CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Binrong Li,Huijie Wang,Yiying Lan,Yanhua Cui,Yunlei Zhang,Yonghai Feng,Jianming Pan,Minjia Meng,Chundu Wu
Fe species/biochar fiber composite (FCF) has become one of promising materials for wastewater treatment via heterogeneous photo-Fenton reaction. However, the powdered form always suffers from inefficient recovery and inherent iron loss, limiting their practical application. Herein, we provide an alternative polydopamine (pDA)-modified PVDF bead as excellent photo-Fenton support for immobilizing FCF by phase inversion, which not only limits the loss of iron ions, but also promotes the H 2 O 2 decomposition. Moreover, these beads can float on the wastewater due to their inner structure, favoring the harvest of light. Thanks to these unique characteristics, these beads displayed almost 100% of decolorization in self-designed flowing dyes wastewater systems. Particularly, the self-floating beads structure makes catalysts be easily recovered and maintains long-term high activity, which significantly eliminates the inherent challenge of powdered catalyst (e.g. FCF) based degradation process. This work provides an “easily applicable platform” for large-scale applications of powdered photo-Fenton catalyst in wastewater treatment.
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高影响因子
Catalysis Science & Technology
·
2019
·Vol. 10
·期 3
·788-800
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IF 5.726
Rong Ji,Zhi Zhu,Wei Ma,Xu Tang,Yang Liu,Pengwei Huo
A new 2D/2D heterojunction of MoS2/CeO2 is successfully prepared by a facile hydrothermal method. The MoS2/CeO2 heterojunction demonstrates superior photocatalytic performance for the degradation of ciprofloxacin (CIP) to that of pure MoS2 and CeO2. The enhanced degradation efficiency of the MoS2/CeO2 heterojunction is on account of the 2D/2D structure, which not only accelerates the interfacial charge separation but also endows the heterojunction with numerous reactive sites to facilitate the degradation reaction. Meanwhile, the Ce4+ ions in 2D CeO2 serve as the redox centers and utilize the photogenerated carriers to generate more oxygen vacancies. In addition, this paper also carefully discusses the possible photocatalytic reaction mechanisms for the transfer behaviors of charge carriers, generation of reactive species and intermediate degradation products by electrochemical impedance spectroscopy (EIS), electron spin resonance (ESR) and HPLC-MS analysis. This work may provide a promising approach for synthesizing 2D/2D heterojunctions in photocatalytic degradation.
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JOURNAL OF CATALYSIS
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2019
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IF 7.723
Jinxi Feng,Jingxiang Sun,Xiaosheng Liu,Jinzhu Zhu,Shuanghong Tian,Rong Wu,Ya Xiong
Piezocatalysis is an emerging green advanced-oxidation technology for the degradation of toxic pollutants; however, piezomaterials are not generally excellent electrocatalysts. Herein, two complex piezocatalysts (SnO 2 / t -BaTiO 3 and SnO 2 -Sb/ t -BaTiO 3 ) consisting of an electrocatalyst and piezomaterial, respectively, are designed to investigate the coupled effect of piezocatalytic and electrocatalytic processes on the degradation of pollutants. SnO 2 , especially SnO 2 -Sb, can considerably enhance the piezocatalytic degradation of the antibiotic metronidazole (MNZ). The piezocatalytic rate constants of SnO 2 / t -BaTiO 3 and SnO 2 -Sb/ t -BaTiO 3 are 2.3 and 3.0 times that of t -BaTiO 3 , respectively. In the degradation process, SnO 2 and SnO 2 -Sb are confirmed to act as dimensionally stable anode-like (DSA-like) catalysts because they can increase the response of the piezoelectrochemical anodic current and the generation of OH radicals as well as reduce the formation of 1 O 2 . Significantly, the piezoelectric field can drive not only the free charges of t -BaTiO 3 and its remnant piezoelectric field but also those of the loaded electrocatalyst SnO 2 to participate in the degradation of MNZ. These results indicate that the coupling of an excellent electrocatalyst and piezomaterial is an effective method to promote piezocatalytic efficiency.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Fei Peng,Ran Yin,Yuhong Liao,Xi Xie,Jianliang Sun,Dehua Xia,Chun He
This study investigates the degradation of a refractory emerging contaminant (i.e., ibuprofen) by a newly developed piezoelectric catalytic persulfate (PS) activation process. BaTiO 3 nanoparticles (NP) and nanowires (NW) were hydrothermally synthesized and used as the piezo-catalysts to activate PS under ultrasonic irradiation for radical generation and ibuprofen (IBP) degradation. IBP was efficiently degraded in the US/BTO NW/PS system with a pseudo first order rate constant of 0.0818 min −1 , and the rate constant was faster than that in the US/BTO NP/PS (0.0492 min −1 ), US/BTO NW (0.0324 min −1 ) and US/PS (0.0057 min −1 ) systems. The outstanding performance of IBP degradation in the US/BTO NW/PS system was attributed to the continuous generation of SO 4 − and OH via PS activation by the piezo-catalysis induced electrons. SO 4 − and OH contributed 53% and 44% to the IBP degradation respectively. Meanwhile, O 2 − , 1 O 2 and H 2 O 2 were in-situ formed and identified as key intermediates for the generation of SO 4 − and OH. The IBP was partially mineralized and transformed to other organic compounds. The degradation products were identified using the UPLC/ESI-tqMS and a degradation pathway was proposed, which involved a sequence of hydroxylation, decarboxylation/demethylation and ring-opening reactions with SO 4 − and OH. This study demonstrates a new energy-saving approach to activating PS for micropollutant abatement and also provides insights into the mechanisms of the PS activation by the piezoelectric catalysis.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2019
·
IF 4.914
Lijie Xu,Lanyue Qi,Yang Sun,Han Gong,Yiliang Chen,Chun Pei,Lu Gan
Excitation of metal-free graphitic carbon nitride (g-C 3 N 4 ) under visible light can successfully achieve efficient activation of peroxymonosulfate (PMS). Synergistic effects and involved mechanism were systematically investigated using a light-inert endocrine disrupting compound, dimethyl phthalate (DMP), as the target pollutant. Under visible light irradiation, DMP could not be degraded by direct g-C 3 N 4 -mediated photocatalysis , while in the presence of PMS, the dominant radicals were converted from •O 2 to SO 4 • - and •OH, resulting in effective DMP degradation and mineralization. Results showed that higher dosage of PMS or g-C 3 N 4 could increase the activation amount of PMS and corresponding DMP degradation efficiency, but the latter approach was more productive in terms of making the most of PMS. High DMP concentration hindered effective contact between PMS and g-C 3 N 4 , but could provide efficient use of PMS. Higher DMP degradation efficiency was achieved at pH lower than the point of zero charge (5.4). Based on intermediates identification, the DMP degradation was found mainly through radical attack (•OH and SO 4 • - ) of the benzene ring and oxidation of the aliphatic chains.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yi Li,Shuanglong Ma,Shengjun Xu,Haichao Fu,Zhuoqian Li,Kai Li,Kai Sheng,Jinge Du,Xin Lu,Xianghua Li,Shiliang Liu
The biochar loaded with CoFe 2 O 4 nanoparticles (CoFe 2 O 4 /HPC) fabricated by pyrolysis exhibited strong magnetic property, hierarchical porous and graphitized structure. CoFe 2 O 4 /HPC showed much better bisphenol A degradation than CoFe 2 O 4 in presence of peroxymonosulfate. The graphitized structure and the synergistic effect between graphitized structure and CoFe 2 O 4 were found to be responsible for the superiority of CoFe 2 O 4 /HPC among all the other catalysts. The prominent role including radical way mainly contributed by SO 4 − and non-radical way achieved by 1 O 2 , and the secondary role of electron transfer way proceeded by graphitized structure were uncovered. The processes such as redox between Co(III)/Co(II) and Fe(III)/Fe(II), the reduction of Fe(III) by O 2 − , and the participation of C O in 1 O 2 production were significant to the excellent catalytic performance of CoFe 2 O 4 /HPC. Considering its excellent separation, stability, adaptability and reusability, CoFe 2 O 4 /HPC opened up a novel way to develop green catalyst to activate PMS for organic pollutants degradation.
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2019
·
IF 5.589
Bing Liu,Xiaochen Xu,Yuan Xue,Lifen Liu,Fenglin Yang
An integrated method of simultaneous desulfurization and denitrification from flue gas by catalytic ozonation combined with NH 3 /(NH 4 ) 2 S 2 O 8 absorption was developed for the first time. It consisted of two parts: (1) the catalytic ozonation of NO over FeO x /SAPO-34 to study the effects of the various influencing factors, and (2) the absorption–oxidation of NO x and SO 2 induced by ozone combined with a NH 3 /(NH 4 ) 2 S 2 O 8 solution in a bubble column reactor. In Part 1, results showed that under the optimal condition of a molar ratio of 0.5 for O 3 /NO, a residence time of 3 s, a water vapor volume fraction of 4%, a NO initial concentration of 536 mg/m 3 , and a SO 2 initial concentration of 343 mg/m 3 , the oxidation rate of NO was 55%. The characterizations of poisoned catalyst are briefly discussed. In Part 2, as the gas passed sequentially through the ozonizing reactor and the absorber (NH 3 /(NH 4 ) 2 S 2 O 8 solution of 0.8% ammonia and 0.2 mol/L (NH 4 ) 2 S 2 O 8 ), a NO conversion rate of approximately 92.6% and SO 2 conversion rate of 100% were obtained. The pH of the NH 3 /(NH 4 ) 2 S 2 O 8 solution had a significant impact on the NO conversion. According to the analysis of the composition of products under different pHs, a mechanism of desulfurization and denitrification based on NH 3 /(NH 4 ) 2 S 2 O 8 solutions was proposed. The reaction product as a compound fertilizer contained up to 24.5% nitrogen.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Dahu Ding,Shengjiong Yang,Liwei Chen,Tianming Cai
Developing carbon-based hybrid catalysts with high reactivity, good stability, and low cost is critical for environmental remediation via heterogeneous advanced oxidation processes (AOPs). In this work, CoFe alloy particles encapsulated in nitrogen doped graphitic carbon (donated as CoFe@N-GC), in situ converted from cobalt modified Prussian blue (PB) precursor through a two-step carbonization route, is rationally designed and synthesized as an advanced catalyst for the degradation of antibiotics norfloxacin (NOF) by coupling with peroxymonosulfate (PMS). The resultant hybrid catalyst can not only offer a conductive network that promotes the electron transfer but also protect the metal species from being leached out. By serving as a catalyst/activator, it shows an outperforming performance in catalytic degradation of organic pollutants than other catalysts (i.e. CuO, CoFe 2 O 4 , and biochar). The electron paramagnetic resonance (EPR) results clearly reveal that the sulfate radicals (SO 4 •− ) and singlet oxygen ( 1 O 2 ) are the dominant reactive oxidative species (ROS). After four successive cycles, CoFe@N-GC still performs excellent catalytic activity, leading to a NOF degradation of 94.4% within 20 min ([NOF] = 15 µM, [PMS] = 0.2 mM, [Catalyst] = 0.05 g L −1 , pH = 6.0). This study highlights the in situ synthesis of CoFe@N-GC with outstanding activities for catalytic degradation of organic pollutants.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Chaoting Guan,Jin Jiang,Suyan Pang,Xiao Chen,Richard D. Webster,Teik-Thye Lim
Previous studies have reported that metal-doped graphitic carbon nitride (g-C 3 N 4 ) materials can activate peroxymonosulfate (PMS) to destruct organic pollutants. Herein, we interestingly found that pure g-C 3 N 4 materials synthesized via a facile calcination protocol without any metal doping could serve as the efficient PMS activator for degrading bisphenol A (BPA). The influences of different precursors (i.e., melamine, dicyandiamide, and urea) and annealing ambience (i.e., air or N 2 ) on the catalytic activity were investigated. The resultant g-C 3 N 4 materials exhibited different catalytic activities for PMS activation. The best performance was found in the case of g-C 3 N 4 synthesized from melamine and annealed in N 2 (g-C 3 N 4 -Melamine-N 2 ); 100% BPA (10 μM) removal was achieved by using 0.5 g/L catalyst and 1 mM PMS at pH 7 in 15 min. The difference in catalytic activities of these g-C 3 N 4 materials might be attributed to the fact that different preparation procedures impacted the chemical composition and structure of catalysts and thus changed the type and density of active sites. Important influencing factors such as PMS dosage, temperature, solution pH, and water matrices on degradation kinetics of BPA were evaluated. Results of quenching experiments and electron paramagnetic resonance spectroscopy revealed that sulfate radical and hydroxyl radical were main reactive species for BPA degradation by the g-C 3 N 4 /PMS system, which was also confirmed by the non-selectivity of this system towards various organics. Furthermore, possible transformation pathways of BPA by the g-C 3 N 4 /PMS system were proposed based on the identified oxidation products, primarily involving hydroxylation, bond cleavage, ring opening, as well as radical coupling. This study deepens mechanistic understanding of g-C 3 N 4 materials driven PMS oxidation processes, and also provides a green and efficient strategy for eliminating BPA in water.
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高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2019
·Vol. 95
·期 3
·567-576
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IF 2.659
Jie Wang,Kankan Shang,Xueyan Guo,Xingyan Xia,Liangjun Da
BACKGROUND This study investigates a novel, efficient and green pretreatment approach using ferrous iron catalyzed peracetic acid oxidation (Fe 2+ /PAA) on anaerobic fermentation of waste activated sludge. The underlying mechanisms are also studied for both the chemical and microbial effects. RESULTS The results indicate that Fe 2+ /PAA exhibit significant positive synergistic effect on short-chain fatty acid (SCFA) generation, especially acetic acid. The maximal SCFA concentration of 272 mg COD g −1 VSS is obtained with Fe 2+ (2.7 mmol L –1 )/PAA (3.0 mmol L –1 ), which is 5.2 times that of the control test. Fe 2+ /PAA can effectively facilitate sludge solubilization due to the disruption of extracellular polymeric substances structure and microbial cells. The biodegradability of released organic substance is also improved due to the oxidation of non-biodegradable substances. The activity of functional enzymes for hydrolysis and acidification is enhanced but that for methanogenesis is inhibited. Further analysis on microbial community structure indicates that phylum Firmicutes and genera Proteiniclasticum showed the maximal positive correlation with SCFA production, while the abundance of methanogenic archaea especially acetoclastic methanogenic archaea is inhibited by Fe 2+ /PAA treatment. Moreover, the presence of Fe 2+ lengthened the oxygen release period of PAA, the main functional reactive oxygen species are hydroxyl radicals and Fe 2+ facilitated PAA generates more hydroxyl radicals thus enhancing the oxidation ability of PAA. CONCLUSION This study demonstrated that Fe 2+ /PAA can be used as an effective pretreatment method for SCFA accumulation in sludge anaerobic fermentation process. The findings obtained in this study will supply information for the application of Fe 2+ catalyzed PAA pre-oxidation in sludge treatment. © 2019 Society of Chemical Industry
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Qian Ye,Hao Xu,Jing Zhang,Qingguo Wang,Peng Zhou,Yunqi Wang,Xue Huang,Xiaowei Huo,Chaorong Liu,Jinfeng Lu
This work presented a new strategy to activate peroxymonosulfate (PMS) by the addition of nano-zero-valent tungsten (nZVT) via accelerating the redox cycles of Cu(II)/Cu(I), which induce the consecutive generation of highly reactive oxygen species ultimately. The oxidation capacity of the nZVT/Cu(II)/PMS process and the detailed mechanisms of PMS activation were investigated with tetracycline (TC) as the targeted pollutant. Our results indicated that about 70% TC removal was obtained in the nZVT/Cu(II)/PMS system in 15 min with an initial pH of 4.6. In addition, hydroxyl radicals ( OH), sulfate radicals (SO 4 − ), and superoxide radicals ( O 2 − ) were identified as the reactive oxygen species (ROSs) attributed to rapid TC decomposition according to the quenching studies and EPR technology. The effective component that was responsible for PMS activation and ROSs generation was ascertained to be the resulting Cu(I), which derived from the direct reduction pathway driven by epigenetic low valence tungsten species and the indirect reduction pathway driven by active hydrogen atoms. Further, the presence of Cu(II) significantly accelerated the corrosion of the nZVT powders, leading to the accumulation of low valence tungsten species and the decrease in the mean diameter of the ZVT nanoparticles. There was no obvious change of the composition and structure between the original and residual nZVT powders, as evidenced by XPS and XRD analysis. The degradation process of TC included the cleavage of specific functional groups, the ring-opening reactions and the hydroxylation process. This study provided theoretical significance in applying zero-valent metals to activate PMS through a cupric/cuprous redox cycling mechanism.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Peng Zhou,Jing Zhang,Zhaokun Xiong,Yang Liu,Xiaowei Huo,Xin Cheng,Wenshu Li,Feng Cheng,Yongli Zhang
Hydroxylated C 60 Fullerene (Fullerol) induced photochemical production of reactive oxygen species (ROS, e.g. singlet oxygen ( 1 O 2 ) and hydroxyl radical ( OH)) is a slow process, and the role of its surface groups other than high water-solubility is still lack of investigation. In this study, we demonstrate Fullerol can promote Fe(III)/Fe(II) cycles to degrade dimethyl phthalate (DMP) in Fe(III)/H 2 O 2 Fenton system as both an electron donor and an electron-transfer mediator. At acidic condition, the formation of carbonyl and carboxyl via pinacol rearrangement and subsequent keto-enol isomerization can produce cage-opened structure of Fullerol, resulting in the pH-dependent formation of Fe(III)-Fullerol complex. Two pathways of Fe(II) recovery via intramolecular electron transfer of Fe(III)-Fullerol complex to enhance Fe(III)/H 2 O 2 Fenton oxidation were proposed: 1) Fullerol direct reduces Fe(III) into Fe(II) as an electron donor in dark, and it was strongly enhanced under visible light irradiation; 2) Fullerol mediates electron transfer from electron donor (e.g. hydrogen peroxide and organics) to Fe(III) in visible light condition. Furthermore, DMP degradation pathway was proposed based on variation of main intermediates.
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