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Remediation techniques for uranium removal from polluted environment – Review on methods, mechanism and toxicology
2022
Akash, S. | Sivaprakash, Baskaran | Raja, V.C Vadivel | Rajamohan, Natarajan | Muthusamy, Govarthanan
Uranium, a radionuclide, is a predominant element utilized for speciality requirements in industrial applications, as fuels and catalyst. The radioactive properties and chemical toxicity of uranium causes a major threat to the ecosystem. The hazards associated with Uranium pollution includes the cancer in bones, liver, and lungs. The toxicological properties of Uranium are discussed in detail. Although there are many methods to eliminate those hazards, this research work is aimed to describe the application of bioremediation methods. Bioremediation methods involve elimination of the hazards of uranium, by transforming into low oxidation form using natural microbes and plants. This study deeply elucidates the methods as bioleaching, biosorption, bioreduction and phytoremediation. Bioleaching process involves bio-oxidation of tetravalent uranium when it gets in contact with acidophilic metal bacterial complex to obtain leach liquor. In biosorption, chitin/chitosan derived sorbents act as chelators and binds with uranium by electrostatic attraction. Bio reduction employs a bacterial transformation into enzymes which immobilize and reduce uranium. Phytoremediation includes phytoextraction and phytotranslocation of uranium through xylems from soil to roots and shoots of plants. The highest uranium removal and uptake reported using the different methods are listed as follows: bioleaching (100% uranium recovery), biosorption (167 g kg⁻¹ uranium uptake), bioreduction (98.9% uranium recovery), and phytoremediation (49,639 mg kg⁻¹ uranium uptake). Among all the techniques mentioned above, bioleaching has been proved to be the most efficient for uranium remediation.
Show more [+] Less [-]Cooperation of multiple active species generated in hydrogen peroxide activation by iron porphyrin for phenolic pollutants degradation
2022
Yang, Xiaorong | Hu, Jingping | Wu, Longsheng | Hou, Huijie | Liang, Sha | Yang, Jiakuan
The narrow acid pH range and the nonselectivity of the dominant •OH limit the Fenton systems to remediate the organic wastewater. Inspired by the role of heme in physiological processes, we employed iron porphyrin as a novel homogeneous catalyst to address this issue. Multiple active species are identified during the activation of H₂O₂, including high-valent iron porphyrin ((por)Fe(IV)) species ((por)Fe(IV)–OH, (por)⁺•Fe(IV)=O) and oxygen-centered radicals (•OH, HO₂•/•O₂⁻), as well as atomic hydrogen (*H) and carbon-centered radicals. With the cooperation of these active species, the degradation of pollutants could be resistant to the interference of concomitant ions and proceed over a wide pH range. This cooperative behavior is further verified by intermediates identified from bisphenol A degradation. Specifically, the presence of *H could facilitate the cleavage of the C–C bond and the addition of unsaturated or aromatic molecules. (Por)⁺•Fe(IV)=O could hydroxylate substrates with an oxygen rebound mechanism. Hydrogen atom abstraction of contaminants could be performed by (por)Fe(IV)–OH to form desaturated products by attacking oxygen-centered radicals. The ecotoxicity of bisphenol A could be significantly decreased through degradation. This study would provide a new approach to wastewater treatment and shed light on the interaction between metalloporphyrin and peroxide in an aqueous solution.
Show more [+] Less [-]Catalytic hydrogenolysis of plastic to liquid hydrocarbons over a nickel-based catalyst
2022
Zhao, Zhigang | Li, Zheng | Zhang, Xiangkun | Li, Tan | Li, Yuqing | Chen, Xingkun | Wang, Kaige
The catalytic hydrogenolysis of a typical model compound of mulching film waste, polyethylene, was investigated as a potential way to improve economic efficiency of mulching film recycling. Nickel-based heterogeneous catalysts are proposed for polyethylene hydrogenolysis to produce liquid hydrocarbons. Among catalysts supported on various carriers, Ni/SiO₂ catalyst shows the highest activity which may due to the interactions between nickel and silica with the formation of nickel phyllosilicate. As high as 81.18% total gasoline and diesel range hydrocarbon was obtained from the polyethylene hydrogenolysis at relatively mild condition of 280 °C, and 3 MPa cold hydrogen pressure. The result is comparable to what have been reported in previous studies using noble metal catalysts. The gasoline and diesel range hydrocarbon are n-alkanes with a distribution at a range of C₄–C₂₂. The gas products are primarily CH₄ along with a small amount of C₂H₆ and C₃H₈. High yield of CH₄ as much as 9.68% was observed for the cleavage of molecule occurs along the alkane chain.
Show more [+] Less [-]Metal-free single heteroatom (N, O, and B)-doped coconut-shell biochar for enhancing the degradation of sulfathiazole antibiotics by peroxymonosulfate and its effects on bacterial community dynamics
2022
Hung, Chang-Mao | Chen, Chiu-Wen | Huang, Jinbao | Dong, Cheng-Di
Metal-free single heteroatom (N, O, and B)-doped coconut-shell biochar (denoted as N-CSBC, O-CSBC, and B-CSBC, respectively) were fabricated in a one-step pyrolysis process to promote peroxymonosulfate (PMS) activation for the elimination of sulfathiazole (STZ) from aquaculture water. B-CSBC exhibited remarkably high catalytic activity with 92% of STZ degradation in 30 min attributed to the presence of meso-/micro-pores and B-containing functional groups (including B–N, B–C, and B₂O₃ species). Radical quenching tests revealed SO₄•⁻, HO•, and ¹O₂ being the major electron acceptors contributing to STZ removal by PMS over B-CSBC catalyst. The B-CSBC catalyst has demonstrated high sustainability in multiple consecutive treatment cycles. High salinity and the presence of inorganic ions such as chloride, enhanced the performance of the sulfate radical-carbon-driven advanced oxidation processes (SR–CAOPs) as pretreatment strategy that significantly facilitated the removal of STZ from aquaculture water. Furthermore, a potential sulfonamide-degrading microorganism, Cylindrospermum_stagnale, belonging to the phylum Cyanobacteria, was the dominant functional bacteria according to the results of high-throughput 16S rRNA gene sequencing conducted after the B-CSBC/PMS treatment. This study provides new insights into the SR–CAOP combined with bioprocesses for removing STZ from aqueous environments.
Show more [+] Less [-]Mechanism of biochar functional groups in the catalytic reduction of tetrachloroethylene by sulfides
2022
Yang, Yadong | Piao, Yunxian | Wang, Ruofan | Su, Yaoming | Qiu, Jinrong | Liu, Na
In recent years, biochar has become of considerable interest for environmental applications, it can be used as a catalyst for sulfides reduction of perchloroethylene, but the crucial role of biochar properties played in catalyzing dechlorination remained ambiguous investigation. To pinpoint the critical functional groups, the modified biochars were respectively produced by HNO₃, KOH and H₂O₂ with similar dimensional structures but different functional groups. Combined with the adsorption and catalytic results of different biochars, the acid-modified biochar had the best catalytic performance (99.9% removal) due to the outstanding specific surface area and ample functional groups. According to characterization and DFT results, carboxyl and pyridine nitrogen exhibited a positive correlation with the catalytic rate, indicating that their contribution to catalytic performance. Customizing biochar with specific functional groups removed depth demonstrated that the carboxyl was essential component. Further, alkaline condition was conducive to catalytic reduction, while tetrachloroethylene cannot be reduced under acidic conditions, because HS⁻ and S²⁻ mainly existed in alkaline environment and the sulfur-containing nucleophilic structure formed with biochar was more stable under this condition. Overall, this study opens new perspectives for in situ remediation by biochar in chlorinated olefin polluted anoxic environment and promotes our insight of modifying for biochar catalyst design.
Show more [+] Less [-]Synthesis of dye-sensitized TiO2/Ag doped nano-composites using UV photoreduction process for phenol degradation: A comparative study
2022
Behera, Amit Kumar | Shadangi, Krushna Prasad | Sarangi, Prakash Kumar
This study investigates a comparison between the photocatalytic action of two nanocomposites (TiO₂ and TiO₂(Ag) doped) on the degradation of phenol from water. The nanocomposites were synthesized by the UV photo-reduction process to get a silver metal loading of 0.25, 0.5, 0.75, and 1% (w/w). In addition to this, Eriochrome Cyanine Red (ECR) and Eosin Yellow (EY) both anionic dyes were used for sensitization of Ag-doped TiO₂ photo-catalyst such as TiO₂(Ag)ECR and TiO₂(Ag)EY. The TiO₂(Ag-1.0)EY photo-catalyst indicated higher absorbance compared to the TiO₂(Ag-1.0)ECR in the 400–700 nm range (visible range). The degradation of phenol was tested by varying the pH, silver loading and catalyst dosage. The maximum degradation of phenol was 98% in 180 min at pH 7 in presence of 1% (w/w) silver loading with 0.5 gL⁻¹ dosage of photo-catalyst TiO₂(Ag-1.0)EY. At this condition, the reduction in the phenol concentration was noticed from 20 mg/L to 0.4 mg/L.
Show more [+] Less [-]Mitigation of hazardous toluene via ozone-catalyzed oxidation using MnOx/Sawdust biochar catalyst
2022
Cha, Jin Sun | Kim, Young-Min | Lee, Im Hack | Choi, Yong Jun | Rhee, Gwang Hoon | Song, Hocheol | Jeon, Byong-Hun | Lam, Su Shiung | Khan, Moonis Ali | Andrew Lin, Kun-Yi | Chen, Wei-Hsin | Park, Young-Kwon
This study investigated catalytic ozone oxidation using a sawdust char (SDW) catalyst to remove hazardous toluene emitted from the chemical industry. The catalyst properties were analyzed by proximate, ultimate, nitrogen adsorption-desorption isotherms, Fourier-transform infrared, and X-ray photoelectron spectroscopy analyses. In addition, hydrogen-temperature programmed reduction experiments were conducted to analyze the catalyst properties. The specific area and formation of micropores of SDC were improved by applying KOH treatment. MnOx/SDC-K3 exhibited a higher toluene removal efficiency of 89.7% after 100 min than MnOx supported on activated carbon (MnOx/AC) with a removal efficiency of 6.6%. The higher (Oₐdₛ (adsorbed oxygen)+Oᵥ(vacancy oxygen))/OL (lattice oxygen) and Mn³⁺/Mn⁴⁺ ratios of MnOx/SDC-K3 than those of MnOx/AC seemed to be important for the catalytic oxidation of toluene.
Show more [+] Less [-]Microwave-responsive SiC foam@zeolite core-shell structured catalyst for catalytic pyrolysis of plastics
2022
Chen, Zhaohui | Monzavi, Mohammad | Latifi, Mohammad | Samih, Said | Chaouki, J.
Catalytic pyrolysis is a promising chemical recycling technology to supplement mechanical recycling since plastics can be broken down into monomers or converted to the required fuels and chemicals. In this study, a microwave (MW) -responsive SiC foam@zeoltie core-shell structured catalyst was proposed for the catalytic pyrolysis of polyolefins. Under microwave irradiation, the SiC foam core works as both microwave adsorber and catalyst support, thus concentrating the generated heat energy on the ZSM-5 zeolite shell, where the catalytic reaction takes place. SiC foam with an open cellular structure can also improve the global transport of mass and heat during plastics pyrolysis. In this work, the effects of the SiO₂/Al₂O₃ ratio and alkaline treatment of ZSM-5 zeolite coated SiC foam under MW irradiation on the variations in product distribution from low-density polyethylene (LDPE) pyrolysis were investigated at 450 °C. The results indicated that the appropriate acidity and pore structure were crucial to upgrading gas and liquid products. Particularly, the creation of a mesoporous structure in ZSM-5 zeolite via alkaline treatment could improve the diffusion of large molecules and products, thus significantly increasing the selectivity of high-valued light olefins and aromatics while inhibiting the formation of unwanted alkanes, which are expected in the chemical industry. Concretely, the concentration of olefins in gas increased to 51.0 vol% for ZSM-5(50)-0.25AT, and 65.6 vol% for ZSM-5 (50)-0.50AT, compared with 45.2 vol% for the parent ZSM-5(50). The relative concentration of aromatics in liquid decreased from 96.6% for ZSM-5(50) to 75.9% for ZSM-5(50)-0.25AT, and 71.1% for ZSM-5(50)-0.50AT. Given the respective yield of gas and liquid, the total selectivity of C2–C4 olefins and aromatics for mesoporous ZSM-5 zeolites could reach 58.6–64.9% during LDPE pyrolysis, which were higher than that for the parent ZSM-5 zeolite.
Show more [+] Less [-]Spatiotemporal assessment of the environmental quality of bottom waters through the study of benthic foraminifera in a semi-enclosed gulf
2022
Prandekou, Amalia | Geraga, Maria | Kaberi, Helen | Sergiou, Spyros | Christodoulou, Dimitris | Ferentinos, George | Koutsikopoulos, Constantin | Papatheodorou, George
The evolution of the bottom water in Amvrakikos Gulf in Ionian Sea at western Greece for a 50-year timespan was assessed by benthic foraminifera assemblages. The degradation of the bottom water of Amvrakikos has been a catalyst for the surface water degradation. The east basin has shown permanent low environmental quality in bottom waters since 1980, while the west basin has been under seasonal hypoxic regime since 2000. The most adverse environmental conditions occurred in 1990–2000 and 2005–2010 coinciding with the recorded fish mortality events. The major cause of the environmental quality improvement of the bottom water is the intrusion of seawater. In western areas of the gulf, where the influence of the seawater is high, the decreased temperature improves the environmental conditions, while in the areas influenced by river discharges (east and northern), the environmental conditions are depended on multiple causes like organic matter input and surface salinity.
Show more [+] Less [-]Modeling and multi-objective optimization of commercial ethylene oxide reactor to strike a delicate balance between profit and negative environmental impact
2022
Lahiri, Sandip Kumar | Chowdhury, Somnath | Hens, Abhiram | Ghanta, Kartik Chandra
The present work emphasizes the development of a generic methodology that addresses the core issue of any running chemical plant, i.e., how to maintain a delicate balance between profit and environmental impact. Here, ethylene oxide (EO) production plant has been taken as a case study. The production of EO takes place in a multiphase catalytic reactor, the reliable first principle-based model of which is still not available in the literature. Artificial neural network (ANN) was therefore applied to develop a data-driven model of the complex reactor with the help of actual industrial data. The model successfully built up a correlation between the catalyst selectivity and other operational parameters. This model was used to establish two objective functions, profit and environmental impact. In this paper, the negative environmental impact has been designated by Eco-indicator 99, which considers all the negative health and environmental impacts of a certain product. A recently developed metaheuristic optimization technique, namely multi-objective firefly (MOF) algorithm, was used to develop Pareto diagram of profit vs. Eco-99. The Pareto diagram will help the plant engineers to make strategy on what operating conditions to be maintained to make a delicate balance between profit and environmental impact. It was also found that by applying this modeling and optimization technique, for a 130 kTA EO plant, approximately 7048 t/year of carbon dioxide can be saved from emission into the atmosphere.
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