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1.
J Colloid Interface Sci ; 659: 1015-1028, 2024 Apr.
Article in English | MEDLINE | ID: mdl-38241973

ABSTRACT

In this study, we prepared a micron zero-valent iron/N-doped graphene-like biochar (mZVI/NGB) composite using a mechanochemical method for tetracycline (TC) degradation through O2 activation. The mZVI and NGB components formed a strong coupling catalytic system, with mZVI acting as an electron pool and NGB as a catalyst for H2O2 generation. Under circumneutral pH (5.0-6.8), the mZVI/NGB composite exhibited exceptional TC removal efficiency, reaching nearly 100 % under optimal conditions. It also showed good tolerance to co-existing anions, such as Cl-, SO42-, and humic acid. Further studies found that the TC degradation mechanism was mainly ascribed to the non-radical pathway (1O2 and electron transfer), and the Fe2+/Fe3+ redox cycle on the composite's surface also played a crucial role in maintaining catalytic activity. This research contributes to the development of advanced materials for sustainable and effective water treatment, addressing pharmaceutical pollutant contamination in water sources.


Subject(s)
Charcoal , Graphite , Water Pollutants, Chemical , Iron/chemistry , Hydrogen Peroxide , Anti-Bacterial Agents , Tetracycline/chemistry , Water Pollutants, Chemical/chemistry
2.
Chemosphere ; 350: 141034, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38147926

ABSTRACT

The removal of Cr(VI) from aqueous solutions using microscale zerovalent iron (mZVI) shows promising potential. However, the surface passivation of mZVI particles hinders its widespread application. In this study, we prepared tannic acid (TA) modified mZVI composite (TA-mZVI) by a simple sonication method. The introduction of TA allowing TA-mZVI composite to adsorb Cr(VI) rapidly under electrostatic forces attraction, guarantying TA-mZVI exhibited remarkable Cr(VI) removal capacity with a maximum adsorption capacity of 106.1 mg⋅g-1. At an initial pH of 3, it achieved a rapid removal efficiency of 96.2% within just 5 min, which was 7.7 times higher than that of mZVI. Various characterizations, including XPS and CV analysis, indicated that the formation of TA-Fe complexes accelerates electron transfer. In addition, TA endows functional groups to TA-mZVI, raising the dispersion and stability and serves as a protective layer hindering passivation. Further mechanistic analysis revealed that Cr(VI) removal by TA-mZVI followed an adsorption-reduction-precipitation mechanism, with TA mitigating the surface passivation of mZVI and facilitating the reduction of most Cr(VI) to Cr(III). Batch cyclic experiments revealed that TA-mZVI exhibited satisfactory performance, maintaining over 85% Cr(VI) removal even after five cycles and minimally affected by various coexisting ions. With notable advantages in cost-effectiveness, ease-synthesis and recovery, this work provides a great promise for developing efficient reactive adsorbent for addressing Cr(VI) contamination in aqueous solutions.


Subject(s)
Iron , Polyphenols , Water Pollutants, Chemical , Iron/chemistry , Water Pollutants, Chemical/analysis , Chromium/chemistry , Adsorption , Water
3.
J Hazard Mater ; 446: 130657, 2023 Mar 15.
Article in English | MEDLINE | ID: mdl-36580785

ABSTRACT

Atomic hydrogen (H*) has long been thought to play an important role in the dechlorination of trichloroethylene (TCE) by carbon-supported zero-valent iron (ZVI), which offers an alternative pathway for TCE dechlorination. Herein, we demonstrate that the reductive dechlorination of TCE by sulfidated microscale ZVI (S-mZVI) can be further enhanced by promoting the formation of H* through the introduction of reduced graphene oxide (rGO). The completely degradation of 10 mg/L TCE can be achieved by S-mZVI/rGO within 24 h, which was 3.3 times faster than that of S-mZVI. The change in the distribution of TCE degradation products over time suggests that the introduction of rGO leads to a change in the dechlorination pathway. The percentage of ethane in the final products of TCE degradation by S-mZVI/rGO was 34.3 %, while that of S-mZVI was only 21.9 %. The electrochemical tests confirmed the occurrence of hydrogen spillover in the S-mZVI/rGO composite, which promoted the reductive dechlorination of TCE by H*. Although the S-mZVI/rGO composite had stronger hydrogen evolution propensity than S-mZVI, the S-mZVI/rGO composite still exhibited higher electron utilization efficiency than S-mZVI thanks to the increased utilization of hydrogen.

4.
Sci Total Environ ; 814: 152745, 2022 Mar 25.
Article in English | MEDLINE | ID: mdl-34979230

ABSTRACT

As a member of chlorophenolic compounds, 2-chlorohydroquinone (H2QCl) has been widely used as intermediates in various chemical industries and leaded to serious threat on the environment. It is urgent to develop simple and robust analytical method for sensitive and selective determination of H2QCl. Carbon quantum dots (CQDs), a promising photoluminescence nanomaterial, have gained sufficient concern as optical sensors owing to their outstanding photochemical properties. In this work, nitrogen doped carbon quantum dots (N-CQDs) were successfully synthesized by a simple secondary hydrothermal method and applied as a fluorescent probe for the quantitation of H2QCl. A new fluorescence region centered at excitation wavelength of 310 nm and emission wavelength of 390 nm appeared after nitrogen doping. It was found that the N-CQDs exhibited a high selectivity towards H2QCl with sensitive fluorescence response and the fluorescence quenching of N-CQDs was linear with the concentration of H2QCl in the range of 30-90 µM (Y = 0.0049X + 0.1255, R2 = 0.996). This is the first time that the dual role of excitation light was observed in the fluorescence detection system. The ultraviolet light acted as not only the excitation energy source for N-CQDs photoluminescence, but also the light source for photolysis of H2QCl. In the detection process, H2QCl was degraded to p-benzoquinone by light, and then the CQDs combined with p-benzoquinone through Michael addition reaction under the action of doped nitrogen. The electron transfer from N-CQDs to the linked p-benzoquinone caused the quenching of fluorescence originated from the edge state of N-CQDs. Furthermore, this established method can be applied for the quantitative determination of H2QCl in environmental water samples with satisfactory recoveries between 94.31 and 105.51%.


Subject(s)
Quantum Dots , Carbon , Fluorescent Dyes , Nitrogen , Photolysis
5.
J Hazard Mater ; 425: 128057, 2022 03 05.
Article in English | MEDLINE | ID: mdl-34910998

ABSTRACT

Carboxymethyl cellulose (CMC) has been widely adopted as stabilizer to enhance the subsurface mobility of nanoscale zerovalent iron (nZVI). However, CMC surface modification also cause severe decrease of the longevity and electron utilization efficiency (εe) of nZVI, which is still not well understood. In this study, we demonstrate the negative influence of CMC on the properties of sulfidated nZVI (S-nZVI) could be reversed by increasing the degree of substitution (D.S.) of CMC. Consistent with previous study, the sample CMC-S-nZVI prepared with commercial CMC with degree of substitution (D.S.) of 0.75 exhibited a considerable low longevity of 33 days with εe of 4.5%, much lower than that of sulfidated nZVI (S-nZVI, 113 days and 13%). In sharp contrast, the sample HCMC-S-nZVI synthesized with CMC with super high D.S. of 1.76 demonstrated significantly enhanced longevity of 139 days and εe of 20%. The enhancement was attributed to compatible molecular structure of CMC with super high D.S. Moreover, the HCMC-S-nZVI also exhibited higher mobility in porous media than CMC-S-nZVI. Our work provides a feasible way to prepare S-nZVI with desired properties including high subsurface transportability, high longevity and high εe.


Subject(s)
Carboxymethylcellulose Sodium , Metal Nanoparticles , Electrons , Iron , Porosity
6.
Sci Rep ; 11(1): 21414, 2021 Nov 01.
Article in English | MEDLINE | ID: mdl-34725381

ABSTRACT

It's highly desired but challenging to synthesize self-supporting nanohybrid made of conductive nanoparticles with metal organic framework (MOF) materials for the application in the electrochemical field. In this work, we report the preparation of Ni2P embedded Ni-MOF nanosheets supported on nickel foam through partial phosphidation (Ni2P@Ni-MOF/NF). The self-supporting Ni2P@Ni-MOF/NF was directly tested as electrode for urea electrolysis. When served as anode for urea oxidation reaction (UOR), it only demands 1.41 V (vs RHE) to deliver a current of 100 mA cm-2. And the overpotential of Ni2P@Ni-MOF/NF to reach 10 mA cm-2 for hydrogen evolution reaction HER was only 66 mV, remarkably lower than Ni2P/NF (133 mV). The exceptional electrochemical performance was attributed to the unique structure of Ni2P@Ni-MOF and the well exposed surface of Ni2P. Furthermore, the Ni2P@Ni-MOF/NF demonstrated outstanding longevity for both HER and UOR. The electrolyzer constructed with Ni2P@Ni-MOF/NF as bifunctional electrode can attain a current density of 100 mA cm-2 at a cell voltage as low as 1.65 V. Our work provides new insights for prepare MOF based nanohydrid for electrochemical application.

7.
RSC Adv ; 11(20): 12086-12094, 2021 Mar 23.
Article in English | MEDLINE | ID: mdl-35423729

ABSTRACT

In the present study, to develop the application of biostimulation for the in situ remediation of trichloroethylene (TCE) in contaminated groundwater/soil, a mixed culture containing Dehalococcoides spp. was employed to investigate the biological effects of the polarized mineral tourmaline on the dechlorination performance, community structure, cell proliferation and expression of two model gene (tceA and vcrA) coding for reductive dehalogenases (Rdase). It was observed that tourmaline could speed up the biological dechlorination of TCE by promoting the growth and metabolism of the bacteria, impacting the expression of RDase genes. Compared with the bacteria system, the time for the complete removal of TCE was reduced from 7 d to 4 d when 5 g L-1 tourmaline was added to the bacterial system, and the yield of the innocuous product ethene increased from 53% to 91% on the 15th day of reaction. At this time, the community similarity of the tourmaline-added bacteria system and the bacteria system was 83.1%. The Dehalococcoides spp. in the tourmaline system grew 2 times more than that in the bacteria system. Moreover, an increase in the expression levels and decrease in the relative expression ratios of the functional genes (tceA and vcrA) were observed with the addition of tourmaline. The above analysis provides a molecular basis for the investigation of the biostimulation process by minerals.

8.
R Soc Open Sci ; 5(6): 172242, 2018 Jun.
Article in English | MEDLINE | ID: mdl-30110440

ABSTRACT

A method developed based on the capillary effect and capillary condensation theory was used to synthesize an innovative Fe/C/Pd composite in this study. This composite (Fe@CNTs@Pd) consists of carbon nanotubes (CNTs) with nanoscale zerovalent iron (NZVI) on the inner surface and palladium nanoparticles supported on the outer surface of CNTs. This structure successfully addresses the problems of high iron corrosion rate and lower utilization rate of hydrogen in the application of bimetal nanoparticles for trichloroethylene (TCE) removal. TCE degradation experiments and electrochemical tests were conducted to investigate the material properties and reaction mechanisms of the composite. It is found that the prepared composite material contribute a high level of TCE dechlorination rate and substantially reduced hydrogen production during iron corrosion in water compared with the conventional CNTs-supported bimetal materials (Fe/Pd@CNTs). Hydrogen spillover effect helps the reactivity of Fe@CNTs@Pd for TCE degradation and suppressed the galvanic cell effect, which results in a stronger resistance to corrosion. Although the Kobs of Fe@CNTs@Pd was 16.87% lower than that of Fe/Pd@CNTs, the hydrogen production rate of Fe@CNTs@Pd was 10 times slower than that of Fe/Pd@CNTs. Therefore, Fe@CNTs@Pd shows a significant reduction in the corrosion rate at a cost of slightly slower degradation of TCE. In sum, the prepared composites demonstrate important characteristics, including alleviating NZVI agglomeration, maintaining high TCE removal efficiency and reducing the corrosion of NZVI.

9.
Chemosphere ; 194: 9-19, 2018 Mar.
Article in English | MEDLINE | ID: mdl-29195092

ABSTRACT

Dehalococcoides spp. were extensively studied and applied to in-situ trichloroethylene (TCE) remediation since it is the only genus that can reduce TCE to harmless ethene completely. However, this technology was hindered because of the requirement of electron donor (i.e. hydrogen or fermentable organic substrate). Considering the spontaneous electric field and in-situ hydrogen production capacity of tourmaline, this mineral was used as an environmental-friendly bio-promoter for dechlorinating mixed culture containing Dehalococcoides spp. in this work. Research results showed that biodegradation of TCE and the intermediates were both significantly improved by tourmaline. The first-order TCE degradation rate coefficient increased from 0.0125 h-1 for the tourmaline-free system to 0.0306 h-1 for the system combined with 5 g L-1 tourmaline, and ethene production increased by 36%. The outstanding TCE-degrading ability in the tourmaline-bacteria system without the addition of fermentative electron donor (i.e. methanol) indicated that tourmaline could also produce electron donor to support dechlorinating bacteria. Tourmaline could have direct electric biostimulatory effect and indirect enhanced effect associated with water-derived H2 production in the electric field of tourmaline. Meanwhile, PCR-DGGE analysis exhibited that tourmaline could accelerate the succession of a bacterial, dechlorinating community. The distinctive effects of tourmaline on bacteria were related to its stable electric properties. Therefore, tourmaline could be continuously used in the bioremediation. The present study provided a safe, convenient and persistent alternative to the commonly used enhancement approaches for anaerobic reductive dechlorination process.


Subject(s)
Biodegradation, Environmental/drug effects , Chloroflexi/metabolism , Trichloroethylene/metabolism , Ethylenes , Fermentation , Halogenation , Hydrogen/chemistry , Kinetics , Trichloroethylene/chemistry
10.
J Anal Methods Chem ; 2013: 649503, 2013.
Article in English | MEDLINE | ID: mdl-24455425

ABSTRACT

Core-shell silica-coated Fe(0) nanoparticles (Fe@SiO2) were prepared in one-step synthesis by aqueous reduction combined with modified Stöber method. The as-prepared Fe@SiO2 were then used for simultaneous removal of Cr(VI) and Cd(II) from aqueous solution. Batch tests indicated that Fe@SiO2 exhibited high removal capacity toward Cr(VI) and Cd(II). Cr(VI) was removed by Fe@SiO2 through reduction rather than adsorption, while Cd(II) removal was mainly through adsorption. The removal rate increased with increasing initial Fe NPs dose and decreased with increasing initial Cr(VI) and Cd(II) concentrations. Cd(II) adsorption was also strengthened by Cr(VI) reduction with the release of OH(-). The removals of Cr(VI) and Cd(II) were weakened in the presence of cations or humic acid, as a result of aggregation and less active site of Fe@SiO2. Overall, the simply prepared Fe@SiO2 were potential material for the heavy metals removed from water.

11.
Environ Technol ; 33(16-18): 2185-92, 2012 Sep.
Article in English | MEDLINE | ID: mdl-23240214

ABSTRACT

Bimetallic Fe/Ni nanoparticles were synthesized and their nitrate reduction capacity was studied. Nitrate (354 mg L(-1), equal to 5.71 mmol L(-1)) reduction was performed using Fe/Ni nanoparticles with various Ni contents (1.0, 5.0, 10 and 20%) in an unbuffered condition. Optimum nitrate reduction rate (1.03 +/- 0.087 x 10(-4) mol x min(-1) x greduc(-1)) was obtained with 5.0% nano-scale Fe/Ni, while only 25% nitrate (1.05 +/- 0.091 x 10(-5) mol x min(-1) x greduc(-1)) was transformed by nano-scale Fe(0) within the same reaction time, which means that these bimetallic nanoparticles are obviously more reactive than monometallic nano-scale Fe(0). For this bimetallic system a near-neutral initial pH (6.5) is more favourable than an acidic condition (2.0 and 4.0). Relatively air-stable nano-scale Fe/Ni particles were developed by slowly aging them for 22 h and exhibited similar reactivity to freshly synthesized nano-scale Fe(0). Although undesirable transformation of nitrate (91.0 +/- 0.37%) to ammonium was observed in this study, Fe/Ni particles showed a much higher nitrate reduction rate and an optimum reduction rate at near-neutral pH, which may have important implications for nitrate-contaminated site remediation.


Subject(s)
Metal Nanoparticles/chemistry , Nitrates/chemistry , Water Pollutants, Chemical/chemistry , Catalysis , Hydrogen-Ion Concentration , Oxidation-Reduction
12.
Sci Total Environ ; 421-422: 260-6, 2012 Apr 01.
Article in English | MEDLINE | ID: mdl-22381028

ABSTRACT

A facile one-step method was developed to fabricate mono-dispersed Fe nanoparticles (Fe NPs) coated with SiO(2) shell by aqueous reduction method combined with modified Stöber method. Borohydride was acted not only as a reductant for iron salt but also as a catalyst for hydrolysis and polycondensation reaction of tetraethylorthosilicate (TEOS), and more importantly, there was no need to use surface primer for the generation of Fe NPs and catalyst NH(4)OH for SiO(2). Both the Fe NPs agglomeration and SiO(2) shell thickness can be controlled through the synthetic conditions. Lower potassium borohydride (KBH(4)) injection speed was preferable to assemble Fe NPs. The SiO(2) shell thickness increased gradually with the increase of TEOS amount. Under the condition of TEOS amount of 0.1mL and KBH(4) injection speed of 5mL/min, 25nm single Fe NP was coated with SiO(2) shell with thickness of about 9nm. The resulting nanoporous SiO(2) shell was proved to allow reactant to reach the Fe NPs while at the same time protect them from aggregation. The reactivity characterization of the SiO(2)-coated Fe nanoparticles (Fe@SiO(2)) showed that both TEOS concentration and KBH(4) injection speed had effect on Cr (VI) degradation ability. The highest removal capacity of Fe@SiO(2) can reach 467mgCr/gFe at an initial Cr (VI) concentration of 70mg/L under pH 6.0±0.1. XPS and TEM results showed that Cr (VI) was converted to nontoxic Cr (III) and the reaction product was completely adsorbed to SiO(2) shell.


Subject(s)
Chemistry Techniques, Synthetic/methods , Chromium/isolation & purification , Environmental Pollutants/isolation & purification , Iron/chemistry , Metal Nanoparticles/chemistry , Silicon Dioxide/chemistry , Chromium/chemistry , Environmental Pollutants/chemistry , Environmental Restoration and Remediation/methods , Microscopy, Electron, Transmission , Oxidation-Reduction , Particle Size , Spectrophotometry, Atomic , Surface Properties , X-Ray Diffraction
13.
J Environ Sci (China) ; 23(7): 1211-8, 2011.
Article in English | MEDLINE | ID: mdl-22125917

ABSTRACT

Effective in situ remediation of Cr(VI) in groundwater requires the successful delivery of reactive iron particles to the subsurface. Fe(0) nanoparticles (20-110 nm diameter) supported on silica fume were synthesized by borohydride reduction of an aqueous iron salt in the presence of a support material. The experimental result showed that attachment of Fe(0) nanoparticles on the commercial available sub-micrometer silica fume prevented them from aggregation while maintaining the particle reactivity. When the Fe(0) concentration was 0.4 g/L, 88.00% of 40 mg/L Cr(VI) was removed by silica fume-supported Fe(0) nanoparticles (SF-Fe(0) in 120 min, 22.55% higher than unsupported Fe(0). Furthermore, transport experiments confirmed that almost all unsupported Fe(0) was retained, whereas 51.50% and 38.29% of SF-Fe(0) were eluted from the vertical and horizontal sand column, respectively. Additionally, the effect of solution ionic strength on the transport ability of SF-Fe(0) was evaluated. The result showed that increase in the salt concentration led to a decrease in the mobility and also the divalent ion Ca2+ had a greater effect than that of monovalent ion Na+.


Subject(s)
Chromium/chemistry , Iron/chemistry , Nanoparticles/chemistry , Silicon Dioxide/chemistry , Soil Pollutants/chemistry , Water Pollutants, Chemical/chemistry , Chromium/isolation & purification , Microscopy, Electron, Transmission , Nanoparticles/ultrastructure , Soil Pollutants/isolation & purification , Water Pollutants, Chemical/isolation & purification
14.
Water Sci Technol ; 63(12): 2781-7, 2011.
Article in English | MEDLINE | ID: mdl-22049699

ABSTRACT

Silica fume supported-Fe(0) nanoparticles (SF-Fe(0)) were prepared using commercial silica fume as a support. The feasibility of using this SF-Fe(0) for reductive immobilization of Cr(VI) was investigated through batch tests. Compared with unsupported Fe(0), SF-Fe(0) was significantly more active in Cr(VI) removal especially in 84 wt% silica fume loading. Silica fume had also been found to inhibit the formation of Fe(III)/Cr(III) precipitation on Fe nanoparticles' surface, which was increasing the deactivation resistance of iron. Cr(VI) was removed through physical adsorption of Cr(VI) onto the SF-Fe(0) surface and subsequent reduction of Cr(VI) to Cr(III). The rate of reduction of Cr(VI) could be expressed by pseudo first-order reaction kinetics. The rate constant increased with the increase in iron loading but decreased with the increase in initial Cr(VI) concentration. Furthermore, column tests showed that the SF-Fe(0) could be readily transported in model soil.


Subject(s)
Chromium/isolation & purification , Fresh Water/chemistry , Iron/chemistry , Silicon Dioxide/chemistry , Soil Pollutants/isolation & purification , Water Pollutants, Chemical/isolation & purification , Environmental Restoration and Remediation/methods , Feasibility Studies , Kinetics , Microscopy, Electron, Scanning , Microscopy, Electron, Transmission , Nanoparticles , Particle Size , Surface Properties
15.
J Environ Qual ; 40(6): 1878-85, 2011.
Article in English | MEDLINE | ID: mdl-22031571

ABSTRACT

Sequestration of organic contaminants in carbonaceous materials can significantly affect contaminant fate and transport. We investigated the reductive dechlorination of granular-activated carbon (GAC)-adsorbed trichloroethylene (TCE) by nanoscale zero-valent iron (nZVI) to understand the effect of sequestration on abiotic reactivity of organic contaminants. Significant reduction of TCE sequestered in GAC micropores was observed, even though direct contact with nZVI was unlikely. Reduction of sequestered TCE by reactive Fe(II) species or molecular hydrogen was ruled out as the reaction mechanisms. We propose that GAC served as the conductor for the transfer of electrons or atomic hydrogen from nZVI to the micropores, wherein adsorbed TCE molecules were reduced. An important implication for environmental remediation is that carbonaceous adsorbents not only function as a superb sink for organic contaminants but also allow them to be slowly degraded while being trapped.


Subject(s)
Carbon/chemistry , Iron/chemistry , Trichloroethylene/chemistry , Electrons , Environmental Pollutants/chemistry , Hydrogen-Ion Concentration
16.
Bioresour Technol ; 101(24): 9825-8, 2010 Dec.
Article in English | MEDLINE | ID: mdl-20727742

ABSTRACT

Bimetallic nanoparticles (nano Fe-Ni, nano Fe-Cu) and coated iron nanoparticles (chitosan-Fe(0), sodium oleate-Fe(0)) were utilized to support autotrophic denitrification. In comparison to nanoscale zero-valent iron (NZVI) particles, Ni-containing nanoparticles resulted in faster nitrate removal, but generated 17% more ammonium. The nano Fe-Cu integrated system, required two days less than the unmodified NZVI integrated system to remove all the nitrate and decrease ammonium by 13%, but a large amount of nitrite remained in the system. Compared to uncoated NZVI particles, chitosan-coated nanoparticles allowed the same nitrate removal time but 23% more ammonium production. The sodium oleate-Fe(0) nanoparticles did not only decrease the generation of ammonium by 17%, but also reduced the toxicity of the nanoparticles to bacteria. Therefore, sodium oleate-Fe(0) nanoparticles may be an appropriate substitute for NZVI particles to support autotrophic denitrification provided that additional time (two days) is allowed for complete nitrate removal.


Subject(s)
Alcaligenes/drug effects , Alcaligenes/metabolism , Denitrification/drug effects , Iron/pharmacology , Metal Nanoparticles/chemistry , Polymers/pharmacology , Autotrophic Processes/drug effects , Chitosan/pharmacology , Copper/pharmacology , Nickel/pharmacology , Nitrates/analysis , Nitrites/analysis , Oleic Acid/pharmacology , Quaternary Ammonium Compounds/analysis , RNA, Bacterial/analysis
17.
J Hazard Mater ; 173(1-3): 724-30, 2010 Jan 15.
Article in English | MEDLINE | ID: mdl-19773119

ABSTRACT

The unstable characteristic of nanoscale zerovalent iron (NZVI) has been a drawback in practical application, despite the expectation of an enhanced reactivity. It has been ever-increasing interests to maintain the NZVI stability in air without significant reactivity sacrifice. This study demonstrated a novel method of coating NZVI particles with poly(methyl methacrylate) (PMMA), which protected the core iron nanoparticles from oxidation in air and enhanced their dispersion stability in organic solvents. The reactivity studies on trichloroethene (TCE) reduction showed that the PMMA coated nanoscale zerovalent iron (PNZVI) particles were capable of effectively reducing TCE. The main roles of PMMA on the dechlorination reactions were confirmed to be sorption enhancement, competitive sorption and corrosion inhibition.


Subject(s)
Environmental Restoration and Remediation/methods , Iron/chemistry , Nanoparticles/chemistry , Polymethyl Methacrylate/chemistry , Trichloroethylene/chemistry , Cetrimonium , Cetrimonium Compounds/chemistry , Emulsions , Indicators and Reagents , Microscopy, Electron, Transmission , Spectroscopy, Fourier Transform Infrared , Surface-Active Agents/chemistry , X-Ray Diffraction
18.
Bioresour Technol ; 101(4): 1141-6, 2010 Feb.
Article in English | MEDLINE | ID: mdl-19819128

ABSTRACT

Nano-scale zero-valent iron particles (NZVI) are increasingly being used to treat sites contaminated with chlorinated solvents. This study investigated the effect of NZVI on dechlorinating microorganisms that participate in the anaerobic bioremediation of such sites. NZVI can have a biostimulatory effect associated with water-derived cathodic H(2) production during its anaerobic corrosion (730+/-30 micromol H(2) was produced in 166 h in abiotic controls with 1 g/L NZVI) or an inhibitory effect upon contact with cell surfaces (assessed by transmission electron microscopy). Methanogens, which are known to compete for H(2) with dechlorinators, were significantly biostimulated by NZVI and methane production increased relative to NZVI-free controls from 58+/-5 to 275+/-2 micromol. In contrast, bacteria dechlorinating TCE were inhibited by NZVI, and the first-order degradation rate coefficient decreased from 0.115+/-0.005 h(-1) (R(2)=0.99) for controls to 0.053+/-0.003 h(-1) (R(2)=0.98) for treatments with 1 g/L NZVI. Ethene production from TCE was initially inhibited by NZVI, but after 331 h increased to levels observed for an NZVI-free system (7.6+/-0.3 micromol ethene produced in 502 h compared to 11.6+/-0.5 mmol in the NZVI-free system and 3.8+/-0.3 micromol ethene for NZVI alone). Apparently, cathodic H(2) was utilized as electron donor by dechlorinating bacteria, which recovered following the partial oxidation and presumably passivation of the NZVI. Overall, these results suggest that reductive treatment of chlorinated solvent sites with NZVI might be enhanced by the concurrent or subsequent participation of bacteria that exploit cathodic depolarization and reductive dechlorination as metabolic niches.


Subject(s)
Bacteria/cytology , Halogenation , Iron/chemistry , Nanoparticles/microbiology , Trichloroethylene/isolation & purification , Bacteria/metabolism , Biodegradation, Environmental , Electrodes , Ethylenes/chemical synthesis , Hydrogen/analysis , Methane/analysis , Nanoparticles/ultrastructure
19.
J Environ Monit ; 12(5): 1153-8, 2010 May.
Article in English | MEDLINE | ID: mdl-21491683

ABSTRACT

A new class of nano-scale Fe0 particles (NZVI) supported on a PAA/PVDF membrane (NZVI-PAA/PVDF) were synthesized and the feasibility of using NZVI-PAA/PVDF for reductive immobilization of Cr(VI) in water was investigated through laboratory batch tests. The results showed that the Cr(VI) removal capacity of NZVI-PAA/PVDF was 181 mg Cr/g Fe at an initial Cr(VI) concentration of 20 mg L(-1) under pH 6.5 +/- 0.1. XPS results showed that Cr(VI) was converted to nontoxic Cr(III). Interfering ions exerted various degrees of impact on NZVI-PAA/PVDF's Cr(VI) removal capacity. Specifically, Ca2+ alone showed the mildest impact while the presence of ions (Mg2+ and HCO3-) exerted the greatest impact. An advantage of NZVI-PAA/PVDF is that the nano-scale Fe0 and resultant particles were combined within a PAA/PVDF membrane, which prevents secondary pollution. Moreover, a piece of PAA/PVDF membrane (4.7 cm diameter) can still support 6.51 mg of nano-scale Fe0 particles after being renewed.


Subject(s)
Chromium/chemistry , Iron/chemistry , Water Pollutants, Chemical/chemistry , Water Purification/methods , Acrylic Resins/chemistry , Metal Nanoparticles/chemistry , Oxidation-Reduction , Polyvinyls/chemistry
20.
Sci Total Environ ; 407(21): 5465-70, 2009 Oct 15.
Article in English | MEDLINE | ID: mdl-19665759

ABSTRACT

An integrated nitrate treatment using nanoscale zero-valent iron (NZVI) and Alcaligenes eutrophus, which is a kind of hydrogenotrophic denitrifying bacteria, was conducted to remove nitrate and decrease ammonium generation. Within 8 days, nitrate was removed completely in the reactors containing NZVI particles plus bacteria while the proportion of ammonium generated was only 33%. That is a lower reduction rate but a smaller proportion of ammonium relative to that in abiotic reactors. It was also found that ammonium generation experienced a biphasic process, involving an increasing period and a stable period. After domestication of the bacteria, the combined NZVI-cell system could remove all nitrate without ammonium released when the refreshed nitrate was introduced. Nitrate reduction and the final product distribution were also studied in batch reactors amended with different initial NZVI contents and biomass concentrations, respectively. Both the nitrate removal rate and the ammonium yield decreased when the initial content of NZVI reduced and the initial biomass concentration increased. However, about 27% of the nitrate was converted to ammonium when excess bacteria (OD(422)=0.026) were used, which was higher than that with appropriate amount of bacteria.


Subject(s)
Alcaligenes/metabolism , Iron/chemistry , Nitrates/metabolism , Quaternary Ammonium Compounds/metabolism , Water Purification/methods , Biomass , Bioreactors
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