs/CF) system. TiO2/WO3 heterojunction as photoanode provided rapid charge separation and good stability, and the composite of poly-Si enhanced the light harvest and charge transfer. HO· played critical role in degrading organic amines, while Cl· was responsible for selectively oxidizing amine group or NH4+ to N2. Besides, trace amount of NO2- and NO3- formed by over-oxidation was eliminated on CuNWs/CF cathode due to large specific surface area and fast charge transfer. Moderate Cl- concentration and initial pH had vital influence on strengthening Cl· and HO· generation in the system, and the optimal conditions were 50 mM NaCl and pH = 7. For methylamine, ethylamine and dimethylamine wastewater, the system showed total nitrogen removal efficiency of 94.93%, 91.81%, 93.10% and total organic carbon removal of 58.47%, 53.57%, and 56.71% within 2 h, respectively. Moreover, the corresponding maximum power densities of 2.49, 2.40, 2.27 mW cm-2 were also generated, respectively. The study proposes an efficient, sustainable method for the treatment of hazardous organic amine wastewater and simultaneous energy recovery.


Assuntos
Nanofios , Águas Residuárias , Aminas , Ecossistema , Eletricidade , Eletrodos , Humanos , Titânio
2.
Nanomaterials (Basel) ; 11(11)2021 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-34835546

RESUMO

Urine is the main source of nitrogen pollution, while urea is a hydrogen-enriched carrier that has been ignored. Decomposition of urea to H2 and N2 is of great significance. Unfortunately, direct urea oxidation suffers from sluggish kinetics, and needs strong alkaline condition. Herein, we developed a self-driving nano photoelectrocatalytic (PEC) system to efficiently produce hydrogen and remove total nitrogen (TN) for urine treatment under neutral pH conditions. TiO2/WO3 nanosheets were used as photoanode to generate chlorine radicals (Cl•) to convert urea-nitrogen to N2, which can promote hydrogen generation, due to the kinetic advantage of Cl-/Cl• cyclic catalysis. Copper nanowire electrodes (Cu NWs/CF) were employed as the cathode to produce hydrogen and simultaneously eliminate the over-oxidized nitrate-nitrogen. The self-driving was achieved based on a self-bias photoanode, consisting of confronted TiO2/WO3 nanosheets and a rear Si photovoltaic cell (Si PVC). The experiment results showed that hydrogen generation with Cl• is 2.03 times higher than in urine treatment without Cl•, generating hydrogen at 66.71 µmol h-1. At the same time, this system achieved a decomposition rate of 98.33% for urea in 2 h, with a reaction rate constant of 0.0359 min-1. The removal rate of total nitrogen and total organic carbon (TOC) reached 75.3% and 48.4% in 2 h, respectively. This study proposes an efficient and potential urine treatment and energy recovery method in neutral solution.

3.
Environ Sci Technol ; 55(21): 14854-14862, 2021 11 02.
Artigo em Inglês | MEDLINE | ID: mdl-34634907

RESUMO

H2S and CO2 are the main impurities in raw natural gas, which needs to be purified before use. However, the comprehensive utilization of H2S and CO2 has been ignored. Herein, we proposed a fully resource-based method to convert toxic gas H2S and greenhouse gas CO2 synchronously into CO and elemental S by using a novel electrochemical reactor. The special designs include that, in the anodic chamber, H2S was oxidized rapidly to S based on the I-/I3- cyclic redox system to avoid anode passivation. On the other hand, in the cathodic chamber, CO2 was rapidly and selectively reduced to CO based on a porous carbon gas diffusion electrode (GDE) modified with polytetrafluoroethylene and cobalt phthalocyanine (CoPc). A high Faraday efficiency (>95%) toward CO was achieved due to the enhanced mass transfer of CO2 on the GDE and the presence of the selective CoPc catalyst. The maximum energy efficiency of the system was more than 72.41% with a current density of over 50 mA/cm2, which was 12.5 times higher than what was previously reported on the H2S treatment system. The yields of S and CO were 24.94 mg·cm-2·h-1 and 19.93 mL·cm-2·h-1, respectively. A model analysis determined that the operation cost of the synchronous utilization of H2S and CO2 method was slightly lower than that of the single utilization of H2S in the existing natural gas purification technology. Overall, this paper provides efficient and simultaneous conversion of H2S and CO2 into S and CO.


Assuntos
Dióxido de Carbono , Gás Natural , Catálise , Eletrodos , Oxirredução
4.
Environ Sci Pollut Res Int ; 26(23): 23696-23706, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-31203550

RESUMO

Excessive nitrogen accumulated from wastewater with low C/N ratio is a new threat to water ecosystem. In this study, surface flow constructed wetland (SFCW) and floating treatment wetland (FTW) planted with Iris pseudacorus were set in parallel for nitrogen removal. The nitrogen removal efficiencies and pathways, as well as the abundance and functional diversities of the microbial community, were investigated. The results demonstrated that SFCW generally had better nitrogen removal performance than FTW did over four seasons. The average total nitrogen removal efficiency was 66.0% and 43.8% in SFCW and FTW, respectively. The plant uptake played a vital role in nitrogen reduction, which accounted for 29.3% and 7.7% of the total removed nitrogen in SFCW and FTW, respectively. A combination of high-throughput sequencing and quantitative polymerase chain reaction analysis revealed that the two wetland systems had complete nitrogen cycling, and the narG gene was the dominant nitrogen-transformation functional gene in both systems. More abundant denitrifying genes in SFCW than in FTW were also responsible for higher removal capacity of nitrogen. The results suggest that the planting pattern of wetland vegetation has an important impact on nitrogen removal efficiency by influencing the plant absorption and the development of microbial communities.


Assuntos
Gênero Iris/metabolismo , Nitrogênio/metabolismo , Poluentes Químicos da Água/metabolismo , Áreas Alagadas , Desnitrificação , Ecossistema , Nitrogênio/análise , Ciclo do Nitrogênio , Plantas/metabolismo , Estações do Ano , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias/análise , Água/análise , Poluentes Químicos da Água/análise
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