ACS Applied Materials & Interfaces
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2018
·
IF 8.097
Yanan Wei,Bingfeng Wang,Xinfang Cui,Yaseen Muhammad,Yanjuan Zhang,Zuqiang Huang,Xuesheng Li,Zhenxia Zhao,Zhongxing Zhao
MIL(Fe)/Fe-doped nanospongy porous biocarbon (Fe-SPC) composite was fabricated from MIL-100(Fe) via in situ growth on a unique Fe-doped nanospongy porous biocarbon (Fe-SPC) and was used as Fenton-like catalyst for advanced degradation of thiamethoxam (THIA). Fe was loaded on silkworm excrement and calcined to Fe-SPC with nanospongy and high sp2 C structure. The in situ growth strategy embedded the Fe-SPC into MIL-100(Fe) crystals and formed conductive heterojunctions with an intensified interface by Fe-bridging effect, which was confirmed by negative shift of Fe3+ binding energy in X-ray photoelectron spectroscopy. MIL(Fe)/Fe-SPC composites exhibited high degree of crystallinity and surface area (Brunauer–Emmett–Teller: 1730 m2/g). Liquid chromatography–mass spectrometry and density functional theory simulations demonstrated that THIA was converted to a relatively stable compound (C4H5N2SCl), which could be captured by MIL-100(Fe) with strong chemical bonding energy (Fe–N, −587 kJ/mol), followed by a significant geometric distortion, resulting in a thorough degradation. Efficient charge separation and synergistic chemisorption-catalysis strategy resulted in the high catalytic activity of MIL(Fe)/Fe-SPC. The composite catalyst concurrently exhibited high mineralization ratio with 95.4% total organic carbon removal (at 25 °C and 180 min) and good recycling ability under wider neutral/alkaline conditions. Endorsing to these intriguing properties, MIL(Fe)/Fe-SPC can be deemed an efficient contender for removal of hard-degradable pesticides and other environmental pollutants in practical applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Zhenying Jiang,Lingzhi Wang,Juying Lei,Yongdi Liu,Jinlong Zhang
The application of photo-Fenton process is restricted by the acidic pH and additional hydrogen peroxide (H 2 O 2 ). In order to overcome these drawbacks, a photo-Fenton system of CdS/rGO/Fe 2+ which can perform at natural pH with in situ -generated H 2 O 2 has been successfully developed. Highly efficient photo-Fenton degradation of phenol was achieved under the visible light irradiation via the CdS/rGO/Fe 2+ system. Experimental results showed that phenol could be degraded completely in 1 h at natural pH. The plentiful in situ generation of H 2 O 2 was further proved to act as an important role in phenol degradation with the addition of Fe 2+ . The advantages of degradation at natural pH with in situ -generated H 2 O 2 can provide a new prospective to the environmental-friendly Fenton process.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2018
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IF 4.61
Zeng-Hui Diao,Jian-Jun Du,Dan Jiang,Ling-Jun Kong,Wen-Yi Huo,Cui-Mei Liu,Qi-Hang Wu,Xiang-Rong Xu
Cr 6+ and Pb 2+ are both highly toxic pollutants and commonly co-exist in some industrial effluents and contaminated waters . In this study, simultaneous removal of Cr 6+ and Pb 2+ by a novel sewage sludge-derived biochar immobilized nanoscale zero-valent iron (SSB-nZVI) was systematically investigated. It was well demonstrated that a porous structure was successfully formed on the SSB-nZVI when the starch was used as an additive. A synergistic effect on the adsorption and reduction over the SSB-nZVI was achieved, resulting in nearly 90 and 82% of Cr 6+ and Pb 2+ removal within 30 min, respectively. Cr 6+ was reduced prior to Pb 2+ . A low pH could accelerate the corrosion of nZVI as well as phosphate leaching. When Malachite green was added as a coexisting organic pollutant, its effective removal was found due to the formation of a Fenton-like system. The SSB-nZVI could be run consecutively three times with a relatively satisfactory performance. Most of Cr 6+ was converted into Cr 2 O 3 and Cr(OH) 3 on the SSB-nZVI surface, whereas most of Pb 2+ species existed as Pb(OH) 2 (or PbO). A possible reaction mechanism on the SSB-nZVI involved the adsorption, reduction and precipitation of both Cr 6+ and Pb 2+ over the particles. Present study sheds light on the insight of the fate and transport of Cr 6+ and Pb 2+ in aquatic environment, as well provides helpful guide for the remediation of coexistence of pollutants in real applications.
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Catalysis Science & Technology
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2019
·Vol. 9
·期 16
·4365-4373
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IF 5.726
Shiyuan Gao,Haoran Zhou,Yannan Xia,Xiudan Liu,Yuyuan Yao,Wentao Wang,Haixiang Chen
The development of efficient and environment-benign catalytic materials to activate peroxymonosulfate (PMS) for refractory pollutant removal has been considered as an attractive yet challenging topic in the field of wastewater treatment. Herein, carbon fiber-assisted iron carbide (Fe3C@CFs) was innovatively prepared by a hydrothermal and calcination method. Fe3C@CFs could activate PMS and remove the pollutant Acid Red 1 (AR1) up to 97.3%, and even the rate constant was 12.4 times higher than that of Fe3C. The leaching of iron ions was only 0.002 ppm, which was extremely lower than the European standard. Furthermore, Fe3C@CFs still exhibited a favorable catalytic performance after 4 cycles. The catalytic mechanism was investigated by a hybrid method of various radical scavengers combined with electron spin resonance, suggesting that 1O2 served as the main reaction oxidation species rather than ˙OH or SO4˙− during the catalytic process, different from most of the reported radical paths for activating PMS. In addition, Fe3C@CFs possessed wide pH adaptability (3–10) and relatively low activation energy (24.47 kJ mol−1) for AR1 removal. These findings pave a promising avenue to develop highly efficient and eco-friendly catalytic materials for environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Xiaohui Wang,Zhipeng Li,Yadan Ding,Kexin Wang,Zhenkai Xing,Xue Sun,Wanqiu Guo,Xia Hong,Xiaojuan Zhu,Yichun Liu
It is challenging and urgent in neurosurgery to improve therapeutic effect of the most common and lethal malignant glioma in central nervous system. The superadditive therapeutic effect of photothermal therapy and photodynamic therapy holds great promise. Herein, a highly efficient photothermal-photodynamic therapy nanoplatform was developed on the basis of Fe 3 O 4 -IR806 superparticles. The introduction of the near-infrared (NIR) dye IR806 and the fabrication of the self-assembled structure of the superparticles warrant 3.5 times increase in the photothermal conversion efficiency compared with the Fe 3 O 4 nanoparticles . The Fe 3 O 4 -IR806 superparticles generated reactive oxygen species (ROS) with the NIR light irradiation by virtue of the dye IR806. Both in vitro and in vivo experiments demonstrated that the Fe 3 O 4 -IR806 superparticles exhibited negligible toxicity. The Fe 3 O 4 -IR806 superparticles efficiently inhibited the cultured glioma cells via photothermal ablation and ROS cytotoxicity in vitro, as well as suppressed the bearing glioma growth in vivo with the NIR light induction. Our results highlight the promise of the Fe 3 O 4 -IR806 superparticles for improved photothermal-photodynamic therapy of cancer.
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ANALYTICAL CHEMISTRY
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2019
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IF 6.35
Lei Jiao,Weiqing Xu,Hongye Yan,Yu Wu,Chunrong Liu,Dan Du,Yuehe Lin,Chengzhou Zhu
Recently, in situ detection of hydrogen peroxide (H2O2) generated from live cells have caused tremendous attention, because it is of great significance in the control of multiple biological processes. Herein, Fe–N–C single-atom nanozymes (Fe–N–C SAzymes) with intrinsic peroxidase-like activity were successfully prepared via high-temperature calcination using FeCl2, glucose, and dicyandiamide as precursors. The Fe–N–C SAzymes with FeNx as active sites were similar to natural metalloproteases, which can specifically enhance the peroxidase-like activity rather than oxidase-like activity. Accordingly, owing to the excellent catalytic efficiency of the Fe–N–C SAzymes, colorimetric biosensing of H2O2 in vitro was performed via a typical 3,3′,5,5′-tetramethylbenzidine induced an allochroic reaction, demonstrating the satisfactory specificity and sensitivity. With regard to the practical application, in situ detection of H2O2 generated from the Hela cells by the Fe–N–C SAzymes was also performed, which can expand the applications of the newborn SAzymes.
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JOURNAL OF HAZARDOUS MATERIALS
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2019
·
IF 7.65
Aihua Xu,Yi Wei,Qiancheng Zou,Wenyu Zhang,Yezi Jin,Zeyu Wang,Lizhen Yang,Xiaoxia Li
Herein, a new peroxymonosulfate (PMS) activation system was proposed employing nonredox metal ions as Lewis acids (LA), which have been widely recognized to play important roles in many biological and chemical oxidations. With Co 2+ ions as model catalysts, it was found that oxidizing power of PMS was enhanced after binding weak LA such as Ca 2+ ions, leading to its easier reduction to active radicals and substantial enhancement of dye degradation. The promoting effect of Ca 2+ was also observed with other cobalt catalysts including CoFe 2 O 4 and Co 3 O 4 . The rate of PMS decomposition in Co 2+ +LA/PMS system was correlated with Lewis acidity; while in the presence of strong LA including La 3+ and Y 3+ , the dye degradation rate declined. The interactions of LA with PMS were characterized and the detailed mechanism was proposed. The present study provides the first example of the promoting effect of weak LA on PMS activation with cobalt based catalysts.
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JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Mingyu Wei,Xiaowen Shi,Ling Xiao,Haifei Zhang
Polyimide-modified carbon nanotubes (PI/CNTs) were synthesized via a solvent-free thermal method and used as a metal-free catalyst to activate peroxymonosulfate for organic contaminant degradation without light irradiation. The characterization results suggested that PI was loaded onto the surface of CNTs . The catalytic ability of the PI/CNTs was strongly correlated with the content of PI in the catalysts. The PI/CNTs (22% of PI) showed the highest catalytic efficiency for organic pollutant degradation at room temperature. The degradation efficiency of acid orange 7 (AO7) dye was significantly enhanced to 98.9% within 15 min, compared to the efficiency of 2.2% exhibited by pure PI. The radical quenching tests and electron paramagnetic resonance spectrometry proved that singlet oxygen, instead of hydroxyl radicals or sulfate radicals, played a dominant role during the catalytic oxidation of AO7. The influences of operation parameters including temperature and catalyst amount were investigated. The PI/CNTs metal-free catalyst exhibited high catalytic activity under a broad range of pH values. The recycling study of four repeated reactions demonstrated good stability of the PI/CNTs. This work provided a promising metal-free catalyst for degradation of organic pollutants in aqueous solutions, contributing to the development of green materials for sustainable remediation.
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FOOD CONTROL
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2019
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IF 4.248
Yulin Zhu,Changzhu Li,Haiying Cui,Lin Lin
As a non-thermal sterilization method, pulsed light (PL) has been widely applied in food industries to control the microbial contamination, however little is known about the antimicrobial mechanism of PL. This study deeply investigated the antimicrobial mechanism of PL against Escherichia coli O157:H7 ( E. coli O157:H7). The changes of morphology, endoenzyme, entocyte, respiratory metabolism and DNA of E. coli O157:H7 after PL treatment were emphatically studied. TEM and SEM results exhibited that cell integrity was destroyed heavily after PL treatment. Entocyte including proteins, ATP and DNA were reduced remarkably for PL-treated samples. In addition, the activity of ATPase, β-galactosidase, alkaline phosphatase, topoisomerase, as well as the metabolism were inhibited for E. coli O157:H7 with PL treatment. The electron spin resonance spectrum validated the production of hydroxyl radical by PL, thus resulting in the elevation of intracellular reactive oxygen and the acceleration of cell death. Finally, PL displayed better antibacterial activity in carrot juice without adverse effect on its quality.
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CHEMICAL ENGINEERING JOURNAL
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2017
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IF 6.216
Ziyang Lu,Zehui Yu,Jinbo Dong,Minshan Song,Yang Liu,Xinlin Liu,Zhongfei Ma,Hang Su,Yongsheng Yan,Pengwei Huo
The Z-scheme imprinted ZnFe 2 O 4 /Ag/PEDOT was synthesized by the microwave polymerization method and surface imprinting technique, which possessed good partial hollow spherical structure, good light response ability, good magnetic separation performance, good photocatalytic stability and reproducibility. More importantly, due to the introduction of Ag/PEDOT into the surface imprinted layer, Z-scheme structure was formed to enhance the photocatalytic activity based on Ag acted as the mediator, meanwhile, owing to the existence of the imprinted cavity in the surface imprinted layer, the selectivity had been significantly improved, in a word, the as-prepared Z-scheme imprinted ZnFe 2 O 4 /Ag/PEDOT achieved the goal for simultaneously improving the photocatalytic activity and selectivity. Z-scheme imprinted ZnFe 2 O 4 /Ag/PEDOT possessed the highest photodegradation rate (71.77%) for degradation of tetracycline under the simulated sunlight irradiation of 120 min, which was approximately 4.74 times to that of ZnFe 2 O 4 , 1.42 times to that of Ag/PEDOT and 1.31 times to that of non-imprinted ZnFe 2 O 4 /Ag/PEDOT, respectively. And the coefficient of selectivity of Z-scheme imprinted ZnFe 2 O 4 /Ag/PEDOT relative to ZnFe 2 O 4 , Ag/PEDOT, non-imprinted ZnFe 2 O 4 /Ag/PEDOT was 1.84, 1.82, 1.79 in the single antibiotic solution and 1.78, 1.75, 1.67 in the binary antibiotic solution, respectively. This work provided a new synthesis strategy for the imprinted photocatalysts and also provided a new idea for the treatment of specific pollutants in the water environment.
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CHEMOSPHERE
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2017
·
IF 4.208
Xiaoxue Pan,Liqing Yan,Ruijuan Qu,Zunyao Wang
The goals of this study were to bring forward new data and insights into the effect of activation methods, operational variables and reaction pathways during sulfate radicals-based oxidation of benzophenone-3 (BP-3) in aqueous solution. Heat, transition metal ions (Fe 2+ , Cu 2+ , Co 2+ ), UV and visible light irradiation were used to activate persulfate (PS) to degrade BP-3. The results showed that these three activation methods can remarkably enhance BP-3 removal efficiency. Under the conditions of [BP-3] 0 : [PS] 0 = 1: 500, pH = 7.0, and 40 °C, complete removal of BP-3 (1.31 μM) was observed in 3 h. In the pH range of 3.0–9.0, the degradation of BP-3 decreased with increasing pH. Increasing the PS dosage accelerated the reaction, while the presence of humic acid (HA) significantly inhibited the efficiency of BP-3 removal. Based on electron paramagnetic resonance (EPR) and radical quenching studies, sulfate and hydroxyl radicals contributed to the oxidation process. According to the evolution of BP-3 and its 7 by-products, as well as frontier electron densities (FED) calculation, two routes were proposed involving hydroxylation, demethylation and direct oxidation. On the whole, this work is a unique contribution to the systematic elucidation of BP-3 removal by PS.
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AICHE JOURNAL
·
2017
·Vol. 64
·期 2
·538-549
·
IF 2.836
Yiyi Sheng,Yang Sun,Jing Xu,Jie Zhang,Yi-Fan Han
Cu-embedded mesoporous alumina, as a Fenton-like catalyst prepared via a sol-gel method, showed excellent activity and durability for the degradation of refectory compounds. The origin of active sites for the generation of hydroxyl radicals (•OH) were thoroughly studied using multitechniques. Cu, as the only active element, could be penetrated into the bulk of alumina and some Cu atoms were embedded into the framework. The dynamic structure of surface Cu species (the variety of Cu + /Cu 2+ ratio) during the reaction were determined as well. Furthermore, the structure plasticity of catalyst has proved by optimizing preparation and reaction conditions. A 98.53% degradation of RhB was recorded within 30 min, following a pseudo-first-order reaction rate expression. Electron spin resonance spectra and •OH scavenging experiments have confirmed that •OH is the main reactive oxidant for the elimination of RhB. By the surface-enhanced Raman spectroscopy and gas chromatography-mass spectrometer results, plausible pathways of RhB degradation were elaborated. © 2017 American Institute of Chemical Engineers AIChE J , 64: 538–549, 2018
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