INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Like Ouyang,Yuan Wang,Ping Zhang,Xinlong Wang,Shaojun Yuan
Arsenite contamination in groundwater seriously impairs human health due to its high mobility and toxicity. Herein, a novel heterostructured MWCNTs@PANI@TiO2 nanocomposite was synthesized via a one-pot polymerization process for the adsorption and photocatalytic oxidation of As(III) from aqueous solution. In the dark, the as-synthesized nanocomposite had a high adsorption capacity of As(III) at about 0.29 mmol·g–1 with an initial As(III) concentration of 0.067–0.801 mmol·L–1 at 298.15 K and exhibited a stable adsorption capacity in a wide pH range of 2–9. The adsorption kinetics of As(III) on MWCNTs@PANI@TiO2 was in accordance with the PSO model and was mainly controlled by chemical adsorption. Under visible light irradiation, the adsorption amount of As(III) on MWCNTs@PANI@TiO2 was substantially enhanced by about 57%, and the photocatalytic conversion of As(III) to As(V) was found to be caused by the photogenerated holes and superoxide free radical (•O2–). The hypothesized adsorption mechanisms of As(III) and As(V) ions on the nanocomposite were possibly ascribed to surface complexation and hydrogen-bonded interactions. The heterostructured MWCNTs@PANI@TiO2 nanocomposite offers a promising candidate for highly efficient removal of As(III) ions from arsenite-polluted groundwater.
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DALTON TRANSACTIONS
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2020
·Vol. 49
·期 27
·9274-9281
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IF 4.174
He Li,Yu Zou,Jiang Jiang
Ag and CuO in the form of nanoparticles have been widely used in our daily life as antibacterial agents, through releasing Ag ions and generating reactive oxygen species (ROS). In this work, we demonstrate that by synthesizing Ag@CuO nanohybrids with core–shell configurations, their bactericidal activity can be synergistically enhanced compared to the respective constituents. Upon AM 1.5G light illumination for short durations, the measured minimum inhibitory concentrations of the Ag@CuO nanohybrids show a significant decrease against both Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus bacterial strains, requiring only 7% and 34% of those when conducted in the dark. The spread plate results demonstrate that with nanohybrid concentrations of 11.0 and 21.9 mg L−1, at least 7 orders of magnitude decrease in Escherichia coli and Staphylococcus aureus colony forming units is achieved, when the Ag@CuO nanohybrids are exposed to light illumination for 10 min. The effect of illumination is found to induce Ag+ release and enhance 1O2 generation, which act concertedly to facilitate the remarkable photo-enhanced bactericidal effect.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Yunqi Wang,Peng Zhou,Qingguo Wang,Xiaowei Huo,Xue Huang,Qian Ye,Hao Xu,Guanyu Zhou,Yuhang Liu,Jing Zhang
Hydroxylated fullerene, Fullerol, has applied in many areas because of its high electron affinity and antioxidant potential, while it was few used in wastewater treatment. In this study, the mechanism involved that Fullerol accelerated the regeneration of Fe(II) in the Fe(III)/H 2 O 2 system under dark condition, which was investigated with chloramphenicol (CAP) as a model pollutant. In Fullerol/Fe(III)/H 2 O 2 system, CAP removal was completely achieved at 60 min via a non-photochemical pathway. In addition, the quenching experiments and electron spin resonance (ESR) results indicated that hydroxyl radical ( OH) was the main reactive oxygen species (ROSs). The Fullerol/Fe(III)/H 2 O 2 system had a rate constant of CAP degradation about 5.0 × 10 −2 min −1 , which was about 22 times higher than it in Fe(III)/H 2 O 2 Fenton-like system (2.3 × 10 −3 min −1 ). Fe(II) was ascertained the effective component that was responsible for H 2 O 2 activation to produce OH, which derived from 1) the first pathway: Fullerol complexed with Fe(III) and the redox potential of the complex is much lower than Fe(III)/Fe(II); 2) the second pathway: Fullerol acted as an electron donor to reduce Fe(III) into Fe(II). Moreover, CAP degradation intermediates were identified and its degradation pathways were proposed. This study suggested a new approach for improving the Fe(III)/H 2 O 2 system by accelerating Fe(III)/Fe(II) cycles with Fullerol.
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Journal of Environmental Sciences
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2020
·
IF 4.302
Ting Li,Jianru Liang,Lixiang Zhou
Here we reported an effective method to solve the rate-limiting steps, such as the reduction of Fe 3+ to Fe 2+ and an invalid decomposition of H 2 O 2 in a conventional Fenton-like reaction. A magnetic heterogeneous photocatalyst, Fe 3 O 4 -schwertmannite (Fe 3 O 4 -sch) was successfully developed by adding Fe 3 O 4 in the formation process of schwertmannite . Fe 3 O 4 -sch shows excellent electrons transfer ability and high utilization efficiency of H 2 O 2 (98.5%). The catalytic activity of Fe 3 O 4 -sch was studied through the degradation of phenol in the heterogeneous photo-Fenton process. Phenol degradation at a wide pH (3 - 9) was up to 98% within 6 min under visible light illumination with the Fe 3 O 4 -sch as heterogeneous Fenton catalyst, which was higher than that using pure schwertmannite or Fe 3 O 4 . The excellent photocatalytic performance of Fe 3 O 4 -sch is ascribed to the effective recycling between Fe 3+ and Fe 2+ by the photo-generated electron, and also profit from the formation of the “Z-Scheme” system. According to the relevant data, photocatalytic mechanism of Fe 3 O 4 -sch for degrading phenol was proposed. This study not only provides an efficient way of enhancing heterogeneous Fenton reaction , but also gives potential application for iron oxyhydroxysulfate mineral.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Zehua Zeng,Aimal Khan,Zixuan Wang,Mengmeng Zhao,Wanling Mo,Zhuqi Chen
In this study, a series of Mn based catalysts with different oxidative states, crystal structures and morphologies was applied to activate peroxymonosulfate (PMS) for the degradation of atrazine (ATZ). Among them, α-MnO 2 nanowires (Mn-1) demonstrated the highest efficiency. The structure-performance relationship study revealed that the generation of Mn(III) along with the transformation of lattice oxygen to surface hydroxyl groups played the dominant role in controlling the efficiency, and Mn-1 are prone to undergo electron transfer to achieve the transition from Mn(IV) to Mn(III) or even Mn(II). Both radical (sulfate radical (SO 4 •− ) and hydroxyl radical (•OH)) and non-radical species ( 1 O 2 ) contributed to ATZ degradation and accordingly inhibit the formation of toxic BrO 3 − from Br − . Sixteen intermediates were identified in proposed degradation pathways. The toxicity tests, the consistent performance with coexisting anions and humic acid in water matrix, and the satisfying reusability implied the sustainable application of Mn-1/PMS in future.
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WATER RESEARCH
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2020
·
IF 9.13
Zhenxing Zeng,Yaofang Fan,Xie Quan,Hongtao Yu,Shuo Chen,Shushen Zhang
Polymeric photocatalysts are promising candidates for water purification , however their catalytic performance are still unsatisfactory due to the fast charge recombination that leads to low reactive oxygen radicals production. In this study, a conceptual energy-transfer-mediated photocatalytic oxygen activation system over polymeric carbon nitride without the need of electron-hole separation is proposed, exhibiting remarkable singlet oxygen triggered bacteria inactivation performance as well as organic pollutants degradation . By structure and excitonic effect modulation, the oxygen activation process changes from the traditional electron-transfer mechanism to the final energy-transfer pathway, leading to the selective generation of singlet oxygen with high efficiency. The generated singlet oxygen is found to fervently attack the bacteria membrane, creating irreparable pores or holes on the cell membrane for cytoplasmic contents leaking out to accelerate bacteria destruction. The work demonstrated here offers a new photocatalytic oxygen activation pathway for achieving high-efficient reactive oxygen species generation performance without the need of charge separation.
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Molecular Catalysis
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2020
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IF 3.687
Li Fang,Qionghao Xu,Yanyan Qi,Xiaoxue Wu,Yanghe Fu,Qiang Xiao,Fumin Zhang,Weidong Zhu
The preparation of efficient and recyclable solid catalysts exhibiting high activity and selectivity toward the target product is a prerequisite to enhance the overall efficiency of a catalytic process. Herein, we study a series of Fe/Fe 3 C-containing nitrogen-doped porous carbon microspindles (Fe/Fe 3 C@NC–x, where x stands for the pyrolysis temperature), which are core-/shell-structured hybrids, constructed by the pyrolysis of a metal–organic framework precursor as highly selective catalysts for the oxidation of sulfides to the corresponding sulfoxides under mild conditions. The Fe/Fe 3 C@NC–x microspindles comprising Fe and Fe 3 C nanocrystals inlaid in nitrogen-doped porous carbon shells are fabricated by the direct carbonization of NH 2 –MIL–88B(Fe) polyhedra at 500 °C–800 °C and under nitrogen atmosphere. Among the various investigated catalysts, the Fe/Fe 3 C@NC–600 microspindles exhibit the best catalytic activity, higher than those exhibited by the analogue Fe/Fe 3 C@C–600 without N doping and the commercial Fe 2 O 3 , Fe 3 O 4 , and Fe 3 C used for the catalytic oxidation of sulfides owing to the synergistic contribution of the Fe 3 C sites and adequate nitrogen doping in the porous carbon support. Furthermore, the magnetically separable properties of the Fe/Fe 3 C@NC–600 microspindles enable their convenient isolation from the reaction system using an external magnet, and they can be repeatedly used for six cycles without any loss in catalytic efficiency.
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ANALYTICAL CHEMISTRY
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2020
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IF 6.785
Weiwei Cheng,Xu Teng,Chao Lu
Highly ordered structure of catalysts could spring up unique properties in catalytic activities. There is apparently no good reason to disregard the structurally ordered catalyst-amplified chemiluminescence (CL) signals. Herein, we have fabricated the structurally ordered ionic liquid-layered double hydroxide (LDH) assembly through the hydrogen bonding interactions between abundant hydroxyl groups on the surfaces of LDHs and the amino groups in 1-(3-aminopropyl)-3-methyl-imidazolium tetrafluoroborate ([apmim]BF4). Interestingly, we found that the CL signals of luminol–H2O2 system in the presence of structurally ordered [apmim]BF4 ionic liquid-LDH assembly were extraordinarily enhanced, in comparison with those in the presence of the disordered 1-aminoethyl-3-methyl imidazolium tetrafluoroborate ([aemim]BF4) ionic liquid-LDH assembly. The improved CL performances of the structurally ordered [apmim]BF4 ionic liquid-LDH assembly were attributed to the increasing amounts of superoxide anion radicals (O2•–) and hydroxide radicals (•OH) by accelerating of the mass transport from the solution to the surface of ionic liquid–LDH assembly. In addition, such a highly orderly arrangement could increase the emission of the luminol oxidation products by facilitating the electron transfer. Our findings open up new possibilities in the structurally ordered catalyst-enhanced CL emissions, which can be expected to provide a novel and sensitive platform for the CL amplified detection.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Wei Li,Yongli Zhang,Pingju Zhao,Peng Zhou,Yang Liu,Xin Cheng,Jingquan Wang,Bo Yang,Hongguang Guo
Advanced oxidation processes (AOPs) based on the bimetallic system has been demonstrated as a promising way to enhance the degradation of pollutants in the water. In this study, the degradation of Rhodamine B (RhB) in a zero-valent iron (ZVI)/ peroxymonosulfate system with Cu 2+ was thoroughly investigated. RhB could be efficiently removed (99.3 %) in the optimal ZVI/PMS/Cu 2+ system, while only 58.2 % of RhB could be degraded in the ZVI/PMS system. The influence of reaction parameters on the degradation of RhB was further investigated. Quenching experiments and electron paramagnetic resonance (EPR) tests revealed that various reactive oxygen species could be generated in the ternary system, of which, 1 O 2 and O 2 − were identified for the first time. The effect of various anions, NOM and different water matrix were also considered at different concentrations. A variety of byproducts and degradation pathways were identified using HPLC/MS/MS. Finally, the Quantitative Structure Activity Relationship (QSAR) method of Toxicity Estimation Software Tool (TEST) was applied to estimate the toxicity of the byproducts and the results indicated that the overall toxicity of the target was relatively reduced. This study demonstrated the potential for the removal of environmental reluctant pollutants in water via the combined radical and non-radical pathways.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
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IF 5.162
Yiming Zhou,Juanli Shen,Yong Bai,Te Li,Guoxin Xue
Carboxymethyl cellulose-based hydrogel coated Fe 3 O 4 magnetic nanoparticles were prepared using a coprecipitation combining graft copolymerization method, and characterized by various techniques to study their structure-property relationships. The nanocomposite was used as a heterogeneous Fenton-like catalyst for Acid Red 73 degradation. The effects of several key parameters, solution pH, H 2 O 2 concentration, catalyst dosage, and temperature of the reaction medium on the pseudo-first-order kinetics of dye degradation was evaluated. The results showed that the nanocomposite catalyst were highly effective in activating H 2 O 2 to produce reactive radicals for dye degradation, achieving complete decomposition under optimal conditions of 300 min at 25 °C and pH 3.5 with 100 mM H 2 O 2 and 200 mg·L −1 catalyst. The complexing hydrogel-Fe 2+ /Fe 3+ were the key factors that speed up the redox cycling between Fe 2+ and Fe 3+ species, thus accelerate the fast degradation rate of target pollutants. Scavenging experiments and electron paramagnetic resonance analyses revealed that Acid Red 73 was decomposed mainly by the attack of •OH radicals. Besides, reusability of the prepared nanocatalyst was also tested.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Hao Xu,Qian Ye,Qingguo Wang,Peng Zhou,Xiaowei Huo,Yunqi Wang,Xue Huang,Guanyu Zhou,Jing Zhang
Developing a low-cost and environmental friendly way to promote the Fe(III)/Fe(II) cycling is crucial to enhance the efficiency of Fenton reaction. In this study, g-C 3 N 4 was introduced into the Fe(III)/H 2 O 2 system as electron donor to accelerate Fe(III)/Fe(II) cycling and improve the degradation of organic pollutants under visible light. The g-C 3 N 4 /Fe(III)/H 2 O 2 /light system can achieve excellent degradation of different kinds of organic pollutants under low Fe(III) and H 2 O 2 dosages. The central composite design (CCD) and response surface methodology (RSM) were applied to evaluate the effects of g-C 3 N 4 dosage, Fe(III) dosage, H 2 O 2 dosage and light intensity on the DMP degradation efficiency. The mechanisms were investigated by quenching experiments and electron spin resonance (EPR) analyses that the photo-generated electrons and O 2 – were responsible to the Fe(III) reduction through interfacial and aqueous pathways, respectively. OH was the dominant reactive radical in the DMP degradation. Moreover, DMP degradation routes were proposed including the elimination of specific groups, the hydroxylation process and the ring-opening reactions. This study demonstrates an economical and green approach which provides a promising direction for the practical application of g-C 3 N 4 based photocatalysis by integrating it with the Fe(III)/H 2 O 2 Fenton process.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
·
IF 7.864
Jie Miao,Wei Geng,Pedro J. J. Alvarez,Mingce Long
Nitrogen-doped carbon materials attract broad interest as catalysts for peroxymonosulfate (PMS) activation toward an efficient, nonradical advanced oxidation process. However, synthesis of N-rich carbocatalysts is challenging because of the thermal instability of desirable nitrogenous species (pyrrolic, pyridinic, and graphitic N). Furthermore, the relative importance of different nitrogenous configurations (and associated activation mechanisms) are unclear. Herein, we report a “coating-pyrolysis” method to synthesize porous 2D N-rich nanocarbon materials (PCN-x) derived from dopamine and g-C3N4 in different weight proportions. PCN-0.5 calcined at 800 °C had the highest surface area (759 m2/g) and unprecedentedly high N content (18.5 at%), and displayed the highest efficiency for 4-chlorophenol (4-CP) degradation via PMS activation. A positive correlation was observed between 4-CP oxidation rates and the total pyridinic and pyrrolic N content. These N dopants serve as Lewis basic sites to facilitate 4-CP adsorption on the PCN surface and subsequent electron-transfer from 4-CP to PMS, mediated by surface-bound complexes (PMS–PCN-0.5). The main degradation products were chlorinated oligomers (mostly dimeric biphenolic compounds), which adsorbed to and deteriorated the carbocatalyst. Overall, this study offers new insights for rational design of nitrogen-enriched carbocatalysts, and advances mechanistic understanding of the critical role of N species during nonradical PMS activation.
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