SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yan Li,Liangmin Gao,Yu Wang,Shuo Cheng,Guowei Wu,Xuan Yang,Shunli Wan
Biochar-supported metallic oxides are attractive adsorbents for heavy metal cleanup, but the adsorption performance is still unsatisfactory as a result of the self-aggregation of the incorporated metallic oxides. A new hybrid nano-material was prepared through impregnating hydrated ferric oxide (HFO) nanoparticles within biochar bearing high-density charged oxygen-containing groups (e.g., carboxyl and hydroxyl groups) (ABC) derived from HNO 3 treatment. The as-made adsorbent, denoted as HFO-ABC, possesses highly dispersed HFO nanoparticles with typical size lower than 20 nm, and exhibits greater sorption capacity for Cd(II) and Cu(II) than the pristine biochar-supported HFO. It also shows great sorption preference toward Cd(II) and Cu(II) in co-presence of high levels of Ca 2+ , Mg 2+ and humic acid (HA). Such prominent performance is put down to the high-density charged functional groups on the host ABC, which not only promote the dispersion of the immobilized HFO nanoparticles but also generate the potential Donnan membrane effect, i.e., the pre-concentration and permeation of target metals prior to their preferable adsorption by nano-HFO. The predicted effective coefficients of intra-particle diffusion for Cu(II) and Cd(II) are 3.83 × 10 −9 and 4.33 × 10 −9 cm 2 /s, respectively. HFO-ABC exhibits excellent performance for fixed-bed column application, and yields 513 and 990 BV effluents for Cd(II) and Cu(II) to achieve their discharge standards, respectively. The spent HFO-ABC could be in situ regenerated using binary HCl-CaCl 2 solution with desorption efficiency higher than 95%. All results manifest that increasing charged functional groups via HNO 3 treatment is an effective measure for boosting sorption performance of biochar-based nanocomposites.
研究领域:
环境科学
·
材料科学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Shuai Yang,Dongqi Tian,Xinhao Wang,Peng Zhou,Zhaokun Xiong,Heng Zhang,Yang Liu,Gang Yao,Bo Lai
Fenton-like technology has been widely used in the field of water treatment as an advanced oxidation processes (AOPs), and a multitude of non-homogeneous catalysts have been reported effectively to enhance it. Herein, nitrogen and sulfur co-doped nanocarbon materials (NSC) was designed and synthesized, which formed a unique mesoporous structure and abundant functional groups on the surface. It exhibits superior catalytic performance to enhance the Fe(III)/H 2 O 2 system for sulfamethoxazole (SMX) degradation, k obs is 18 times higher than Fe(III)/H 2 O 2 system after the introduction of NSC under the same experimental conditions. Also, the working pH of Fe(III)/H 2 O 2 system was broadened by NSC. Quenching and probe experiments demonstrate that hydroxyl radical (∙OH) was the dominant active species. Both dissociative and surface-bound iron species were observed, which indicates direct reduction and in-situ binding of Fe(III), respectively. Further investigation found nitrogen and sulfur co-doped attribute to the formation of abundant functional groups, the C O bond and C S C bond on the surface of NSC result in the directly reduce of Fe(III), while –COOH contributes to the in-situ binding. The intermediates and possible degradation pathway of SMX degradation were proposed based on the results of liquid chromatography-quadrupole time of flight-mass spectrometer (LC-QTOF-MS). The results of cycling and co-existing ions experiments demonstrate that NSC has outstanding potential for application. This work provides a novel insight into the sustained removal of micropollutants from the aqueous environment based on the nanocarbon materials enhancing the Fenton-like oxidation.
研究领域:
环境科学
·
材料科学
·
化学工程
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DOI
高影响因子
Journal of Materials Chemistry B
·
2014
·Vol. 2
·期 37
·6306-6312
·
IF 0
Fangyuan Gai,Xiang Li,Tianlei Zhou,Xiaogang Zhao,Dongdong Lu,Yunling Liu,Qisheng Huo
This work demonstrates a luminescent chemosensor based on silica cross-linked micellar nanoparticles (SCMNPs) designed by encapsulating a phenothiazine-derived Schiff base, (4E)-4-((10-dodecyl-10H-phenothiazin-7-yl)methyleneamino)-1,2-dihydro-1,5-dimethyl-2-phenylpyrazol-3-one (EDDP), for the selective detection of Fe3+. The encapsulation of EDDP inside SCMNPs (EDDP–SCMNPs) can avoid the metal (Fe3+/Fe2+)-promoted hydrolysis of EDDP and, thus, exhibit highly selective determination of Fe3+. The electron transfer (ET) from EDDP in the core to Fe3+ adsorbed on the shell of EDDP–SCMNPs was verified using UV-vis absorption, fluorescent emission and 3D fluorescence spectra. Moreover, EDDP–SCMNPs showed no sensing ability of Fe2+ due to the weak electron-accepting ability of Fe2+. Significantly, because of their ultrasmall size, nontoxicity, good water solubility and biocompatibility, EDDP-SCMNPs have potential applications in biological systems.
研究领域:
分析化学
·
材料科学
·
生物医学
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DOI
PubMed
Chemical Engineering Journal Advances
·
2021
·
IF 0
Kai Wei,Xiufan Liu,Shiyu Cao,Huijuan Cui,Yu Zhang,Zhihui Ai
In this study, we fabricated a micro-nano structured Fe 2 O 3 @FeB composites by treating commercial Fe 2 O 3 with sodium borohydride. The outside amorphous FeB alloy shell endowed the Fe 2 O 3 @FeB with remarkable Fenton-like performance in organic pollutants oxidation by efficient Fe(III)/Fe(II) cycle. For instance, the pseudo first-order rate constants of RhB degradation using Fe 2 O 3 @FeB as Fenton reagent was 74.6 times that of the Fe 2 O 3 counterpart, the hydroxyl radical generation rate of Fe 2 O 3 @FeB was 1-3 orders of magnitude larger than that of other heterogeneous Fenton reagent. Further mechanistic study unveiled that FeB was oxidized accompanying with Fe(0) and B(0) continuously donated electrons to Fe(III) to secure the efficient generation of surface Fe(II), which could generate additional H 2 O 2 by consecutive single-electron molecular oxygen activation (O 2 →•O 2 − →H 2 O 2 ), leading to enhance •OH production and Fenton-degradation toward typical pollutants. This study provides a facile route for efficient heterogeneous Fenton and strengthens the vital role of molecular oxygen activation on Fenton-like process.
研究领域:
环境科学
·
材料科学
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DOI
Materials Today Energy
·
2017
·
IF 0
Ge Ma,Zhen Chen,Zhihong Chen,Mingliang Jin,Qingguo Meng,Mingzhe Yuan,Xin Wang,Jun-Ming Liu,Guofu Zhou
In this work, we have prepared a series of efficient visible-light-driven WO 3 /Fe(III) nanofiber photocatalysts by electrospinning and impregnation method. The physical and optical properties of the prepared photocatalysts were characterized by field emission scanning electron microscope (FESEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and the nitrogen adsorption analysis. Under the irradiation of visible light , all the prepared WO 3 /Fe(III) nanofiber photocatalysts exhibit much higher activity for degrading methyl orange (MO) solution than the pristine WO 3 nanofibers, and reaches 94.6% under visible light irradiation for 3 h when the relative grafting amount of Fe(III) ions was 0.003 by mass percentage. Grafting of Fe(III) ions on the surface of WO 3 nanofiber could enhance its visible-light absorption and reduce the photo-generated electron-hole pairs recombination due to the interfacial charge transfer (IFCT) effect, and thus improve its photocatalytic activity , which were further verified by the ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRS), photoluminescence (PL) and the ns-level time-resolved fluorescence decay spectrum measurements.
研究领域:
材料科学
·
光催化化学
·
纳米技术
·
环境功能材料
·
物理化学
✓ 已验证
DOI
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Fei Miao,Zehao Liu,Xin Kang,Cheng Cheng,Xiaoyu Mao,Ruimeng Li,Heng Lin,Hui Zhang
Heterogeneous catalytic oxidation based on iron species for peroxymonosulfate (PMS) activation is considered as one of the most attractive strategies for wastewater treatment. However, the rate-limiting regeneration of Fe(II) from Fe(III) heavily hampers the efficient activation of PMS. In this study, the introduction of electric field to the Fe-supported bentonite (Fe-B) activated PMS process was proposed to enhance the Fe(III)/Fe(II) redox cycle. The Fe-B catalyst performed well in the removal of Acid Orange 7 (AO7) through the synergistic effect of electrolysis and the continuous redox cycle of Fe(III)/Fe(II) for PMS activation. The use of 0.5 g L −1 Fe-B catalyst and 10 mM PMS yielded nearly complete removal of the AO7 (50 mg L −1 ) in 60 min at 2 mA cm −2 of current density. Based on the results of electron paramagnetic resonance (EPR) spectroscopy, chemical quenching tests, X-ray photoelectron spectroscopy (XPS) analysis, and electrochemical measurements, the decolorization of AO7 was dominantly attributed to surface-bound radicals (SO 4 •− ads and • OH ads ) and also the direct electron transfer at DSA anode. Moreover, the electro/Fe-B/PMS system showed an effective pH range from 2.6 to 9.0 and the abatement of AO7 was slightly affected in the presence of natural background anions. This work provides a feasible strategy of PMS activation by cost-effective Fe-B catalyst coupling with electric field and gives an insight into the accelerated oxidation of recalcitrant pollutants.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Shunlong Pan,Xinrui Guo,Rong Li,Hao Hu,Jingwei Yuan,Biming Liu,Shengqiang Hei,Yongjun Zhang
Advanced oxidation processes (AOPs) have been successfully applied for the degradation of fluoroquinolones, but most studies ignored the removal of fluorine ions (F − ) generated after the degradation, and the remaining F − would cause secondary pollution to the water body. In this study, a novel UV radiation/hydrated Fe(III) oxide (HFO) coupling strategy was utilized to activate peroxymonosulfate (PMS) for the comprehensive enhanced removal of norfloxacin (NX) and the generated F − . Results showed that UV/HFO/PMS process significantly improved NX degradation efficiency compared with individual system, and NX degradation efficiency of 97.3% could be achieved by reactive oxygen species (ROS) generated in the process, in which singlet oxygen ( 1 O 2 ) was the main ROS. Moreover, the remaining concentration of F − was generally below 0.35 mg/L within a wide pH range (4–10). And the simultaneous adsorption of HFO for F − is mainly related to coordination and electrostatic interaction . After five cycles, the catalytic efficiency of HFO for NX removal only dropped by 4.4%. Besides, UV/HFO/PMS system had great anti-interference ability on coexisting anions. UV/vis two-dimensional correlation spectroscopy (2DCOS) analysis revealed that ROS would preferentially degrade the piperazine ring, and the quinolone group would be destroyed before the heteroatom during the degradation of NX. This work provides new insights for the treatment of antibiotic pollution.
研究领域:
环境科学
·
水处理工程
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2015
·
IF 4.529
Zhouwei Miao,Xiaogang Gu,Shuguang Lu,Mark L. Brusseau,Ni Yan,Zhaofu Qiu,Qian Sui
In this study, the effects of reducing agents on the degradation of tetrachloroethene (PCE) were investigated in the Fe(II)/Fe(III) catalyzed sodium percarbonate (SPC) system. The addition of reducing agents, including hydroxylamine hydrochloride, sodium sulfite, ascorbic acid and sodium ascorbate, accelerated the Fe(III)/Fe(II) redox cycle, leading to a relatively steady Fe(II) concentration and higher production of free radicals. This, in turn, resulted in enhanced PCE oxidation by SPC, with almost complete PCE removal obtained for appropriate Fe and SPC concentrations. The chemical probe tests, using nitrobenzene and carbon tetrachloride, demonstrated that HO was the predominant radical in the system and that O 2 − played a minor role, which was further confirmed by the results of electron spin resonance measurements. PCE degradation decreased significantly with the addition of isopropanol, a HO scavenger, supporting the hypothesis that HO was primarily responsible for PCE degradation. It is noteworthy that Cl − release was slightly delayed in the first 20 min, indicating that intermediate products were produced. However, these intermediates were further degraded, resulting in the complete conversion of PCE to CO 2 . In conclusion, the use of reducing agents to enhance Fe(II)/Fe(III) catalyzed SPC oxidation appears to be a promising approach for the rapid degradation of organic contaminants in groundwater.
研究领域:
环境化学
·
水处理
·
修复技术
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Ying Cai,Jinhong Fan,Zhigang Liu
This study constructed a FeS-based Fenton-like process to explore the degradation of TTC in the presence of copper ions . The acidic condition of pH 3 was more favorable to the H 2 O 2 decomposition and TTC degradation , and it was slightly enhanced by Cu(II). The production of •OH from H 2 O 2 was revealed through radical scavenging and benzoic acid probe experiments, and the ratio of H 2 O 2 decomposition to •OH production was about 1–1.5, which is comparatively consistent with the theoretical ratio. FeS-based Fenton process was proved to be a homogenous system, the slow release of Fe(II) source and the autocatalytic cycle of Fe(III) to Fe(II) resulting from the reductive species of TTC and dissolved S(-II) improved the production of •OH and the degradation of TTC, which was proved by comparing TTC degradation, TOC removal, H 2 O 2 decomposition and Fe(II) concentration with different iron sources (FeS, Fe(II) and Fe(III)) and external addition of dissolved S(-II). The possible degradation pathways of TTC were subsequently inferred according to the detected products by LC-MS. Understanding these autocatalytic processes is essential to reveal the transformation of redox-active substances in environments and may have potential significance in applying FeS-based Fenton-like process for the treatment of wastewater containing reductive organic matters.
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Sitao Wang,Zhijie Liu,Bolun Pang,Yuting Gao,Santu Luo,Qiaosong Li,Hailan Chen,Michael G Kong
Antibiotics are widely used to treat or prevent infectious diseases in human and veterinary medicine. Excessive residues in the aquatic environment lead to increasingly prominent antibiotic pollution; therefore, it is urgent to develop sustainable strategies for rapidly degrading antibiotics. In this study, a highly synergetic effect for norfloxacin (NOR) remediation is achieved by coupling underwater bubble plasma formation with a Fe (III)–S (IV) system due to the efficient utilization of reactive species in chain reactions. The degradation rate using synergetic approach can reach 76.4% within 50 min discharge, and further increases significantly to 94.4% after 5 h post-discharge. The effects of pulsed peak voltage and Fe (III)/S (IV) dosage on NOR removal are characterized. The existence of hydroxyl radicals ( • OH) and sulfate radicals (SO 4 •− ) are proved by electron spin resonance spectrometer (ESR) during degradation. Furthermore, radical scavenger experiments demonstrate that • OH and SO 4 •− play a crucial role in degradation. Underwater bubble plasma provides the oxic and acidic liquid environment for the Fe (III)–S (IV) system to accelerate the self-perpetuating chain reactions. These reactions not only introduce SO 4 •− and generate more • OH during plasma-on, but also induce their regeneration and further prolong the degradation process during plasma-off through plasma-generated effects. Finally, the degradation intermediates of NOR are identified, and a possible degradation pathway is proposed. The possible contribution weight of each approach on the degradation rate is speculated. These new findings offer promising applications for developing a technology with real potential for the treatment of organic compounds in industrial wastewater treatment.
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产品关联
DOI
高影响因子
MATERIALS RESEARCH BULLETIN
·
2022
·
IF 5.6
Qianyu Wei,Qiuhu Lin,Zezhen Zhang,Lili Wu,Chaocan Zhang
Polyvinylidene fluoride (PVDF)/polyhexamethylene guanidine (PHMG)/tannic acid (TA) coatings have some degree of hydrophilicity but lack stability. To improve the hydrophilicity and stability of antimicrobial PVDF/PHMG/TA membranes, Fe(III) is introduced into the composite system. As a weakly acidic hydrophilic nanoion, Fe(III) can enhance the hydrophilicity and resistance to contamination of the membranes. Furthermore, the stability can be enhanced because a three-dimensional cross-linked coating structure is formed by the complexation of Fe(III), TA and PHMG. This work investigates the effects of different tannic acid concentrations and pH conditions on the hydrophilicity, anti-pollution and stability of the modified coatings. The surface morphology of the membranes was analyzed by field-emission scanning electron microscopy. Additionally, the hydrophilicity and the antipollution performance were evaluated based on the water contact angle, submerged oil contact angle, emulsion flux and flux recovery rate. The stability was evaluated by the changes in flux recovery rate and water contact angle before and after emulsion scouring and ultrasonic treatment. The results show that the modified membranes have favorable hydrophilicity and stability after the addition of Fe(III). The water contact angle can be reduced to 19°, the pure water flux can reach 13,850 L·m −2 ·h −1 , and the emulsion flux can reach 2650 L·m −2 ·h −1 . Moreover, 99.68% flux recovery was achieved after 7 days of deionized water flushing, and the water contact angle remained almost unchanged.
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产品关联
DOI
高影响因子
JOURNAL OF FLUORESCENCE
·
2022
·Vol. 32
·期 5
·1743-1754
·
IF 2.525
Xu Ouwen,Wan Shuyu,Yang Jing,Song Hanyang,Dong Luzheng,Xia Ji,Zhu Xiashi
In this work, an “on-off-on” fluorescent probe based on Ni-MOF functionalized Nitrogen-doped carbon quantum dots (Ni-MOF-NCDs) was developed. Ni-MOF-NCDs was characterized by FT-IR, TEM, SEM, and XPS. The presence of Fe (III) will reduce the fluorescence intensity of Ni-MOF-NCDs and “turn off” the fluorescence signal at emission peak of 390 nm, while the signal can be “turn on” after the addition of ascorbic acid (AA). The Ni-MOF-NCDs was established as an “on-off-on” fluorescent probe for the detection of Fe (III) and AA with the linear ranges of 0.029-8.0 µg/mL and 0.263-18.0 µg/mL, respectively. The method has been successfully applied to the detection of water samples and foods with satisfactory recovery. The experimental results showed that Ni-MOF-NCDs not only had the fluorescence properties of NCDs, but also had the adsorption performance of Ni-MOF.
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产品关联
DOI
PubMed
高影响因子
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