INORGANIC CHEMISTRY COMMUNICATIONS
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2022
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IF 3.428
Zihao Hu,Huiqi Wu,Fang Zhu,Sridhar Komarneni,Jianfeng Ma
MIL-101(Fe)/Co 3 O 4 composites were synthesized using a facile solvothermal method to establish the superiority of a heterogeneous photochemical catalysis system in the presence of Na 2 S 2 O 8 with visible light irradiation. In the present system, the MIL-101(Fe)/Co 3 O 4 catalyst showed better catalytic performance than the single photocatalytic or chemical catalytic system, implying that the MIL-101(Fe)/Co 3 O 4 catalyst can combine both photocatalysis and chemical catalysis well. When tetracycline (TC) is the target pollutant, the highest degradation efficiency can be achieved within 40 min, reaching to 86 %. Crystallinity, morphology, and elemental valence of the MIL-101(Fe)/Co 3 O 4 composite were explored by using X-ray diffraction (XRD), scanning electron microscopy (SEM) as well as X-ray photoelectron spectroscopy (XPS). From the quenching experiments, it was found that 1 O 2 , SO 4 ‾, OH, and O 2 ‾ make contributions to the effective removal of tetracycline. Apart from that, the recovery and reuse characteristics of MIL-101(Fe)/Co 3 O 4 may facilitate the sustainable wastewater treatment.
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International Journal of Applied Ceramic Technology
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2022
·Vol. 20
·期 1
·24-38
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IF 2.328
Cong Zhou,HaiPeng Feng,GuangAo Liu,Feng Tao,Qi Liu
SiFeCO ceramic nanocomposites with porous structure have been successfully prepared via pyrolysis of novel iron-containing precursors, which were synthesized by modification of polycarbosilane with different contents of MIL-101(Fe), a kind of metal-organic framework made by our laboratory. Iron-containing precursors were pyrolyzed at relatively low temperatures ranging from 500 to 900°C under nitrogen atmosphere, the polymer-to-ceramic conversion process were investigated by Fourier transform infrared spectroscopy, X-ray diffraction (XRD), and thermo gravimetric analysis (TGA) measurements. SiFeCO ceramics with different iron contents were intensively studied with respect to their crystallization behavior, microstructure evolution, and porous morphology influenced by additive amount of MIL-101(Fe). The results of XRD and Transmission electron microscopy revealed that MIL-101(Fe)-modified precursors converted into amorphous SiFeCO ceramics when pyrolyzed below 700°C under nitrogen, extremely small Fe 3 O 4 and α-Fe crystallites with grain size of only 2–5 nm were in situ generated and dispersed uniformly in the SiCO ceramic matrix. Simultaneously, interconnected porous structure was created in the matrix by the decomposition of MIL-101(Fe). The as-obtained SiFeCO ceramics could serve as heterogeneous Fenton-like catalysts for the degradation of xylene orange and exhibit outstanding catalytic properties.
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WATER AIR AND SOIL POLLUTION
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2021
·Vol. 232
·期 9
·1-13
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IF 2.52
Li Qiuyue,Huang Kaibo,Duan Xingchun,Liang Jiahao,Chen Xinran,Tao Xueqin,Lu Guining
In this research, the feasibility of UV/Fe(III) photocatalytic technology for the degradation of tris (2-chloroethyl) phosphate (TCEP) was investigated. Experimental results showed that TCEP had a significant removal efficiency in UV/Fe(III) ([TCEP] 0 = 10 ppm, [Fe 2 (SO 4 ) 3 ] 0 = 0.5 mM, near-100% degradation rate after 90 min). A free radical scavenging experiment and EPR detection indicated that the formation of ·OH by the Fe(III) under ultraviolet light played a major role. Experiments on influencing factors revealed that oxygen accelerated the degradation of TCEP by accelerating the Fe(II)/Fe(III) cycle, but Cl − and PO 4 3− inhibited TCEP degradation. Three intermediate products were generated, including C 4 H 9 Cl 2 O 4 P (product A, m/z 222.9690), C 6 H 13 Cl 2 O 5 P (product B, m/z 266.9954), and C 2 H 6 ClO 4 P (product C, m/z 160.9762). Moreover, the degradation pathways primarily involved the C–Cl bond and phosphoric center being attacked. Escherichia coli toxicity test revealed that UV/Fe(III) treatment reduced environmental risk of TCEP. Therefore, UV/Fe(III) photocatalysis is a promising technique for TCEP control in wastewater treatment. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Ahmed Mahmoud Idris,Xinyan Jiang,Jun Tan,Zhenzhi Cai,Xiaodan Lou,Jin Wang,Zhengquan Li
Dye-sensitized system holds great potential for the development of visible-light-responsive photocatalysts not only because it can enhance the light absorption and charge separation efficiency of the systems but also because it can tune the band structure of catalysts. Herein, two-dimensional (2D) Fe-MOF nanosheets (Fe-MNS) with a LUMO potential of 0.11 V ( vs. RHE) was prepared. Interestingly, it has been found that when the 2D Fe-MNS catalyst was functionalized with visible-light-responsive [Ru(bpy)] 3 2+ as a dye-sensitizer, the electrons from the [Ru(bpy)] 3 2+ can effectively inject into the 2D Fe-MNS, which resulted in a negative shift of the LUMO potential of the 2D Fe-MNS to −0.15 V ( vs. RHE). Consequently, the [Ru(bpy)] 3 2+ /Fe-MNS catalytic system exhibits a sound photocatalytic CO 2 -to-CO activity of 1120 μmol g -1 h −1 under visible-light-irradiation. The photocatalytic CO production was further ameliorated by regulating the electronic structure of the 2D Fe-MNS by doping Co ions , achieving a remarkable photocatalytic activity of 1637 μmol g -1 h −1 . This work further supports that the dye-sensitized system is an auspicious strategy worth exploring with different catalysts for the development of visible-light-responsive photocatalytic systems.
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Catalysis Science & Technology
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2021
·Vol. 11
·期 24
·7943-7954
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IF 6.119
Hao Zhang,Xiaojing Song,Hao Sun,Zhenyu Lei,Shouxin Bao,Chen Zhao,Dianwen Hu,Wenxiang Zhang,Jingyao Liu,Mingjun Jia
Developing highly efficient and durable eco-friendly heterogeneous catalysts for the Friedel–Crafts acylation (FCA) reaction has been a long-term and significant target, yet remains a great challenge. Herein, a series of Fe–Ni alloy nanoparticles (NPs) encapsulated inside N-doped carbon spheres (FexNi1−x@NC) was rationally fabricated by pyrolyzing the Fe–Ni bimetallic metal–organic frameworks (BMOFs-FexNi1−x) to this end. Various characterization results demonstrated that FeNi alloy NPs (25 nm) covered by a thin carbon shell (5 nm) were uniformly distributed throughout the entire carbon-based composite. A number of oxidized metal species (Fe3+, Ni2+) are present on the surface of the inner bimetallic core, which should be the main source of catalytically active centers of the carbon-wrapped metal NP catalysts. The composition-optimized Fe0.8Ni0.2@NC with relatively higher positive surface charges exhibited the highest catalytic activity and excellent stability for the acylation of aromatic compounds with acyl chlorides. The density functional theory calculations revealed that the catalytic activity of the FexNi1−x@NC catalysts could arise from the electron transfer, i.e., from the outermost layer of the carbon shell to the inner positively charged Fe-based metal NPs, which can lead to a positive charge distribution (by acting as weak Lewis acid sites) on the external surface of the carbon-encapsulated metal NP catalysts. In this case, the external carbon shell can function as ‘chainmail’ to transfer the Lewis acidity (positive charge), and also to protect the inner metal core from the destructive reaction environment, thus resulting in the formation of highly efficient and durable FCA catalysts.
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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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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2021
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IF 6.789
Zixuan Zhang,Jingfang Li,Yunliang Zhao,Tong Wen,Tingting Zhang,Shaoxian Song
In this work, the iron-containing smectite nontronite (NNT) was artificially prepared by hydrothermal process and used as a heterogeneous catalyst to activate bisulfite (BS) for degradation of tetracycline (TC). Two NNT samples with different iron content (NNT1 and NNT2) were characterized by XRD, FTIR, XPS and SEM-EDS analysis. Under dark condition, the TC removal rates of NNT1/BS and NNT2/BS reached about 91.7% and 95.5% respectively at 60 min. Due to the heterogeneous catalysis of structural Fe(III), the NNT catalysts showed great catalytic activity and low iron leaching at the pH range 3.0–7.5. In addition, NNT particles were also stable and reusable in activating BS for TC removal. According to the EPR and radical quenching experiments, it could be proved that the precursor radical • SO 3 ˉ was first generated in NNT/BS system, then • SO 4 ˉ and • OH were the active species that played a role in TC degradation . The synthetic NNT clay is a promising Fe-based catalyst for treatment of TC wastewater thanks to its high activity, good stability and effective reusability .
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Yuehui Tan,Xirui Wan,Ting Zhou,Le Wang,Xianqiang Yin,Aisheng Ma,Nong Wang
In this study, a novel adsorbent made from kiwi branch biochar modified with Zn-Fe (KB/Zn-Fe) was compared with original biochar to the Pb(II)'s adsorptivity from waste water. The adsorbent was synthetized by liquid-phase deposition. Batches of sorption tests were performed, and the biochars' representative properties were tested. Characterizations revealed the physicochemical properties of biochars and showed that the KB/Zn-Fe composites were successfully synthesized. The Langmuir model and pseudo-second-order kinetic model were proven to satisfactorily fit the original biochar and KB/Zn-Fe. The KB/Zn-Fe showed Langmuir maximum adsorption ability to Pb (II) in aqueous solution of 161.29 mg g -1 , compared with 36.76 mg g -1 for original biochar. The adsorption ability of Pb(II) decreased and the Pb(II) removal efficiency increased with increasing biochar dose. The effect of co-existence of NO 3 - to the absorptive capacity of KB/Zn-Fe on Pb(II) was unremarkable, but Cl - could increase the absorptive capacity. Multiple Pb(II) adsorption mechanisms by KB/Zn-Fe include surface precipitation of metal hydroxides, complexation with active functional groups and ion-exchange. This work provides guidance for future production of biochar with efficient adsorption ability, which could be used to remove Pb(II) ions from wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Shabab Hussain,Xinsheng Peng
Metal organic frameworks (MOFs) based Nanofiltration (NF) membranes have promising advantages in the separation of dyes and salts to purify the industrial polluted water. Herein, we report the synthesis of porphyrinic, porous and ultra-fast photothermal sensitive iron tetrakis(4-carboxyphenyl)porphyrin) (Fe-TCPP) MOFs nanofibers and the corresponding thin film nanocomposite (TFN) membranes by facile interfacial polymerization (IP). The Fe-TCPP nanofibers based TFN membrane enhances the pure water permeance to 28.1 L·m −2 ·h −1 ·bar −1 ( i.e., 3.5-fold higher than thin film composite (TFC)) by providing continuous hydrophilic flow pathways to permeate. The Fe-TCPP nanofibers contribute to the surface of TFN membrane, resulting not only fast permeation, but also ultra-high rejection of dyes i.e., 97.2%, 98.3% and 99.1% for Indocyanine Green, Brilliant Blue-R and Direct Red-80, respectively. Additionally, the TFN membrane also demonstrates 23–43 % salts rejection. Due to the ultra-fast photothermal responsive nature of Fe-TCPP nanofibers (88.4 °C increased temperature in 2 sec photo exposure), the water permeation of TFN NF membrane increases 30 % with 0.5 min under visible light-irradiation. This photo-induced ON/OFF separation is switchable. The enhanced permeation, high dyes rejection and photo-modulated ON/OFF nano-separation opens a new avenue for TCPP-based MOFs in the water purification technologies.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2021
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IF 4.291
Yuliya E. Tyutereva,Petr S. Sherin,Evgeniya V. Polyakova,Vyacheslav P. Grivin,Victor F. Plyusnin,Olga V. Shuvaeva,Jing Xu,Feng Wu,Ivan P. Pozdnyakov
The p-arsanilic acid (p-ASA) is widely used in agriculture as a food additive to control parasites. It leaves the body almost unchanged and is subsequently destroyed by environmental factors with the formation of toxic forms of inorganic arsenic. UVA irradiation of p-ASA with the addition of the Fe(III) oxalate complex leads to an effective photodegradation of the target compound. However, this method needs high concentrations of reagents and the keeping high [oxalate]:[Fe(III)] ratio to maintain proper efficiency of Fe(III) oxalate system. In this work, to overcome these problems, potassium persulfate (PS) was used as an additional oxidizer to improve Fe(III) oxalate system. It was found that the sulfate radical produced upon PS activation reacts readily with both neutral and monoanionic forms of p-ASA yielding corresponding organic cation radical, bimolecular rate constants are (7.3 ± 0.6) × 10 9 and (2.4 ± 0.4) × 10 9 M −1 s −1 , accordingly. Addition of 1 mM of PS reduces to one order (from 1.6 to 0.12 mM) the working concentration of oxalate and allows to achieve the complete degradation of both p-ASA and organic byproducts to inorganic As(V). Also the proposed approach demonstrates high efficiency in a wide range (from <0.5 to 3 ppm) of p-ASA concentrations.
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ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Wenwu Zhou,Yue Liu,Qi Sun,Jianyong Ye,Long Chen,Jia Wang,Guiqin Li,He Lin,Yuanqing Ye,Weifan Chen
A new series of orange highly near-infrared reflective pigments based on Fe-doped La2W2O9 were effectively fabricated via solution combustion synthesis. The acquired pigment powders were characterized by powder X-ray diffraction, scanning electron microscopy, energy dispersive spectroscopy, X-ray photoelectron spectroscopy, ultraviolet–visible–near-infrared spectrophotometry, and CIE 1976 L*a*b* color scales. Then, the energy consumption of the air-conditioning system was simulated based on EnergyPlus software. The results showed that the doping of Fe3+ ions will change the color of the pigment from white to orange. Meanwhile, the band gaps of La2W1.85Fe0.15O9-δ and La2W1.8Fe0.2O9-δ shifted from 3.71 to 3.07 eV and 2.96 eV, respectively. The typical La2W1.85Fe0.15O9-δ pigment powders showed the highest near-infrared reflectance of 89.25% between 700 and 2500 nm and impressive color (L* = 74.20, a* = 22.69, and c* = 22.42). The simulation results illustrated that the homeowner could save $7.32 per month by coating the walls and roofs of the building with the energy-saving paint composed of La2W1.8Fe0.2O9-δ. Excellent chemical stability and high near-infrared reflectance made the synthesized pigments a potential candidate for energy-saving coatings.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Chengbao Liu,Dongchen Shen,Zhengkai Tu,Song Li
Li + doping is regarded as an effective strategy to enhance the room-temperature hydrogen storage of metal-organic frameworks (MOFs). In this work, Li + is doped into both MIL-100(Fe) and MIL-100(Fe)/graphene oxide (GO) composite, and it is demonstrated that the hydrogen uptake of Li + doped MIL-100(Fe)/GO (2.02 wt%) is improved by 135% compared with Li + doped MIL-100(Fe) (0.86 wt%) at 298 K and 50 bar, which is ascribed to its higher isosteric heat of adsorption (7.33 kJ/mol) resulting from its more accessible adsorption sites provided by doped Li + ions and ultramicropores. Grand canonical Monte Carlo (GCMC) simulation reveals that Li + ions distributing in the interface between MIL-100(Fe) and GO within MIL-100(Fe)/GO composite is favorable for hydrogen adsorption owing to the increased number of adsorption sites, thus contributing to the enhanced hydrogen storage capacity. These findings demonstrate that MIL-100(Fe)/GO is a more promising Li + doping substrate than MIL-100(Fe).
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