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Effective degradation of phenol via catalytic wet peroxide oxidation over N, S, and Fe-tridoped activated carbon
2020
Yang, Guo | Mo, Sha | Xing, Bo | Dong, Jingwen | Song, Xiang | Liu, Xingyong | Yuan, Jigang
The N, S, and Fe-tridoped carbon catalysts (NSFe-Cs), Fe/ACNS1 and Fe/ACNS2, were synthesized by wet impregnation with different concentration of ammonium ferrous sulfate solution. The prepared catalysts have a similar textural structure. The N species, S species, Feᴵᴵ and Feᴵᴵᴵ were simultaneously introduced onto the surface of catalysts. Comparison with the only Fe doped catalyst, NSFe-Cs showed greater stability and higher phenol removal in catalytic wet peroxide oxidation at different reaction condition. The main intermediates including p-hydroxybenzoic acid, formic acid, and maleic acid were determined in the treated wastewater. The high catalytic activity for NSFe-C was related to the ability of H₂O₂ decomposition. NSFe-Cs have more amount of Feᴵᴵ partially due to the formation of FeS₂, which promoted the decomposition of H₂O₂ on Fe/ACNS1 and Fe/ACNS2 surface. The generation of ·OH and ·HO₂/·O₂⁻ radicals in the bulk solution was crucial to phenol degradation, and the decomposition of H₂O₂ complied with the pseudo-first-order kinetics. The highly linear relationship between decomposition kinetic constant for H₂O₂ and the amount of surface groups suggested, including Feᴵᴵ species, pyridinic N/Fe-bonded N, pyrrolic N as well as graphitic N were responsible to the high activity of NSFe-Cs.
显示更多 [+] 显示较少 [-]Selenium and arsenic removal from water using amine sorbent, competitive adsorption and regeneration
2021
Wei, Jinshan | Shen, Bo | Ye, Gan | Wen, Xianghua | Song, Yonghui | Wang, Jin | Meng, Xiaoguang
Selenium (Se) and arsenic (As) are toxic contaminants in surface water and drinking water. The human body needs little quantity of Se, but too high dose is not allowed. Metal oxides such as iron oxides were used for adsorption or co-precipitation removal of As from water. However, the regeneration and stability problems of metals oxides sorbents are unsatisfactory , and there is not enough adsorbent for Se removal from water also. We developed the acrylic amine fiber (AAF) for adsorption reomval of Se and As from water and systematically studied the influenced factors. Batch experiments were conducted for investigating the adsorption edges, while column filtration tests were employed for dynamic application edges. At neutral pH, the Langmuir isotherm fittings gave the maximum adsorption capacities of As(V), As(III), Se(VI) and Se(IV) are 270.3, 40.5, 256.4, and 158.7 mg/g, respectively. Effects of co-existing inorganic anions on As(V) and Se(VI) adsorption using AAF gave the order of PO₄³⁻ > SO₄²⁻ > NO₃⁻ > SiO₃²⁻, while different organic acids obey the order of citric acid > oxalic acid > formic acid. Fourier transform infrared analysis showed the PO₄³⁻ and SO₄²⁻ competition mechanisms are electrostatic repulsions, while the competition of organic acids derived from acid-base reaction between the carboxyl group and the amino group. Column filtration and regeneration results showed that the spent AAF can be regenerated using 0.5 mol/L HCl solution and reused with no much decrease of adsorption capacity.
显示更多 [+] 显示较少 [-]Multisize particulate matter and volatile organic compounds in arid and semiarid areas of Northwest China
2022
Zhou, Xi | Li, Zhongqin | Zhang, Tingjun | Wang, Feiteng | Tao, Yan | Zhang, Xin
To investigate the chemical components, sources, and interactions of particulate matter (PM) and volatile organic compounds (VOCs), a field campaign was implemented during the spring of 2018 in nine cities in northwestern (NW) China. PM was mainly contributed by organic matter and water-soluble inorganic ions (41% for PM₁₀ and approximately 60% for PM₂.₅ and PM₁). Two typical haze patterns were observed: anthropogenic pollution type (AP-type), wherein contributions of sulfate, nitrate, and ammonium (SNA) increased, and dust pollution type (DP-type), wherein contributions of Ca²⁺ increased and SNA decreased. Source appointment suggested that regional sources contributed close to half to PM₂.₅ pollution (40% for AP-type and 50% for DP-type). Thus, sources from regional transport are also important for haze and dust pollution. The ranking of VOC concentrations was methanol > acetaldehyde > formic acid + ethanol > acetone. Compared with other cities, there are higher oxygenated VOCs (OVOCs) and lower aromatics in NW China. The relationships between VOCs and PM were discussed. The dominating secondary organic aerosols (SOA) formation potential precursors were C₁₀–aromatics, xylene, and styrene under low–nitrogen oxide (NOx) conditions, and benzene, C₁₀–aromatics, and toluene dominated under high–NOx conditions. The quadratic polynomial was the most suitable fitting model for their correlation, and the results suggested that VOC oxidations explained 6.1–10.8% and 9.9–20.7% of SOA formation under high–NOx and low–NOx conditions, respectively.
显示更多 [+] 显示较少 [-]Streptomyces pactum and sulfur mediated the rhizosphere microhabitats of potherb mustard after a phytoextraction trial
2021
Guo, Di | Ali, Amjad | Zhang, Zengqiang
To explore the performance of Streptomyces pactum (Act12) alone (A) and jointly with sulfur (SA) in the phytoextraction practice of potentially toxic elements (PTEs) (Cd and Zn), as well as their effects on soil chemical properties and microbial community composition, this paper selected potherb mustard (Brassica juncea, Coss.) as the test plant to assess the feedback of soil-plant ecosystems. Metal uptake values in lone Act12 treatments were higher than that of Act12 + sulfur treatments, and showed dose dependent with Act12 due to the higher biomass production. According to the biochemical analyses of rhizosphere soils, Act12 inoculation significantly increased urease (20.4%) and dehydrogenase (58.5%) while reducing alkaline phosphatase (68.0%) activity. The production of soil organic acids was, in descending order, formic acid > oxalic acid > malic acid > propionic acid and indicated a stimulated variation under treatments (SA > A > control). High-throughput sequencing revealed that bacterial community compositions were consistent in both phylum and genus taxonomies, while the final overall proportions were modified. The populations of the predominant phyla Proteobacteria and Bacteroidetes increased after sulfur application. The contribution of Act12 to the relative abundance of microbiota was minor compared to sulfur. Based on a redundancy analysis, soil chemical properties are the drivers of microbial activities and the main contributor to plant growth. Our results suggested Act12 inoculation may be part of an effective strategy enhancing phytoremediation of PTE-contaminated soils through chemical and biotic processes, and provided important implications for sustainable land utilization and crop production.
显示更多 [+] 显示较少 [-]Heterologous expression of bacterial cytochrome P450 from Microbacterium keratanolyticum ZY and its application in dichloromethane dechlorination
2021
Hu, Jun | Zhang, Yan | Wu, Yuexin | Zheng, Jiajun | Yu, Zhiliang | Qian, Haifeng | Yu, Jianming | Cheng, Zhuowei | Chen, Jianmeng
Dichloromethane (DCM) is a volatile halogenated hydrocarbon with teratogenic, mutagenic and carcinogenic effects. Biodegradation is generally regarded as an effective and economical approach of pollutant disposal. In this study, a novel strain was isolated and its cytochrome P450 was heterologously expressed for DCM degradation. The isolate, Microbacterium keratanolyticum ZY, was characterized as a Gram-positive, rod-shaped and flagella-existed bacterium without spores (GenBank No. SUB8814364; CCTCC M 2019953). After successive whole-genome sequencing, assembly and annotation, eight identified functional genes (encoding cytochrome P450, monooxygenase, dehalogenase and hydrolase) were successfully cloned and expressed in Escherichia coli BL21 (DE3). The recombinant strain expressing cytochrome P450 presented the highest degradation efficiency (90.6%). Moreover, the specific activity of the recombinant cytochrome P450 was more than 1.2 times that of the recombinant dehalogenase (from Methylobacterium rhodesianum H13) under their optimum conditions. The kinetics of DCM degradation by recombinant cytochrome P450 was well fitted with the Haldane model and the value of maximum specific degradation rate was determined to be 0.7 s⁻¹. The DCM degradation might occur through successive hydroxylation, dehydrohalogenation, dechlorination and oxidation to generate gem-halohydrin, formyl chloride, formaldehyde and formic acid. The study helps to comprehensively understand the DCM dechlorination process under the actions of bacterial functional enzymes (cytochrome P450 and dehalogenase).
显示更多 [+] 显示较少 [-]Research on the nitrogen cycle in rhizosphere of Kandelia obovata under ammonium and nitrate addition
2013
Weng, Bosen | Xie, Xiangyu | Yang, Jinjin | Liu, Jingchun | Lu, Haoliang | Yan, Chongling
The present study investigated nitrogen process in rhizosphere of Kandelia obovata under nitrogen input. Results showed that nitrogen additions significantly increased 4 kinds of enzyme activities (Urease, Nitrate reductase, Nitrite reductase and hydroxylamine reductase). The pH value increased to 7.1 under ammonium addition, but decreased to 6.9 under nitrate addition. Potential Nitrification Intensity (PNI) increased 200–1500% compared with control under ammonium addition, and Potential Denitrification Intensity (PDI) increased more than 200% under nitrate addition. Ten types of organic acids were detected from root exudates, which mainly included oxalic acid, tartaric acid, formic acid, acetic acid, and citric acid. The abundance of 5 kinds of microbial functional groups (nifH, AOA, AOB, nirS, nirK) responded differently. Total nitrogen in organs of K. obovata increased more than 200%. This indicated that nitrogen additions accelerated the transformation of nitrogen directly and stimulated the exudation of root exudates and 5 kinds of genes indirectly.
显示更多 [+] 显示较少 [-]Treatment of methyldiethanolamine wastewater using subcritical and supercritical water oxidation: parameters study, process optimization and degradation mechanism
2022
Ghasemi, Mohammad Noor | Esmaeilzadeh, Feridun | Mowla, Dariush | Elhambakhsh, Abbas
In this examination, sub/supercritical water oxidation (SCWO) in a batch reactor was employed to degrade methyldiethanolamine (MDEA). To do so, the impact of different operating parameters including temperature (300–500 °C), time (0–100 s), initial MDEA concentration (1000–4000 ppm), oxidant coefficient (0.7–2), and pH (7.3–9.5) on MDEA degradation was separately and together investigated. Subsequently, the response surface method (RSM) was applied to optimize the operating condition of MDEA degradation. Based on the obtained results, a maximum amount of 97.4% MDEA degradation was achieved at the initial MDEA concentration of 1095 ppm in optimal condition (i.e., oxidant coefficient: 1.913, temperature: 472 °C and residence time: about 17 s). Furthermore, according to the HPLC analysis, there was a negligible amounts of formic acid (CH₂O₂) and nitrous acid (HNO₂) in the solution at the end of MDEA removal experiment. Eventually, the mechanism of MDEA degradation was acquired using molecular dynamics simulation (MDS), which had an acceptable coordination with the experimental results. In this way, the MDS results revealed that the presence of CH₂O₂ and HNO₂ compounds in the products was related to the degradation of MDEA and their production as by-products during the SCWO experiments.
显示更多 [+] 显示较少 [-]Superficial properties of activated carbon fiber catalysts produced by green synthesis and their application in water purification
2020
Zoppas, Fernanda Miranda | Beltrame, Thiago Favarini | Sosa, Florencia Agustina | Bernardes, Andrea Moura | Miró, Eduardo | Marchesini, Fernanda Albana
Catalysts of Pd-In supported on activated carbon fiber were synthesized, characterized, and evaluated for the removal of nitrogen oxyanions from water. The work was carried out aiming the development of a green synthesis process, and the studies were accomplished with the following objectives: (a) to evaluate whether catalysts produced by wet impregnation (WI) and autocatalytic deposition (AD) have enough catalytic activity for the removal of oxyanions in water; (b) to determine the efficiency of ion removal using formic acid as a reducing agent; (c) to determine which synthesis method produces less waste. It was found that the two synthesis processes modified the properties of the support and that the distribution of the particles of the metallic phase was of the nanometric order, being these particles found predominantly at the support surface. By using formic acid as a reducing agent, although low nitrate conversions were obtained (32%), a selectivity to N₂ higher than 99% was achieved. These findings were attributed to the low decomposition of formic acid on the catalyst surface. The Pd:In (0.45:0.2) catalyst prepared by WI was the most suitable for the catalytic reduction of both nitrate and nitrite oxyanions. Regarding the green point of view of the synthesis method, catalysts prepared by WI generated less waste. Graphical abstract
显示更多 [+] 显示较少 [-]Antituberculosis drug isoniazid degraded by electro-Fenton and photoelectro-Fenton processes using a boron-doped diamond anode and a carbon-PTFE air-diffusion cathode
2019
Solutions with 0.65 mM of the antituberculosis drug isoniazid (INH) in 0.050 M Na₂SO₄ at pH 3.0 were treated by electro-Fenton (EF) and UVA photoelectro-Fenton (PEF) processes using a cell with a BDD anode and a carbon-PTFE air-diffusion cathode. The influence of current density on degradation, mineralization rate, and current efficiency has been thoroughly evaluated in EF. The effect of the metallic catalyst (Fe²⁺ or Fe³⁺) and the formation of products like short-chain linear aliphatic carboxylic acids were assessed in PEF. Two consecutive pseudo-first-order kinetic regions were found using Fe²⁺ as catalyst. In the first region, at short time, the drug was rapidly oxidized by ●OH, whereas in the second region, at longer time, a resulting Fe(III)-INH complex was much more slowly removed by oxidants. INH disappeared completely at 300 min by EF, attaining 88 and 94% mineralization at 66.6 and 100 mA cm⁻², respectively. Isonicotinamide and its hydroxylated derivative were identified as aromatic products of INH by GC-MS and oxalic, oxamic, and formic acids were quantified by ion-exclusion HPLC. The PEF treatment of a real wastewater polluted with the drug led to slower INH and TOC abatements because of the parallel destruction of its natural organic matter content.
显示更多 [+] 显示较少 [-]Degradation of p-Nitrophenol in Soil by Dielectric Barrier Discharge Plasma
2015
Li, Rui | Liu, Yanan | Sun, Yu | Zhang, Wenjuan | Mu, Ruiwen | Li, Xiang | Chen, Hong | Gao, Pin | Xue, Gang | Ognier, Stephanie
Dielectric barrier discharges (DBDs) were utilized for the remediation of soil contaminated with p-nitrophenol (PNP). The effect of treatment time, applied discharge voltage, initial PNP concentration, pH of contaminated soil, and airflow rate were investigated in this study. The results showed that 63.2 % of the PNP in the contaminated soil was degraded in 50 min with a voltage of 38.2 kV with no airflow. This degradation reaction followed the first order reaction kinetics. The degradation by ozone alone was compared with the plasma treatment to identify the role of ozone. Chromatographic analysis was applied to monitor the intermediates produced during the oxidation process, and the main byproducts were maleic acid, p-benzoquinone, 4-nitrocatechol, methanoic acid, acetic acid, oxalic acid, NO₂ ⁻, and NO₃ ⁻. Possible pathways for the degradation of PNP in this system were deduced, which would provide evidence for the researches about the remediation of soils polluted by organic pollutants.
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