Advanced Science
·
2022
·Vol. 10
·期 2
·2204079
·
IF 17.521
Xu Chen,Ziqi Tian,Qihao Yang,Linjuan Zhang,Qiu Yang,Liang Chen,Zhiyi Lu
The reuse of powdered activated carbon (PAC) vitally determines the economics and security of the PAC-based adsorption process, while state-of-the-art PAC regeneration technologies are usually unsatisfactory. Here, it is demonstrated that isolated Fe sites anchored on commercial PAC enable fast H 2 O 2 activation to produce Fe-based reactive oxygen species for highly efficient PAC regeneration at room temperature. Taking rhodamine B as a representative pollutant, PAC decorated with isolated Fe sites realize H 2 O 2 based regeneration with negligible adsorption capacity degradation for 10 cycles. Moreover, in terms of the PAC loss rate, this technology is greatly superior to traditional Fenton-based regeneration technology. Further operando experiments and theoretical calculations reveal that the high regeneration performance can be attributed to the isolated HO FeO motifs, which activate H 2 O 2 via a nonradical reaction pathway. These findings provide a very promising strategy toward reducing the cost of H 2 O 2 -based PAC regeneration technology.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yan Wu,Tao Liu,Bin Ji,Wei Wang
Iron-cobalt alloy is a potential and economical magnetostrictive material, however, our microscopic understanding of the co-electrodeposition process of Fe-Co alloys is still unsatisfactory. In this work, a flat Fe-Co film with 10 μm was successfully prepared by electrodeposition with a non-toxic sulfate solution. The effects of (NH 4 ) 2 SO 4 , an important additive, were studied and DFT calculation was used to analyze the mechanism of (NH 4 ) 2 SO 4 . EIS shows that (NH 4 ) 2 SO 4 can promote the Fe-Co co-deposition process and obviously inhibits the hydrogen evolution reaction. In addition, (NH 4 ) 2 SO 4 can significantly reduce the internal stress of the Fe-Co film by 110,000 MPa, so that the cracks caused by the internal stress are obviously removed. The results of quantum chemistry calculation further show that NH 4 + is more inclined to adsorb on Fe-Co surface than H 2 O and H + , which reduces the hydrogen evolution on the electrode surface. The results are beneficial to improve the Fe-Co co-deposition process, reduce the internal stress and to prepare a high-performance Fe-Co magnetic film. The films will be assembled on the electronic devices with sensors.
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CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Jie Xue,Ziyu Wang,Andrew Comstock,Zhiyu Wang,Herman H. Y. Sung,Ian D. Williams,Dali Sun,Junwei Liu,Haipeng Lu
Recent discoveries of novel physics in two-dimensional (2D) magnetic materials have sparked the search of new layered magnetic semiconductors. Compared to the traditional inorganic 2D van der Waals crystals, hybrid organic–inorganic metal–halide frameworks offer significantly enhanced chemical and structural versatility, where their optical, electronic, and magnetic properties can be readily modulated with both organic and inorganic components. Here, we reported a series of new Fe–Cl-based layered double perovskites LnMIMIIICl8, [n = 4, L = phenylethylammonium or chiral R-(+)-β-methylphenethylammonium and n = 2, L = 1,4-butanediammonium; MI = Ag/Na; MIII = Fe/In]. UV–vis measurements show that their optical band gaps are highly tunable by varying the organic cations, MI ion, and MIII ion. Magnetic susceptibility measurements suggest an antiferromagnetic coupling between the nearest FeIII–FeIII, where the Curie–Weiss temperature, Néel temperature, and frustration factors can be easily modulated with their compositions and dimensionality. Our study demonstrates the rich and interesting magnetic properties in these layered transition-metal–halide double perovskites and paves the way for design of multifunctional magnetic materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Liwei Yang,Yin Wei,Yaqi Peng,Yang Liu,Zhou Shu,Yansong Wang,Qingli Meng,Chuanliang Zhao,Hongmei Zhao,Fashan Yang,Bo Lai
Aiming at realizing heavy metal recycling and resource utilization, a carbon-based bimetallic material (Fe 1 Co 2 @C) was fabricated via calcining cationic resin exchanged with Fe and Co cations. It exhibited superior peroxymonosulfate (PMS) activation performance to degrade atrazine (ATZ) compared with the monometallic materials (Fe@C and Co@C). Fe 1 Co 2 @C/PMS performed high degradation of 5 mg/L ATZ with the reaction rate constant ( k obs ) of 0.0869 min −1 within 30 min of reaction time. The effects of catalyst loading, PMS dosage, initial pH, and the presence of inorganic ions (NO 3 − , SO 4 2− Cl − , and HCO 3 − ) and natural organic matters (NOMs) were also investigated in this work. According to the radical quenching experiments and electron paramagnetic resonance (EPR), hydroxyl radical ( • OH) and sulfate radical (SO 4 • − ) were identified to be the primary reactive oxygen species (ROS) responsible for the ATZ degradation, especially • OH. What’s more, reaction mechanism of Fe 1 Co 2 @C was demonstrated that −(C− SO 3 ) x − Co(II) and the synergy between Fe and Co on the surface could both promote the heterogeneous redox cycles of Co(II)/Co(III) and Fe(II)/Fe(III) to activate PMS. Based on the detection results of intermediates by LC-MS, possible degradation pathways of ATZ included dealkylation, dichlorination, hydroxylation, and deamination-hydroxylation processes were proposed. This research not only provides new insights of PMS activation by carbon-based bimetallic catalyst for water treatment, but also proposes a new way for reusing the waste saturated cation resin waste with heavy metal.
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RSC Advances
·
2022
·Vol. 12
·期 13
·7935-7940
·
IF 4.036
Aoping Guo,Xiaobao Zhang,Baiyi Shao,Song Sang,Xiaojing Yang
We report an environmentally friendly strategy for the synthesis of Fe3C/Fe/graphitic carbon based on hydrothermal carbonization and graphitization of carbon spheres with potassium ferrate (K2FeO4) at 800 °C. The obtained sample consisting of Fe3C/Fe nanoparticles and graphitic carbon (FC-1-8) delivered an enhanced pseudocapacitance of 428.0 F g−1 at a current density of 1 A g−1. After removal of the Fe3C/Fe electroactive materials, the graphitic carbon (FC-1-8-HCl) possessed a large specific surface area (SSA) up to 2813.6 m2 g−1 with a capacity of 243.3 F g−1 at 1 A g−1, far outweighing the other amorphous carbon electrodes of FC-0-8 (carbon spheres annealed at 800 °C without the treatment of K2FeO4). The graphitic material with a porous structure could offer more electroactive sites and improved conductivity of the sample. This method provided guidelines for the synthesis of superior performance supercapacitors with synchronous graphitic carbon and electroactive species.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 101
·期 6
·3262-3272
·
IF 2.5
Dongmei Jia,Jia Guo,Jing Li,Yongzheng Duan
The composite of CuO coated MIL-101(Fe) (CuO@MIL-101(Fe)) was successfully prepared using a one-pot hydrothermal technology. X-ray diffraction (XRD), Fourier transform infrared spectrum (FTIR), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), Brunauer–Emmett–Teller (BET), and TG technologies were used to characterize its structural, morphological, and physicochemical properties. CuO@MIL-101(Fe) exhibited a better pH adaptivity, a faster removal ratio of 95.8% for glyphosate within 10 min at pH 7, and a higher selectivity of adsorption capacity, even reaching 231.6 and 233.5 mg g −1 with coexisting Cl − (10 mmol L −1 ) and SO 4 2− (10 mmol L −1 ). The enhanced adsorption performances of CuO@MIL-101(Fe) may be caused by Cu forming a coordination interaction with glyphosate. A possible mechanism of glyphosate removal was discussed on the basis of the FTIR and X-ray photoelectron spectroscopy (XPS) analysis. CuO@MIL-101(Fe) composite would be more favourable to capture glyphosate from wastewater.
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MOLECULES
·
2022
·Vol. 27
·期 11
·3497
·
IF 4.927
Xi Li,Huiying Zheng,Jiehan Chen,Mengyuan Xu,Yan Bai,Tiantian Liu
Metal-organic frameworks (MOFs), which have become popular in recent years as excellent carriers of drugs and biomimetic materials, have provided new research ideas for fighting pathogenic bacterial infections. Although various antimicrobial metal ions can be added to MOFs with physical methods, such as impregnation, to inhibit bacterial multiplication, this is inefficient and has many problems, such as an uneven distribution of antimicrobial ions in the MOF and the need for the simultaneous addition of large doses of metal ions. Here, we report on the use of MIL-101(Fe)@Ag with efficient metal-ion release and strong antimicrobial efficiency for co-sterilization. Fe-based MIL-101(Fe) was synthesized, and then Ag+was uniformly introduced into the MOF by the substitution of Ag+for Fe3+. Scanning electron microscopy, powder X-ray diffraction (PXRD) Fourier transform infrared spectroscopy, and thermogravimetric analysis were used to investigate the synthesized MIL-101(Fe)@Ag. The characteristic peaks of MIL-101(Fe) and silver ions could be clearly seen in the PXRD pattern. Comparing the diffraction peaks of the simulated PXRD patterns clearly showed that MIL-101(Fe) was successfully constructed and silver ions were successfully loaded into MIL-101(Fe) to synthesize an MOF with a bimetallic structure, that is, the target product MIL-101(Fe)@Ag. The antibacterial mechanism of the MOF material was also investigated. MIL-101(Fe)@Ag exhibited low cytotoxicity, so it has potential applications in the biological field. Overall, MIL-101(Fe)@Ag is an easily fabricated structurally engineered nanocomposite with broad-spectrum bactericidal activity.Keywords:metal-organic framework;Ag nanoparticles;hybrid nanoagents;antibacterial activity
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Environmental Progress & Sustainable Energy
·
2022
·Vol. 42
·期 2
·e13986
·
IF 2.824
Fengmin Wu,Qinlin Yuan,Xiaowei Wang,Jie Luo,Yakun Song,Weiwei Lu,Hang Xu
Fe-doped ZnO ceramic nanofibers (CNFs) as specific structural features and unique properties synthesized by using electrospun technology. X-ray diffraction disclosed the wurtzite phase, and the microscopy analysis by SEM revealed the formation uniform nanofibers with 400 nm in diameter. The UV–visible diffuse reflectance spectroscopy (DRS) was used to investigation the optical properties of the pristine and the various percentages Fe doped ZnO photocrystalysts. The photo-reduction activities of photocatalyst were evaluated using methylene blue (MB) as organic contaminant irradiated with simulate solar light from xenon lamp. The photocatalytic results that 1% Fe-doped ZnO CNFs exhibits efficient visible and UV light activity and excellent photo-stability. The kinetic constant of MB degradation over 1% Fe-doped ZnO is about 2.2 times higher than that over pure ZnO. The experiment demonstrated that the photodegradation efficiency of Fe-doped ZnO was significantly higher than that of undoped ZnO.
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JOURNAL OF CHROMATOGRAPHY B-ANALYTICAL TECHNOLOGIES IN THE BIOMEDICAL AND LIFE SCIENCES
·
2022
·
IF 3.318
Yunhui Cheng,Shihua Luo,Fuqi Huang,Xiangyi Yang,Maolong Chen,Ye Jiao,Li Wen,Zhou Xu
Soy sauce residue (SSR) is a valuable biological resource, which contains soy isoflavones (SIs) with antioxidant activity and can be used to scavenge radicals. Herein, MIL-100(Fe) was synthesized for the extraction of SIs from SSR. Under the optimal adsorption conditions, the adsorption capacity of MIL-100(Fe) for SIs was 51.81 mg/g, which could achieve a purity of 56.17% and a recovery of 93.8%. These results demonstrated MIL-100(Fe) possessed effective properties of adsorption and purification for SIs. The content of SIs in the purified product was 167 times than that of SSR. The purified total SIs had a good antioxidant activity. The established method had a good scavenging ability toward 2, 2-diphenyl-1-picrylhydrazyl, superoxide and hydroxyl radicals, with IC 50 values of 0.177, 0.116 and 0.082 mg/mL, respectively. Besides, the ferrous ion chelating potency was better than others, with IC 50 values of 0.63 ± 0.0044 mg/mL. The established method was suitable for large-scale separation of purified total SIs and provided a reference for purification of bioactive factors from complex substrates.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Jia Deng,Xiang Zhan,Feng Wu,Shuxian Gao,Li-Zhi Huang
Trichloroethylene (TCE), one of the most frequently detected chlorinated organic pollutants (COPs) in groundwater, has potential risks to human health. The bimetallic system consisting of zero-valent iron (ZVI) and a second catalytic metal has been widely investigated for reductive dechlorination of COPs. However, the passivation layer of ZVI inhibits the electron transfer causing a low dechlorination efficiency. In this work, we designed a novel bimetallic system using Fe(OH) 2 and Ni for fast dechlorination of TCE. The reduction efficiency of TCE reaches 94.8 % after 5 h of reaction in the Fe(OH) 2 /Ni system. TCE was completely dechlorinated to nontoxic gas products including ethylene and ethane, which was attributed to the generation of active hydrogen species (H*) in the system. The Ni 2+ cations undergo the process of hydroxylation and olation. Subsequently, electrons of Fe(OH) 2 were transferred to Ni(II) causing the formation of Ni(0). The catalytic Ni(0) sites generate H* for TCE dechlorination via catalytic reduction of H 2 O/H + . A part of Fe(II) in the Fe hydroxide layer of Fe(OH) 2 was oxidized to Fe(III) leading to the formation of green rust with a hexagonal structure. Our work demonstrates Fe(OH) 2 /Ni is a promising composite material for the remediation of TCE-contaminated groundwater.
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RSC Advances
·
2021
·Vol. 11
·期 17
·9977-9984
·
IF 3.361
Fuhua Wei,Qinhui Ren,Huan Zhang,Lili Yang,Hongliang Chen,Zhao Liang,Ding Chen
Zirconium-iron metal–organic frameworks (Zr/Fe-MOFs) and Zr/Fe-MOF/graphene oxide (GO) composites were prepared via solvothermal synthesis using ferrous sulfate heptahydrate, zirconium acetate, and 1,3,5-benzenetricarboxylic acid. The MOFs and composites were measured using scanning electron microscopy (SEM), infrared spectrometry (IR), and thermogravimetric analysis (TGA). In this study, we explored the ability of Zr/Fe-MOFs and Zr/Fe-MOF/GO composites to adsorb tetracycline hydrochloride from an aqueous solution. Additionally, we optimized the adsorption performance by varying the ratio of MOFs and MOF composites to tetracycline hydrochloride solution, the concentration of tetracycline hydrochloride solution, and the pH of the solution. The results were investigated and fit to both pseudo-first-order and pseudo-second-order kinetic models. The results of the Freundlich and Langmuir isotherm models indicate that Zr/Fe-MOFs and Zr/Fe-MOF/GO composites have heterogeneous adsorption surfaces and that tetracycline hydrochloride is adsorbed over Zr/Fe-MOFs and Zr/Fe-MOF/GO by multilayer adsorption. Overall, our findings indicate that Zr/Fe-MOFs and Zr/Fe-MOF/GO composites can effectively treat wastewater, providing an inexpensive alternative to other methods.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 23
·4726-4734
·
IF 6.331
Wenli Zhao,Guangpu Zhang,Yang Du,Shuangqin Chen,You Fu,Fan Xu,Xiangyun Xiao,Wei Jiang,Qingmin Ji
The proportion of Fe2+ and Fe3+ in Fe-based nanozymes is a key point in determining their catalytic activity. However, it is hard to adjust the Fe2+/Fe3+ ratio in nanozyme systems to achieve the best catalytic performance. In this work, we successfully regulate Fe2+/Fe3+ ratios in a wide range of 0.81–1.45 based on a novel porous platform of Fe doped silica hollow spheres. The homogeneous distribution and stable fixation of Fe components in Fe doped silica hollow spheres facilitate the valence regulation of Fe in the reduction heating in H2/Ar. When the Fe doped spheres (FeOx@SHSs) were used as nanozymes, different Fe2+/Fe3+ ratios have shown to influence the peroxidase-like catalytic activity greatly. The highest activity at the ratio of 1.41 should be due to the combined effects of the accelerated reaction rate by Fe2+ and the enhanced catalytic cycle efficiency by Fe3+. The FeOx@SHSs-based nanozyme is further applied to construct a facile colorimetric biosensing system, which exhibited extremely sensitive determination of glucose. This work presents an effective platform for controlling Fe valences and optimizing the peroxidase-like activity for catalytic processes or sensing systems.
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