COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
De-Yu Gao,Zan Liu,Zhi-Lin Cheng
The crucial challenge of 2D inorganic nanomaterials-filled composite hydrogel with outstanding mechanical properties was concentrated on the surface modification that was capable to access a better interface between 2D inorganic nanomaterials and hydrogel in past. In this paper, for the first time, we extensively studied the application of as-synthesized 2D Ni-Fe MOF nanosheets with natural organic interface and interlayer structure in PVA hydrogel. The morphology and structure of the as-prepared 2D Ni-Fe MOF/PVA composite hydrogels were determined by a series of characterizations. The results indicated that the as-prepared 2D Ni-Fe MOF/PVA composite hydrogel with porous structure exhibited a desirable dispersion due to the existence of the potential interfacial interaction. Furthermore, the swelling, mechanical and tribological properties of the composite hydrogel were intensively investigated. Dramatically, the tensile strength and compression modulus of the as-prepared 2D Ni-Fe MOF/PVA with 0.1 wt.% filling content were increased by 62.5 % and 113 % relative to pure PVA hydrogel, respectively. Owing to the presence of the interlayer structure of 2D Ni-Fe MOF nanosheets, the friction coefficient of the 2D Ni-Fe/PVA composite hydrogel with 0.15 wt.% filling content was reduced by 41 % compared to pure PVA hydrogel.
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Acta Biomaterialia
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2020
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IF 7.242
Jin He,Ju Fang,Pengbo Wei,Yulei Li,Hui Guo,Qingsong Mei,Fuzeng Ren
Three-dimensional (3D) porous zinc (Zn) with a moderate degradation rate is a promising candidate for biodegradable bone scaffolds. However, fabrication of such scaffolds with adequate mechanical properties remains a challenge. Moreover, the composition, crystallography and microstructure of the in vivo degradation products formed at or near the implant-bone interface are still not precisely known. Here, we have fabricated porous [email protected] scaffolds with skeletons consisting of an inner core layer of Fe and an outer shell layer of Zn using template-assisted electrodeposition technique, and systematically evaluated their porous structure, mechanical properties, degradation mechanism, antibacterial ability and in vitro and in vivo biocompatibility. In situ site-specific focused ion beam micromilling and transmission electron microscopy were used to identify the in vivo degradation products at the nanometer scale. The 3D porous [email protected] scaffolds show similar structure and comparable mechanical properties to human cancellous bone. The degradation rates can be adjusted by varying the layer thickness of Zn and Fe. The antibacterial rates reach over 95% against S. aureus and almost 100% against E. coli . A threshold of released Zn ion concentration (~ 0.3 mM) was found to determine the in vitro biocompatibility. Intense new bone formation and ingrowth were observed despite with a slight inflammatory response. The in vivo degradation products were identified to be equiaxed nanocrystalline zinc oxide with dispersed zinc carbonate. This study not only demonstrates the feasibility of porous [email protected] for biodegradable bone implants, but also provides significant insight into the degradation mechanism of porous Zn in physiological environment.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2020
·Vol. 28
·期 4
·4136-4146
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IF 3.056
Sun Runze,Wang Jie,Peng Yutao,Wang Hongmei,Chen Qing
Arsenic (As) contamination of aquatic and soil environments is a global concern, highlighting the importance of As removal via high-efficiency and low-cost removal technologies. In the present study, novel trimetallic biochar was developed through pyrolyzing corn straw impregnated with inexpensive metal Fe/Al/Zn (hydr)oxides. The results of SEM, FTIR, and XRD verified the formation of metal oxyhydroxides on the surface of the modified biochars, and the modification increased the specific surface area (SSA), total pore volume (TPV), and surface charge of the Fe/Al/Zn (hydr)oxides modified biochar (FAZ-CB). Compared with the original biochar, higher sorption rates and capacities was observed for the FAZ-CB. The maximum As (V) adsorption capacities of FAZ-CB reached 82.9 mg g −1 . A pot experiment showed that application of FAZ-CB decreased bioavailable As fractions in the red soil significantly reduced the uptake of As by arugula in edible part and root (42.6 and 56.8%, respectively). The present study demonstrated the superiority of FAZ-CB in the As(V) immobilization in red soil, suggesting that it is a promising candidate for practical application for As immobilization. Therefore, FAZ-CB can be used as a promising functionalized biochar to remediate As contaminated red soil.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Sijin Zuo,Xuming Jin,Xinwei Wang,Yunhao Lu,Qi Zhu,Jiangwei Wang,Weiping Liu,Yonghua Du,Juan Wang
ABSTRACT Atomically dispersed heterogeneous metal catalysts are promising in dealing with the ever-growing environment and energy issues. However, the practical uses of such catalysts are challenged by the concerns of low reliability and reusability of current compositions under changeable conditions. Here we demonstrate a strategy to stabilize the atomically dispersed Fe catalysts through anchoring the Fe atoms in between a C 3 N 4 -rGO double-layered support. The layered structure is found to significantly prohibit acid leaching and agglomeration of Fe atoms while maintaining activity of the reaction sites, even under extreme pH conditions (pH < 3 or> 11). This allows us to realize high performance Fenton-like reaction via activation of persulfate with unforeseen reactive and recycling abilities over all pH values (0 to 14). This work offers opportunities for understanding the Fenton-like system at extreme reaction conditions, while providing keen insights into the development of stable atomic metal catalysts for practical use.
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CHEMOSPHERE
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2021
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IF 7.086
Liu-Xi Yang,Jia-Cheng E. Yang,Ming-Lai Fu
In this study, porous magnetic CoFe 2 O 4 nanocrystals (NCs) were successfully synthesized by using bimetal-organic framework (MOF) as a precursor, and used as catalysts to activate peroxymonosulfate (PMS) for the removal of chloramphenicol (CAP) in the solution. The structure and physicochemical properties of CoFe 2 O 4 NCs were thoroughly examined by a series of characterization techniques. The results revealed as-synthesized CoFe 2 O 4 had a nanorod-shaped structure with high specific surface area (83.00 m 2 g −1 ) and pore volume (0.31 cm 3 g −1 ). Furthermore, the degradation efficiency (100%) and the removal of total organic carbon (68.09%) were achieved after 120 min with 0.1 g/L CoFe 2 O 4 NCs, 2 mM PMS and 10 mg/L CAP at pH of 8.20. In addition, effects of catalyst dosage, PMS dosage, initial pH values, CAP concentration and co-existing anions as well as natural organic matters in the solution on the degradation efficiencies were studied and all the removal can be well fitted with pseudo-first-order kinetic model (R 2 > 0.96). Sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO•) were proved to be two main reactive species for CAP removal in CoFe 2 O 4 /PMS system based on quenching experiments. CAP was degraded by the main pathways of dichlorination, denitration, decarboxylation , hydroxylation, ring cleavage and chain cleavage on CoFe 2 O 4 /PMS system through high performance liquid chromatograph-mass spectrometry analysis. We believe that this study would be very meaningful to promote the applications of MOFs-derived catalysts on the SO 4 •− based advanced oxidation processes (SR-AOPs) for the environmental remediation.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
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IF 4.464
Cheng Liu,Lei Jin,Jia-Qiang Yang,Fang-Zu Yang,Zhong-Qun Tian
In this paper, the effects of complexing agents (oxalic acid and glycine) and Fe(II) ions on the electro-reduction of Cr(III) ions are studied carefully. Based on the electrochemical analyses, both the complexing agents and Fe(II) ions can obviously decrease the cathodic polarization in the electro-reduction of Cr(III) ions, and the Fe(II) ions can also be co-deposited with Cr(III) ions. One water molecule in [Cr(III)(H 2 O) 6 ] 3+ ion is substituted by one oxalic acid or glycine to form an electrochemically active penta-aqua-Cr(III) coordination ion. In situ infrared spectroscopy and energy dispersive spectroscopy reveal the typical induced-deposition mechanism of ferrochrome alloy. Fe(II) ions are firstly reduced to Fe crystal nuclei, then Cr and Fe atoms grow on the Fe nuclei to form ferrochrome alloy.
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Journal of Materials Chemistry A
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2020
·Vol. 8
·期 33
·17174-17184
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IF 11.301
Jianwei Fan,Xufei Niu,Wei Teng,Peng Zhang,Wei-xian Zhang,Dongyuan Zhao
Catalytic oxidation of formaldehyde (HCHO) is regarded as a promising strategy to eliminate this indoor air pollutant. The design of a highly active and cost-effective catalyst is still pivotal to improve the performance for HCHO oxidation. Herein, we report an Fe–Ce–O solid solution catalyst supported on ordered mesoporous silica (SBA-15) prepared by simple two-step impregnation–calcination, achieving highly efficient HCHO elimination at a low temperature. This strategy brings about the formation of small solid solution nanoparticles (7–12.9 nm) with good dispersion in confined spaces. Meanwhile, the catalysts possess large surface areas (∼500 m2 g−1) and pore volumes (0.5 cm3 g−1) with a pore size of ∼7.5 nm. The results show that Fe content and calcination temperature have great effects on the generation of oxygen vacancies in the catalyst, and further on the catalytic performance. The 20% FeOx-CeOx/SBA-15-350 catalyst displays superior catalytic activity with 65% and 94.9% conversion at 30 °C and 60 °C with a low concentration of HCHO (9.8 μg L−1), respectively, comparable to that for many reported precious metal catalysts. The high ratio of Ce3+ due to the formation of an Fe–Ce–O solid solution and highly dispersed active sites by the spatial confinement is favorable for more oxygen vacancy generation, which mainly contributes to the excellent performance. This work opens up an avenue to design highly efficient non-noble metal nanocatalysts for volatile organic compound (VOC) elimination.
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APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Qing Cheng,Wulin Yang,Qingling Chen,Jiajun Zhu,Deyi Li,Licai Fu,Lingping Zhou
Maintaining a highly negative value of conduction band (CB) potential of photocatalysts through metal doping has been a great challenge. Herein, we investigated the effects of Fe-doping on the crystal structures and electronic structures of zirconia (ZrO 2 ) in detail by combining experiments and Density Functional Theory (DFT). It was revealed that the Fe-doping obviously triggered the formation of tetragonal phase ZrO 2 and induced a defect states in the bandgap of Fe-doped ZrO 2 . Due to the coherent effect between the electrons of the Fe 3 d orbitals and ZrO 2 intrinsic electronic states, the defect states expanded the light absorption edge of ZrO 2 and Fe-doped ZrO 2 showed a small bandgap with maintaining a highly negative value of the CB potential. Meanwhile, Fe-doping significantly enhanced photoelectrochemical properties, the efficiency separation of electron-hole pairs and photocatalytic activity in comparison with the pristine ZrO 2 . We also found that 0.5%Fe-ZrO 2 exhibited the optimum photocatalytic performance, and reached 96% for degradation of Rhodamine B (RhB) within 150 min under visible light irradiation. This work elucidated the mechanism of the photocatalytic degradation of RhB over Fe-doped ZrO 2 and provided a promising approach in designing highly negative CB potential of ZrO 2 via Fe doping toward sustainable environmental remediation.
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Emergent Materials
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2020
·Vol. 3
·期 3
·307-313
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IF 0
Han Yu,Yue Dongting,Zhao Yixin,Qian Xufang
The nano-Fe(0)/mesoporous carbon supported on biochar (MCFe/BC) was synthesized by a co-assembly process followed with carbon thermal reduction method. The specific surface area of MCFe/BC was 582.0 m 2 /g. The highest removal efficiency of pyrene in sand can reach about 40% after 7 h duration on MCFe6.2/BC with 6.2 wt% of iron by the peroxydisulfate advanced oxidation process (PDS-AOP). The removal efficiency of pyrene by adsorption at pH values varied from 4 to 10 in 24 h is around 40%, which shows that adsorption is independent with the pH values, while PDS-AOP is pH dependent, which is more efficient in acidic and basic conditions. The graphitic structure and oxygen-containing groups of carbon materials are benefit for adsorption of PAH. The presence of Nano-Fe(0) is responsible for the activation of peroxydisulfate especially at acidic condition. Our results indicate the potential of PDS-AOP using zero valent iron/porous biochar composite as the activator in practical soil remediation.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Xiang Li,Yan Jia,Minghua Zhou,Xianfa Su,Jianhui Sun
In this study, the Fe, N co-doped biochar (Fe-N-BC) was prepared by pyrolyzing wheat straw, urea and iron salts and used to activate persulfate (peroxydisulfate, PS) for organic contaminant degradation. Iron oxide doping not only introduced magnetism into the biochar for easy separation, but also influenced its catalytic ability for PS activation. In the Fe-N-BC/PS system, almost all acid orange (AO7) was removed within 90 min with an apparent rate constant ( k obs ) of 0.114 min −1 , which was almost 37 times larger than that of pure N-BC (0.003 min −1 ). Factors influencing the removal of AO7 were investigated, including PS concentration, catalyst dosage, and initial pH. The Fe-N-BC/PS system had high removal efficiencies for various organic contaminants and showed high resistance to inorganic anions in aquatic environments. The radical quenching studies, electron paramagnetic resonance (EPR) measurements, and electrochemical analyses verified that the mechanism of AO7 degradation in the Fe-N-BC/PS system included both radical and non-radical pathways involving the generation of OH, SO 4 − , O 2 − , 1 O 2 , and electron transfer. Additionally, persistent free radicals (PFRs) on the catalysts also related to their catalytic efficiencies. These results demonstrated that the Fe-N-BC/PS system had the potential for wastewater treatment applications.
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JOURNAL OF SOLID STATE CHEMISTRY
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2020
·
IF 2.726
Guoqiang Li,Feifei Li,Jianxin Liu,Caimei Fan
The nitrogen activation is the Achilles’ heel of photocatalytic nitrogen fixation . Herein, metal-organic frameworks (MOFs), for first time, are proposed to solve the above bottleneck. A series of Fe-Based MOFs (MIL-101(Fe), MIL-100(Fe), MIL-88(Fe)) demonstrated excellent photocatalytic nitrogen fixation activity. To gain insight into the reaction mechanism, MIL-101(Cr) and MIL-101(Fe), with same molecular structure except the central metal ions , selected for system comparison. Photocatalytic nitrogen fixation activity of MIL-101(Fe) and MIL-101(Cr) are 50.355 μmol L −1 h −1 and inactive, respectively. This suggested that the nitrogen fixation activity originated from the Fe catalytic center. The results of in situ FTIR and quantum computation verifies Fe catalytic center have a higher electron density, a lower reaction activation energy and more generation of N–H bond than those of Cr catalytic center. In view of the analogous outer electron configuration of Cr and Fe, it was suspect that two extra d-orbitals electronics of Fe element are the basic reason of the excellent photocatalytic nitrogen fixation activity. This work provides a new application of MOFs in photocatalytic nitrogen fixation field and emphasizes the vital of d-orbitals electronics during the nitrogen activation process.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Jiajia Zheng,Xinsheng He,Yancheng Li,Biao Zhao,Fengchao Ye,Chunfu Gao,Mengjia Li,Xiping Li,Shiju E
A flaky Fe-based mangetorheological elastomer film (F-Fe/MREF) composite was developed through mixing micron-sized flaky Fe particles into a silicone rubber (SR) matrix by compression molding and vulcanization. The 28 wt % F-Fe/MREF with a thickness of 4.3 mm displays dual resonance peaks with an optimal reflection loss (RL) value of −53.3 dB at 4.8 GHz and an effective frequency bandwidth (RL < −10 dB) reaches 6.0 GHz. Furthermore, anisotropic F-Fe/MREF obtained by assistance of an external magnetic field demonstrates an effective bandwidth of 12.5 GHz in one thickness. This is attributed to the synergistic contributions from magnetic loss and dielectric loss and good impedance matching along with promotion of multiple reflections and scatterings. Besides, an MR effect of 39.2% was obtained for anisotropy F-Fe/MREF because of interaction enhancement between F-Fe particles and the cross-linked matrix. These results suggest that the F-Fe/MREF composites could serve as a potential candidate toward applications of electromagnetic wave absorbing.
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