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Polyethylenimine-grafted nitrogen-doping magnetic biochar for efficient Cr(VI) decontamination: Insights into synthesis and adsorption mechanisms
2022
Qu, Jianhua | Zhang, Xiubo | Bi, Fuxuan | Wang, Siqi | Zhang, Xinmiao | Tao, Yue | Wang, Yifan | Zhao, Jiang | Zhang, Ying
Herein, polyethylenimine (PEI)-grafted nitrogen (N)-doping magnetic biochar (PEIMW@MNBCBM) was synthesized, and characterization results showed that the microwave-assisted PEI grafting and ball milling-assisted N doping introduced abundant amino, pyridine N and pyrrole N structures onto biochar, which possessed high affinity to Cr(VI) in the anion form. The as-prepared PEIMW@MNBCBM displayed pH-dependence adsorption performance and high tolerance to co-existing ions with maximum uptake capacity of Cr(VI) identified as 183.02 mg/g. Furthermore, PEIMW@MNBCBM could bind Cr(VI) through electrostatic attraction, complexion, precipitation, reduction and pore filling. Especially, effective reduction of Cr(VI) was ascribed to cooperative electron transfer of partial oxygen-containing functional groups, intramolecular pyridine/pyrrole N, protonated amino and Fe²⁺ on the adsorbent, while oxygen-containing and amino functional groups from N-doping biochar and PEI synergistically complexed Cr(III) via providing lone pair electrons to form coordinate bonds. Furthermore, the stable precipitation was formed between Fe³⁺ and Cr(III). Additionally, the Cr(VI) elimination efficiency could maintain 95.83% even after four adsorption-desorption cycles, suggesting PEIMW@MNBCBM as a high-performance adsorbent for Cr(VI) contaminated water remediation.
Show more [+] Less [-]Biochar composite derived from cellulase hydrolysis apple branch for quinolone antibiotics enhanced removal: Precursor pyrolysis performance, functional group introduction and adsorption mechanisms
2022
Zou, Mengyuan | Tian, Weijun | Chu, Meile | Gao, Huizi | Zhang, Dantong
In this study, magnetic biochar (MAB) and humic acid (HA)-coated magnetic biochar produced from apple branches without and after cellulase hydrolysis (HMAB and CHMAB, respectively) were prepared and tested as adsorbents of enrofloxacin (ENR) and moxifloxacin (MFX) in aqueous solution. Compared with MAB and HMAB, novel adsorbent CHMAB possessed a superior mesoporous structure, greater graphitization degree and abundant functional groups. When antibiotic solutions ranged from 2 to 20 mg L⁻¹, the theoretical maximum adsorption capacities of CHMAB for ENR and MFX were 48.3 and 61.5 mg g⁻¹ at 35 °C with adsorbent dosage of 0.4 g L⁻¹, respectively, while those of MAB and HMAB were 39.6 and 54.4 mg g⁻¹, and 44.7 and 59.0 mg g⁻¹, respectively. The pseudo-second-order kinetic model and Langmuir model presented a better fitting to the spontaneous and endothermic adsorption process. The maximum adsorption capacity of ENR and MFX onto CHMAB was achieved at initial pH values of 5 and 8, respectively. Additionally, the adsorption capacity of ENR and MFX decreased with increasing concentrations of K⁺ and Ca²⁺ (0.02–0.1 mol L⁻¹). Synergism between the pore-filling effect, π-π electron-donor-acceptor interactions, regular and negative charge-assisted H-bonding, surface complexation, electrostatic interactions and hydrophobic interactions may dominate the adsorption process. This study demonstrated that a novel magnetic biochar composite prepared through pyrolysis of agricultural waste lignocellulose hydrolyzed by cellulase in combination with HA coating was a promising adsorbent for eliminating quinolone antibiotics from aqueous media.
Show more [+] Less [-]Speciation and release risk of heavy metals bonded on simulated naturally-aged microplastics prepared from artificially broken macroplastics
2022
Chen, Gaobin | Fu, Qianmin | Tan, Xiaofei | Yang, Hailan | Luo, Yang | Shen, Maocai | Ku, Yenlin
The negative impact of microplastics (MPs) act as metals vectors to environment and ecosystem have been paid more and more attention, and the accumulation risk of them to human body through the food chains and food webs needs to attract attention. In addition, the MPs bonded with heavy metals transport from river into the sea with high salinity may also have metals release risk. Herein, natural aged microplastics prepared from artificially broken macroplastics adsorbed with heavy metals accumulated from the natural environment were tested for their states and release risk in several simulated solution (NaCl and gastrointestinal solutions) to understand their effects on environment and human health. The adsorption capacity of different heavy metals on MPs was different during natural aging process proved by four-acid digestion method. Metals with high accumulation (including Pb, As, Cr, Mn, Ni, Zn, Co, Cu and Cd) on NAMPs were selected for further study. Results obtained via three-step extraction method showed that these heavy metals were mainly present as acid-extractable and reducible ions, which were characterized by high bioavailability. Release experiments suggested the notable Mn, Zn, As, Cr, Cu and Ni release in NaCl solution, and significant release of Mn, Zn, As, Cr, Cu, Pb and Ni in gastrointestinal solutions. The high metal release ratio in the simulated gastric solution was attributed to the weak binding of metal ions to NAMPs in acidic environment. This study will play a vital rule in assessing the ecological risks associated with MPs in natural environment.
Show more [+] Less [-]Iron-doped hydroxyapatite for the simultaneous remediation of lead-, cadmium- and arsenic-co-contaminated soil
2022
Yang, Zhihui | Gong, Hangyuan | He, Fangshu | Repo, Eveliina | Yang, Weichun | Liao, Qi | Zhao, Feiping
Since lead, cadmium and arsenic have completely opposite chemical behaviors, it is very difficult to stabilize all these three heavy metals simultaneously. Herein, a novel iron-doped hydroxyapatite composite (Fe-HAP) was developed via an ultrasonic-assisted microwave hydrothermal method for the simultaneous remediation of lead-, cadmium-, and arsenic-co-contaminated soil in Hunan Province, South China. Using DTPA/sodium bicarbonate extractant to extract bioavailable Pb, Cd and As in soil after Fe-HAP remediation for 60 days, the immobilization efficiencies were 79.77%, 51.3% and 37.5% for Pb, Cd and As, respectively. The soil extractable and exchangeable fractions of Pb, Cd and As decreased significantly. In batch experiments, the adsorption kinetics of Pb, Cd and As on Fe-HAP were well described by pseudo-second-order models, indicating that the adsorption is controlled by chemisorption. In the Langmuir adsorption isotherm, the maximum adsorption capacities of Cd²⁺ and As(V) were 476.2 mg g⁻¹ and 195.69 mg g⁻¹, respectively, while Pb²⁺ fit the Freundlich model better. The XRD, SEM and XPS analyses indicated that Fe-HAP formed stable minerals of Pb₅(PO₄)₃OH, Cd₃(PO₄)₂·4H₂O, Cd(OH)₂ and Fe₃(AsO₄)₂·6H₂O with Pb, Cd and As. Overall, its facile and efficient immobilization performance indicate that Fe-HAP has potential for practical applications in integrative remediation of Pb-, Cd-, and As- co-contaminated soil.
Show more [+] Less [-]Solidification/stabilization of soil heavy metals by alkaline industrial wastes: A critical review
2022
Jiang, Qi | He, Yongmei | Wu, Yonglin | Dian, Bo | Zhang, Jilai | Li, Tianguo | Jiang, Ming
Solidification/stabilization technology is one of the most desirable technologies for the remediation of heavy metal contaminated soils due to its convenience and effectiveness. The annual production of alkaline industrial wastes in China is in the hundreds of millions of tons. Alkaline industrial wastes have the potential to replace conventional stabilizers because of their cost effectiveness and performance in stabilizing heavy metals in soils. This paper systematically summarizes the use of four alkaline industrial wastes (soda residue, steel slag, carbide slag, and red mud) for the solidification/stabilization of heavy metal contaminated soils and provides a comprehensive analysis of the three mechanisms of action (hydration, precipitation, and adsorption) and factors that influence the process. In addition, the environmental risks associated with the use of alkaline industrial wastes are highlighted. We found that soda residues, steel slag and carbide slag are appropriate for solidification/stabilization of Pb, Cd, Zn and Cu, while red mud is a potential passivation agent for the stabilization of As in soils. However, implementation of remediation methods using alkaline industrial wastes has been limited because the long-term effectiveness, synergistic effects, and usage in soils containing multiple heavy metals have not been thoroughly studied. This review provides the latest knowledge on the mechanisms, risks, and challenges of using alkaline industrial wastes for solidification/stabilization of heavy metal contaminated soils.
Show more [+] Less [-]Insights into the effects of salinity on the sorption and desorption of legacy and emerging per-and polyfluoroalkyl substances (PFASs) on marine sediments
2022
Yin, Chao | Pan, Chang-Gui | Xiao, Shao-Ke | Wu, Qi | Tan, Hong-Ming | Yu, Kefu
Per-and polyfluoroalkyl substances (PFASs) have attracted extensive attention since this century due to their wide distribution, persistence, bioaccumulation/biomagnification potential, and (eco)toxicity. In the present study, we investigated the sorption kinetics, sorption isotherms and desorption behaviors of legacy and emerging PFASs with different chain lengths and functional end groups onto marine sediments at four different salinities (0, 10, 20, and 30 practical salinity units (psu)). Results revealed that the sorption of PFASs onto sediment can be well described by the pseudo-second-order kinetic model. PFASs sorption was influenced by both compound-specific and solution-specific parameters. The distribution coefficient (Kd) for PFASs were increased with the increase of perfluorocarbon chain length and salinity, suggesting that hydrophobic and electrostatic interactions were involved in the adsorption process. 6:2 FTSA showed the lowest adsorption among PFASs with eight carbon atoms (6:2 FTSA, PFOA and PFOS). The increase of perfluorocarbon chain length of PFASs and salinity would result in the decrease of desorption rate of PFASs from sediment. In addition, PFCAs were desorbed more easily from the sediment than the PFSAs with the same perfluorocarbon chain length at all salinity groups. The present study demonstrated that salinity can apparently influence the fate of PFASs in aquatic environment and provided valuable data for modeling the fate of PFASs in real environment.
Show more [+] Less [-]Enhanced propagation of intracellular and extracellular antibiotic resistance genes in municipal wastewater by microplastics
2022
Cheng, Yuan | Lu, Jiarui | Fu, Shusen | Wang, Shangjie | Senehi, Naomi | Yuan, Qingbin
Microplastics (MPs) are an emerging global concern as they are abundant in the environment and can act as vectors of various contaminants. However, whether and how MPs can be vectors of antibiotic resistance genes (ARGs), especially extracellular ARGs (eARGs), remains far from explicit. This study addresses the adsorption of both intracellular ARGs (iARGs) and eARGs by four types of MPs in municipal wastewater, and then explores the potential horizontal gene transfer of iARGs and eARGs exposed to MPs. Results indicate that though MPs significantly adsorbed both iARGs and eARGs, eARGs were adsorbed with a significantly higher fold enrichment (2.0–5.0 log versus 2.0–3.3 log) and rate (0.0056 min⁻¹ versus 0.0037 min⁻¹) than iARGs. While all four types of MPs adsorbed ARGs, polypropylene MPs showed the highest adsorption capacity for ARGs. Background constituents such as humic acid and antibiotics significantly inhibited adsorption of iARGs, but not eARGs on MPs. The presence of sodium chloride didn't significantly affect adsorption of iARGs or eARGs. The adsorption of ARGs was well explained by the extended Derjaguin–Landau–Verwey–Overbeek (XDLVO) interaction energy profile. Higher eARG adsorption was attributed to a lower energy barrier between MPs and eARGs than that between MPs and iARGs. Exposure to MPs enhanced horizontal gene transfer of both iARGs and eARGs by 1.5 and 2.0 times, respectively. The improved contact potential between donors and recipients, as well as the increased cell permeability of recipients induced the improved horizontal gene transfer by MPs. This study underscores the need to address ARG propagation through adsorption to MPs.
Show more [+] Less [-]A state-of-the-art review on capture and separation of hazardous hydrogen sulfide (H2S): Recent advances, challenges and outlook
2022
Chan, Yi Herng | Lock, Serene Sow Mun | Wong, Mee Kee | Yiin, Chung Loong | Loy, Adrian Chun Minh | Cheah, Kin Wai | Chai, Slyvester Yew Wang | Li, Claudia | How, Bing Shen | Chin, Bridgid Lai Fui | Chan, Zhe Phak | Lam, Su Shiung
Hydrogen sulfide (H₂S) is a flammable, corrosive and lethal gas even at low concentrations (ppm levels). Hence, the capture and removal of H₂S from various emitting sources (such as oil and gas processing facilities, natural emissions, sewage treatment plants, landfills and other industrial plants) is necessary to prevent and mitigate its adverse effects on human (causing respiratory failure and asphyxiation), environment (creating highly flammable and explosive environment), and facilities (resulting in corrosion of industrial equipment and pipelines). In this review, the state-of-the-art technologies for H₂S capture and removal are reviewed and discussed. In particular, the recent technologies for H₂S removal such as membrane, adsorption, absorption and membrane contactor are extensively reviewed. To date, adsorption using metal oxide-based sorbents is by far the most established technology in commercial scale for the fine removal of H₂S, while solvent absorption is also industrially matured for bulk removal of CO₂ and H₂S simultaneously. In addition, the strengths, limitations, technological gaps and way forward for each technology are also outlined. Furthermore, the comparison of established carbon capture technologies in simultaneous and selective removal of H₂S–CO₂ is also comprehensively discussed and presented. It was found that the existing carbon capture technologies are not adequate for the selective removal of H₂S from CO₂ due to their similar characteristics, and thus extensive research is still needed in this area.
Show more [+] Less [-]Alkylation modified pistachio shell-based biochar to promote the adsorption of VOCs in high humidity environment
2022
Cheng, Tangying | Li, Jinjin | Ma, Xiuwei | Zhou, Lei | Wu, Hao | Yang, Linjun
The objective of this work was to evaluate the adsorption capacity of alkylated modified porous biochar prepared by esterification and etherification (PSAC-2) for low concentrate volatile organic compounds (VOCs, toluene and ethyl acetate) in high humidity environment by experiments and theoretical calculations. Results showed that PSAC-2 has a large specific surface area and weak surface polarity, at 80% relative humidity, its capacities for toluene and ethyl acetate adsorption could be maintained at 92% and 87% of the initial capacities (169.9 mg/g and 96.77 mg/g). The adsorption behaviors of toluene, ethyl acetate, and water vapor were studied by adsorption isotherms, and isosteric heat was obtained. The desorption activation energy was obtained by temperature programmed desorption experiment. The outcomes manifested that the PSAC-2 can achieve strong adsorption performance for weakly polar molecules. Through density functional theory (DFT) simulations, owing to the interaction of hydrogen bonds, oxygen-containing groups became a significant factor influencing the adsorption of VOCs in humid environments. These results could provide an important reference for VOCs control in a high humidity environment.
Show more [+] Less [-]Poly-NIPAM/Fe3O4/multiwalled carbon nanotube nanocomposites for kerosene removal from water
2022
Abdullah, Thamer Adnan | Juzsakova, Tatjána | Le, Phuoc-Cuong | Kułacz, Karol | Salman, Ali D. | Rasheed, Rashed T. | Mallah, Muhammad Ali | Varga, Béla | Mansoor, Hadeel | Mako, Eva | Zsirka, Balázs | Nadda, Ashok Kumar | Nguyen, X Cuong | Nguyen, D Duc
Multiwalled carbon nanotubes (MWCNTs) were oxidized using a mixture of H₂SO₄ and HNO₃, and the oxidized MWCNTS were decorated with magnetite (Fe₃O₄). Finally, poly-N-isopropyl acrylamide-co-butyl acrylate (P-NIPAM) was added to obtain P-NIPAM/Fe/MWCNT nanocomposites. The nanosorbents were characterized by various techniques, including X-ray diffraction, transmission electron microscopy, scanning electron microscopy, thermogravimetric analysis, and Brunauer–Emmett–Teller analysis. The P-NIPAM/Fe/MWCNT nanocomposites exhibited increased surface hydrophobicity. Owing to their higher adsorption capacity, their kerosene removal efficiency was 95%; by contrast, the as-prepared, oxidized, and magnetite-decorated MWCNTs had removal efficiencies of 45%, 55%, and 68%, respectively. The P-NIPAM/Fe/MWCNT nanocomposites exhibited a sorbent capacity of 8.1 g/g for kerosene removal from water. The highest kerosene removal efficiency from water was obtained at a process time of 45 min, sorbent dose of 0.005 g, solution temperature of 40 °C, and pH 3.5. The P-NIPAM/Fe/MWCNTs showed excellent stability after four cycles of kerosene removal from water followed by regeneration. The reason may be the increase in the positive charge of the polymer at pH 3.5 and the increased adsorption affinity of the adsorbent toward the kerosene contaminant. The pseudo second-order model was found to be the most suitable model for studying the kinetics of the adsorption reaction.
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