Journal of the Taiwan Institute of Chemical Engineers
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2021
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IF 5.876
Kai Zhang,Peipei Miao,Huanling Zhang,Yue Wang,Guowei Wang,Xiaolin Zhu,Chunyi Li
Background In the traditional ethylbenzene dehydrogenation process, much superheated steam is needed to ensure the activity and stability of the catalyst, inevitably leading to high energy consumption. Methods A novel ethylbenzene dehydrogenation process based on a circulating fluidized bed (CFB) reactor was used for the ethylbenzene dehydrogenation reaction under a low steam-to-oil ratio. In this work, a series of Fe-Al-based catalysts were prepared by a sol-gel method and the effect of alumina content on the catalytic performance of Fe-Al-based catalyst for ethylbenzene dehydrogenation was investigated. Significant findings Among a series of Fe-Al-based catalysts, the FeAl40 catalyst (the Fe-Al-based catalyst with 40 wt. % alumina) had the highest dehydrogenation activity and suitable attrition resistance for the CFB reactor. Further investigation found that the adding alumina could inhabit the formation of KFe 11 O 17 , leading to poor stability. Interestingly, the high activity of the FeAl40 catalyst could be completely recovered through a reaction-regeneration operation. Compared with the conventional ethylbenzene dehydrogenation process, the CFB process benefits from high activity, low steam-to-oil ratio and no induction period. Consequently, the FeAl40 catalyst had high dehydrogenation activity (∼51 wt. % yield of styrene) and low preparation cost, showing an extraordinary potential for industrial application.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2019
·Vol. 26
·期 36
·36410-36422
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IF 2.914
Latif Abdul,Kai Sun,Si Youbin
This study demonstrated, for the first time, Fe(III)/peroximonosulphate (PMS) could be an efficient advanced oxidation process (AOP) for wastewater treatment. Bisphenol A (BPA) was chosen as a model pollutant in the present study. Fe(III)-activated PMS system proved very effective to eliminate 92.18% of BPA (20 mg/L) for 30-min reaction time at 0.50 mM PMS, 1.5 g/L Fe(III), pH 7.0. The maximum degradation of BPA occurred at neutral pH, while it was suppressed at both strongly acidic and alkaline conditions. Organic and inorganic ions can interfere with system efficiency either positively or negatively, so their interaction was thoroughly investigated. Furthermore, the presence of organic acids also affected BPA degradation rate, especially the addition of 10 mM citric acid decreased the degradation rate from 92.18 to 66.08%. Radical scavenging experiments showed that SO 4 •– was the dominant reactive species in Fe(III)/PMS system. A total of 5 BPA intermediates were found by using LC/MS. A possible degradation pathway was proposed which underwent through bridge cleavage and hydroxylation processes. Acute toxicity of the BPA degradation products was assessed using Escherichia coli growth inhibition test . These findings proved to be promising and economical to deal with wastewater using iron mineral for the elimination of organic pollutants.
Graphical abstract
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JOURNAL OF SOLID STATE CHEMISTRY
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2019
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IF 2.291
Yixuan Huang,Hao Lin,Yanhui Zhang
Carboxylate systems with inert oxide, namely, MIL-101(Fe)/SiO 2 , have been prepared by hydrothermal reactions and characterized. MIL-101(Fe)/SiO 2 exhibits superior catalytic activities for p -nitrophenol reduction with a high conversion of 93.8% in 4 min. It is obvious that the catalytic activity for reduction of nitroaromatic compounds is enhanced, however, the proportion of active components on a catalyst is reduced. One hypothesis is that the interfacial effect between SiO 2 and MIL-101(Fe) complexes helps to increase the catalytic activity. The increase of the interface component greatly improved the free energy of the interface of the solid, and the structure-related properties such as the ion valence state and the electron motion transfer of the interface have undergone considerable changes. In addition, the stability of the catalyst under the conditions of different acid-base was also investigated. It is supposed to broaden the application of the interface effect of the complex with SiO 2 .
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CARBON
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2019
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IF 7.466
Wei Miao,Ying Liu,Xiaoyan Chen,Yixin Zhao,Shun Mao
In recent years, design high catalytic graphitic carbon nitride (g–C 3 N 4 )–based catalysts has drawn broad attention in environmental remediation. In this work, a series of iron-doped g-C 3 N 4 compounds were synthesized through a simple bottom-up strategy. By controlled pyrolysis , iron-doped g-C 3 N 4 materials split from bulk structure into multi-layer structure with uniformly dispersed mesopores. The catalytic activities of layered iron-doped g-C 3 N 4 in Fenton-like and photo-Fenton-like processes were investigated. Due to the doped iron, unique layered structure, and mesopore feature, the catalysts present greatly enhanced performance in heterogeneous Fenton-like reactions. Moreover, the degradation parameters calculated by the pseudo-first-order kinetic model fitted well with the specific surface area of the catalyst, indicating that the catalytic activities rely heavily on the specific surface area of layered and porous g-C 3 N 4 . This study presents a facile and generic method to regulate C 3 N 4 morphology and structure for enhanced catalytic activity in Fenton-like reactions.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2019
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IF 5.589
Yongjie Wan,Jinquan Wan,Yongwen Ma,Yan Wang,Ting Luo
In this study, four typical modulators (NH 4 OH(A), CH 3 COOH(B), CH 3 COONa(C) and CH 3 COONH 4 (D)) were applied to modulate the microwave-assisted synthesis of Fe-MOFs. The effects of various modulators on the yield, electrochemistry activity and PS activation capacity of prepared catalysts were systematically investigated. The ideal modulator was revealed as the 7.5 mM CH 3 COONH 4 . Contributed by the defects caused by the dual effects of CH 3 COONH 4 , Fe-MOFs-D-7.5/PS system showed excellent orange G (OG) degradation with high reaction stoichiometric efficiency (RSE) and desirable recycling performance. The main radicals should be SO 4 ·− and O 2 ·− which were confirmed by EPR and chemical quenchers. Furthermore, the frontier molecular orbital (FMO) theory and dual descriptor (DD) method were employed in predicting radical attacking sites of OG. According to the results of theoretical computations and experimental detection, degradation pathways of OG in Fe-MOFs-D-7.5/PS system were proposed. Similar to the function of the battery, this study gives new insight into the possible mediatory roles of Fe-MOFs-D-7.5 in PS activation by transferring the electrons between PS and the unsaturated metal sites (CUS). The Fe-MOFs-D-7.5/PS system is a promising process for environmental remediation.
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VACUUM
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2019
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IF 2.515
Kun Wang,Xiaobing Huang,Tao Zhou,Haiyan Wang,Huasheng Xie,Yurong Ren
Li 2 FeSiO 4 /C cathode composites were fabricated from a simple solid-state approach using precursor Fe-MOFs prepared by hydrothermal process. The Li 2 FeSiO 4 /C composites covered by carbon film with diverse contents were characterized using XRD , SEM , galvanostatic charge-discharge measurement and EIS, and so on. Results of the investigation prove that Li 2 FeSiO 4 /C composites with 19.3 wt % carbon layer present prominent electrochemical capability, which delivered the discharge capacity of 154, 138, 129, 117 and 100 mA h g −1 at 0.2, 0.5, 1, 2 and 5 C, respectively. After 100 cycles, discharge capacity retained 97.4% compared to the original value at 2 C. Furthermore, it possesses the lowest charge transfer resistance as well as the highest Li + diffusion coefficient , attributing to uniform carbon coating and porous structure for Li 2 FeSiO 4 /C composites.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
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IF 6.361
Junxia Guo,Jinhe Shu,Jun Nie,Guiping Ma
In this work, oxygen reduction reaction (ORR) electrocatalysts Fe/Ni bimetal and nitrogen co-doped porous carbon fibers (Fe x /Ni y -NPCF), derived from electrospun nanofiber , have been prepared. In order to optimize the ORR performance of one dimension (1D) catalysts, SiO 2 were used as template to create the hierarchical porous structure. The morphology of Fe x /Ni y -NPCF was investigated by scanning electron microscope (SEM) and transmission electron microscope (TEM). By adjusting the ratio of iron and nickel, the influence of the trace of secondary-metal doping in electrocatalyst on catalytic activity was deeply studied. The electrochemical measurements suggested that the trace of secondary-metal doping was good for increasing the half-wave potential of electrocatalyst. The optimized Fe 28 /Ni 2 -NPCF exhibited an excellent catalytic activity with an onset potential of 0.96 V and a half-wave potential of 0.88 V, which are comparable to that of the benchmark 20 wt% Pt/C. This excellent catalytic performance was derived from secondary-metal doping and abundant pore structure .
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
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2019
·Vol. 57
·期 7
·767-775
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IF 2.591
Xianhui Zhang,Guangqian Zhu,Qaiser Mahmood,Mengmeng Zhao,Liang Wang,Chuyang Jing,Xiaowu Wang,Qinggang Wang
A stereoselectivity switchable polymerization of isoprene has been developed, which is catalyzed by iminoimidazole-Co(II) and -Fe(II) complexes. The influence of substituents ranging from electron donating to the electron withdrawing on the iminoimidazole-Co(II) and -Fe(II) catalysts is investigated for isoprene polymerization. Two sets of iminoimidazole-Co(II) and -Fe(II) complexes have been prepared and fully characterized. X-ray crystallography analysis reveals that the complexes Co1 and Fe1 adopt distorted tetrahedral geometries. In the presence of AlEt 2 Cl as co-catalyst, all the Co(II) complexes are active and the catalytic activity is highly dependent on the molar ratio of Al/Co. All the Co(II) complexes exhibit higher activities at low Al/Co ratio. Compared with the Co(II) complexes, the Fe(II) complexes are essentially inactive under the identical condition. However, on activation with combination of AlEtCl 2 and [Ph 3 C][B(C 6 F 5 ) 4 ], both Co(II) and Fe(II) complexes display high activities with good conversions of isoprene (up to >99%). Additionally, low molecular weight and high trans -1,4-unit (>96%) selectivity are characteristics of the resultant polyisoprene. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019 , 57 , 767–775
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WATER RESEARCH
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2019
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IF 7.913
Shuhui Sun,Shu Wang,Yuxuan Ye,Bingcai Pan
Considerable amount of phosphorous is present as organic phosphonates (usually in the form of metal complexes, e.g., Ca(II)-phosphonate) in domestic and industrial effluents , which cannot be effectively removed by traditional processes for phosphate. Herein, we employed a proprietary process, i.e., Fe(III) displacement/UV irradiation/co-precipitation (denoted Fe(III)/UV/NaOH), to enable an efficient removal of Ca(II)-phosphonate complexes from water. The combined process includes three basic steps, i.e., Fe(III) replacement with the complexed Ca(II) to form Fe(III)-phosphonate of high photo-reactivity, UV-mediated degradation of Fe(III)-phosphonate to form phosphate and other intermediates, and the final phosphorous removal via co-precipitation at pH = 6. The operational conditions for the combined process to remove a typical phosphonate Ca(II)-NTMP (nitrilotrismethylenephosphonate) are optimized, where ∼60% NTMP is transformed to phosphate with the total phosphorous reduction from 1.81 mg/L to 0.17 mg/L. Under UV irradiation, the cleavage of NTMP is identified at the C-N and C-P bonds to form the intermediate products and phosphate in sequence. Also, the combined process is employed for treatment of two authentic effluents before and after activated sludge treatment, resulting in the phosphorous drop from 4.3 mg/L to 0.23 mg/L and from 0.90 mg/L to 0.14 mg/L respectively, which is much superior to other processes including Fenton/co-precipitation. In general, the combined process exhibits great potential for efficient removal of phosphonates from contaminated waters .
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Journal of Materials Chemistry A
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2019
·Vol. 7
·期 6
·2845-2854
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IF 10.733
Tianshu Zhang,Jing Wang,Wentao Zhang,Chengyuan Yang,Liang Zhang,Wenxin Zhu,Jing Sun,Guoliang Li,Tao Li,Jianlong Wang
Highly efficient decontamination of naturally occurring As(III) from aqueous media remains a rigorous task for public health and ecosystem protection. As its increasingly acute toxicity and mobile characteristics than those of As(V), it is imperative to exploit a technique for the simultaneous removal and detoxication of As(III). Herein, a novel strategy involving outer and inner structural engineering of an amorphous FeMn-MOF-74 adsorbent was developed via a facile temperature-controlled crystallization method, which integrated the inner amorphous structure with low-coordinated active centers and the outer optimized metal atomic ratio with homogeneous adsorption/oxidation sites for generating the synergistic effects of As(III) removal. An appropriate Fe/Mn ratio (∼1.96) with optimized temperature (denoted as aFMM-120) endows the synergic effect of iron and high-valence manganese nodes in the framework with the highest experimental adsorption capacity of 161.6 mg g−1 among MOF-based arsenic adsorbents. Detailed characterizations through X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy demonstrated the redox behavior of Mn species and surface coordination of oxygen molecules in FeO clusters toward As(III). All these results imply that amorphous aFMM-120 is an effective adsorptive oxidation material for efficient arsenic-contaminated water remediation.
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CHEMOSPHERE
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2019
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IF 5.108
Yufan Chen,Yong Feng,Huaqiang Chu,Deli Wu,Yalei Zhang
Cu(II) enhanced the oxygen activation by Fe(II) to increase the yield of oxidants. However the factors controlling the catalytic performance and indeed the underlying influencing mechanisms remained unclear. Here, we presented the detailed study of Cu(II)-Fe(II) reactions for a range of pH and Cu(II)/Fe(II) ratios. From the results obtained, we provided insight into the factors controlling the redox reactions of Fe-Cu and the catalytic behaviours of active species. A reaction scheme for the Fe(II)/Cu(II) system was developed in which the in-situ formed Cu(I) mainly contributed to producing H 2 O 2 and Fe(II) dominantly decomposed H 2 O 2 to hydroxyl radical (HO ) [see companion article] (Yufan Chen). Circumneutral conditions facilitated the catalytic processes; under acidic conditions, the reverse reaction between Fe(III) and Cu(I) was strongly favoured; alkaline conditions improved the reducing capacity, which subsequently enhanced the generation of Cu(0) instead of Cu(I). There was a saturated Cu(II)/Fe(II) ratio above which further addition of Cu(II) could not be reduced, and then excessive Cu(I) and Cu(II) consumed HO and O 2 – , respectively. Therefore, the highest removal efficiency of organic pollutants was achieved when the stoichiometric Cu(II)/Fe(II) ratio was 60% at circumneutral pH. The new findings have implications for the treatment of mixed wastewater where copper and organic pollutants coexist.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 9
·2282-2290
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IF 5.726
Dawei Zhou,Peixue Wang,Yan Long,Yuqing Fei,Youquan Deng
The thermal cracking behavior of diethyl hexamethylenedicarbamate (EHDC) was investigated in this work. The polymers formed under different conditions were analyzed by IR and TG, indicating that the polymers were mixtures of EHDC, polyureas, imines and others. The polymers could be converted to EHDC by a simple alcoholysis reaction for the first time over Fe–Ni/Al2O3 catalysts. Under the optimized reaction conditions, the yield of EHDC could reach up to 52% with 99% selectivity over 8% Fe–3% Ni/Al2O3 catalysts. The catalysts were extensively characterized by BET, XPS, XRD, SEM, TEM, H2-TPR and NH3-TPD, showing that the interaction effect between Fe species and Ni species may be attributed to high catalytic performance of the catalyst. Meanwhile, the loss of active components resulted in decreased catalytic activity.
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