MICROPOROUS AND MESOPOROUS MATERIALS
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2020
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IF 4.551
Yanshu Luo,Bingqiong Tan,Xianghui Liang,Shuangfeng Wang,Xuenong Gao,Zhengguo Zhang,Yutang Fang
Metal organic frameworks (MOFs) MIL-100(Fe) is considered to be a promising porous adsorbent for dehumidification due to its good hydrophilicity and hydrothermal stability. However, the powdery MIL-100(Fe) prepared by the conventional hydrothermal method is not suitable for industrial rotary desiccant dehumidifier. In order to produce a high-performance rotor core component, a new dry gel conversion in situ synthesis strategy for glass-fiber MIL-100(Fe) monolithic adsorbent was proposed in this paper. The effects of the reaction sol concentration on the crystalline phase, morphology, pore structure , adsorption/desorption performance and the cycling stability of the monolith were discussed in detail. The results showed that MIL-100(Fe) crystals which evenly dispersed in the surface and voids of glass fiber, could be conveniently synthesized in the reaction sols with molar ratios of 1Fe (III)/0.67BTC/xH 2 O (x = 93–185). Among them, the MIL-100(Fe) monolith obtained at x = 93 exhibited a high loading (85.7%), large BET specific surface area (1441 m 2 /g), S-shaped water vapor adsorption isotherm and high saturated adsorption ratio (0.496 g/g) at 298 K and 60% RH , low desorption activation energy (48.28 kJ/mol) as well as a reliable cycling stability. Favorable adsorption/desorption performance of MIL-100(Fe) monolith and convenient dry gel preparation process provide a guidance for the manufacture of high-performance dehumidification rotary wheel.
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Journal of the Taiwan Institute of Chemical Engineers
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2021
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IF 5.876
Wenbo Liu,Jiabin Zhou,Dan Liu,Su Liu,Xianjie Liu,Shuang Xiao,Choujing Feng,Changhong Leng
Background The combination of Fenton catalyst and photocatalyst will lead to the decrease in light absorption on the photocatalyst, and it is difficult for Fe 3+ to be converted into Fe 2+ on the Fenton catalyst, resulting in poor Fenton-like process and photocatalysis effect. Preparing catalysts containing oxygen vacancies (OVs) can simultaneously increase the light absorption and the cycle of Fe(Ⅲ) to Fe(Ⅱ) to improve the catalytic efficiency of Fenton-like process and photocatalysis. Methods A mesoporous H-MIL53 with OV was constructed by ligand selective pyrolysis. The formation mechanism of H-MIL-53 vacancy was analyzed by XPS, EPR, FTIR and TG. Significant findings XPS, EPR, FTIR and TG showed that calcination caused the fracture of Fe-O bond resulted in OV and coordinative unsaturated Fe site. H-MIL-53 showed higher degradation efficiency of tetracycline hydrochloride (93%) and high recycling performance. The electron-rich OV could activate the dissolved oxygen to produce •O 2 − through phot-introduced electrons, while the electron-poor iron site can activate H 2 O 2 to produce •OH. These results provide a new direction for the construction of metal-organic framework (MOF) containing OV for application in Fenton-like process and photocatalysis.
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ENERGY & FUELS
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2021
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IF 3.605
Zenghua Xu,Ximing Zhang,Xufeng Yang,Youfang Yu,Hongjian Lin,Kuichuan Sheng
Corncob, as a sustainable biomass waste, is mainly composed of hemicellulose. Herein, on the basis of natural corncob as substrates, Fe/N co-doped porous carbon spheres were designed via a consecutive FeCl3-mediated hydrothermal reaction and mild KHCO3 activation route for supercapacitor electrode materials. Owing to the low hydrolysis temperature of hemicellulose and hydrolysis promotion of Fe3+, the corncob-derived hydrochar exhibited special carbon sphere morphology. Interestingly, the carbon sphere morphology was well-preserved upon the melamine-mediated KHCO3 activation. As a result of the short ion diffusion distance, unique packing architecture, and developed micro–mesoporous structure of the carbon spheres, optimized CCAC-Fe-M-50% manifested superior ion transfer kinetics and rate performances (87% up to 20 A g–1). Meanwhile, the electrochemical investigation of CCAC-Fe-M-50% in a three-electrode setup illustrated high capacitance (338 F g–1 at 1 A g–1). In a two-electrode setup, the CCAC-Fe-M-50%||CCAC-Fe-M-50% device revealed supreme cyclability (102.7% retention after 5000 cycles) and extremely low Rct (0.59 Ω) and Rs (4.54 Ω). These superior properties were attributed to the large SBET (2305.7 m2 g–1), the multiple redox possibilities (Fe3+, Fe2+, and N functional groups), and the carbon sphere morphology with a micro–mesoporous structure, which enhanced ion physisorption, pseudocapacitance, and electrolyte/ion diffusion, respectively. Besides, the fabricated CCAC-Fe-M-50%||CCAC-Fe-M-50% device in a neutral electrolyte demonstrated a superb energy density (ED) of 18.60 Wh kg–1 at the power density (PD) of 455 W kg–1. The currently presented strategy with superior results might lead to the novel development of biomass-based ultraperformance electrode materials for supercapacitors and other high-tech applications.
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CHINESE CHEMICAL LETTERS
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2021
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IF 6.779
Min Zhang,Bolong Yang,Ting Yang,Yahui Yang,Zhonghua Xiang
Unremitting and intensive researches about efficient non-precious metal electrocatalysts are necessary for large-scale commercial applications of fuel cells, while iron and nitrogen co-doped carbon (Fe-N-C) materials has become one of the most promising electrocatalysts to replace Pt-based noble metal catalysts . However, the traditional Fe-doped ZIF with rhomb dodecahedron morphology limits the exposure of active sites and the utilization of atoms, even affecting the performance of the catalyst. Herein, a Fe/N co-doped catalyst with a flower-like morphology was prepared using ferric citrate source along with secondary NH 3 heat treatment. The optimal catalyst (termed as 4Fe citrate -N-C-3) showed distinguished oxygen reduction reaction (ORR) activity with a half-wave potential of 0.8 and 0.9 V ( vs . RHE) in acid and alkaline media, respectively. In addition, 4Fe citrate -N-C-3 maintained more than 80% of original activity even after 50,000 s which is superior to the benchmark Pt/C. The strategy of controlling morphology and composition is meaningful for the optimization of non-precious metal electrocatalysts for ORR in fuel cells or metal-air batteries .
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MICROCHIMICA ACTA
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2021
·Vol. 188
·期 10
·1-11
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IF 5.833
Qin
Peige,Han Lizhen,Zhang Xiaowan,Li Mengyuan,Li Dan,Lu Minghua,Cai Zongwei
Abstract Using MIL-101(Fe) as the source of carbon and Fe, a magnetic porous carbon (MPC) material with Fe 3 C nanoparticles encapsulated in porous carbon was prepared through one-pot pyrolysis under N 2 atmosphere. With MPC as adsorption material, a stir bar sorptive-dispersive microextraction (SBSDME) method was proposed to extract and preconcentrate sulfonamides (SAs) prior to HPLC-DAD determination. To investigate their extraction ability, different MPC materials were prepared under different carbonization temperatures (600, 700, 800, 900, and 1000 °C). The material prepared under 900 °C (MPC-900) exhibited the highest extraction ability for SAs. The as-prepared MPC materials were also characterized by Raman spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, zeta potential, and other techniques. The main parameters that affect extraction were systematically studied. Under optimal conditions, favorable linearity ( R 2 ≥ 0.9938) and detection limits (0.02–0.04 ng mL −1 ) of sulfonamides were obtained. The average recoveries for spiked milk and lake water samples ranged from 76.9 to 109% and from 75.4 to 118% with RSDs of 3.10–9.63% and 1.71–11.3%, respectively. Sulfameter and sulfisoxazole were detected in milk sample. Sulfisoxazole was detected in the lake water sample. The MPC-900 material demonstrated excellent reusability. It can be reused 24 times with peak areas having no obvious decline. The method can be applied to extract ultra-trace compounds in complex sample matrices. Graphical abstract
Schematic presentation of a stir bar sorptive-dispersive microextraction (SBSDME) by using magnetic porous carbon (MPC) composites as sorbent combined with high-performance liquid chromatography for sensitive analysis of sulfonamides in milk and lake water samples.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Jianan Yu,Zhiliang Zhu,Hua Zhang,Yanling Qiu,Daqiang Yin
Fenton-like catalysis has received much attention as the promising technology for organic pollutant degradation, whereas it suffers from low atomic utilization, poor catalysts durability and difficult after-treatment to hamper the catalytic oxidation activity. Herein, a Fe– and nitrogen-codoped carbon (Fe–N–C) originated from nanocellulose-based hydrochar, nitrogen source, and iron salt precursor was developed for improved PMS activation and identification of exclusive role of each species. The catalyst formed with interconnected bamboo-shaped 3D tubular structures and high Fe-doping level (up to ~9.0 wt%) not only realized excellent efficiencies in oxidative degradation of various aromatic pollutants, but was also endowed with high durability and stability toward PMS activation. Compared with that of the control catalysts only comprising either C–N network or supported Fe nanoparticles (Fe–C) with Fe IV –oxo complex sites, the co-existent active sites of Fe–N configuration and atomic Fe cluster in Fe–N–C could simultaneously improve the graphitization degree, and act as a “support” for constructing the stable structure. It is likely that the coordinated Fe–N formed with annealing process is devoted to decompose PMS by radical generation for pollutants degradation via a radical oxidation process; while the enhanced C–N bonded with graphitic N contribute to produce 1 O 2 through the nonradical processes interacted with PMS. This Fe–N–C/PMS-coupled process provided a designed strategy to construct the highly active and stable metal-nitrogen-codoped hydrothermal carbons, and deepened insights on structure-activity-stability relationship for persulfate-based environmental remediation.
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CHEMOSPHERE
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2021
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IF 7.086
Jian Cheng,Yirui Xie,Ying Wei,Dongrun Xie,Wenbo Sun,Ying Zhang,Menghong Li,Jiutao An
Dielectric barrier discharge (DBD) plasma coupled with Fe–Mn doped AC (Fe–Mn/AC) was used to enhance the degradation of tetracycline hydrochloride (TCH) wastewater. Fe–Mn/AC catalysts with different Fe/Mn molar ratios were prepared by hydrothermal method, and the physical and chemical properties of the samples were explored by different characterization techniques, including XRD, SEM , TEM and XPS. The results showed that the combination of DBD with Fe 2 –Mn 1 /AC system had the highest effect, and the degradation efficiency of TCH could reach 98.8 % after 15 min treatment, which was 25.5 % higher than that of DBD-only. With the increase of discharge voltage and catalyst dosage, the degradation efficiency of TCH promoted. And initial pH had little effect on the degradation of TCH. In the combined system, the Fe 2 –Mn 1 /AC catalyst could retain an excellent stability and reusability. The addition of dimethyl sulfoxide (DMSO) showed that ·OH participated in the TCH degradation. The generated O 3 might be catalyzed by Fe–Mn/AC catalyst to produce more ·OH. And more H 2 O 2 was produced in DBD-only system than that in DBD-catalytic system. Nine main degradation intermediate products in the combined system were detected by HPLC-MS, and three possible degradation pathways were proposed.
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LANGMUIR
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2021
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IF 3.882
Yu Wang,Jia Chen,Ming Guan,Hongdeng Qiu
An iron–nickel bimetallic oxide porous graphene composite material (Fe/Ni-PG) was prepared by a simple partial combustion method, which can be used to effectively remove sulfonamides (SAs) from an aqueous solution. The adsorption performance of Fe/Ni-PG, Fe-PG, and Ni-PG on six kinds of SAs was compared, and the influence of time, temperature, pH, and initial concentration of SAs on the adsorption behavior of SAs of Fe/Ni-PG in an aqueous solution was studied. The adsorption kinetics and thermodynamics exhibited that the Langmuir model and pseudo-second-order kinetics model can describe the adsorption isotherm and kinetics. The maximum adsorption capacities of sulfadiazine (SD), sulfamerazine (SM), sulfamethazine (SDM), sulfathiazole (STZ), sulfapyridine (SPD), and sulfisoxazole (SIZ) calculated by the Langmuir model were 26.3, 50.3, 42.2, 27.3, 34.5, and 41.7 mg/g, respectively, which exceeded those of most reported adsorbents. In the adsorption process, hydrogen bonding, π–π electron donor–acceptor, electrostatic interaction, and bimetallic synergies play a major role, and the entire adsorption process is spontaneously endothermic. In addition, the material has excellent stability, and the Fe/Ni-PG after desorption is consistent with the raw material. This work provides a favorable way for the removal of SAs in the environment.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Dongting Wu,Aiqun Kong,Wei Li,Yan Fu,Jinli Zhang
Bimetallic Ni–Fe phosphide electrocatalysts were in-situ synthesized through direct phosphorization of metal salts on carbon cloth (CC). The Fe dopant remarkably enhances the OER performance of Ni 2 P in alkaline medium through the electronic structure modulation of Ni. The (Fe 0.5 Ni 0.5 ) 2 P/CC electrode, composed of uniform films coated on carbon fibers, delivers a low overpotential of 260 mV with a small Tafel slope of 45 mV·dec −1 at the current density of 100 mA cm −2 , outperforming most reported non-noble electrocatalysts and commercial RuO 2 electrocatalyst. The (Fe 0.5 Ni 0.5 ) 2 P/CC also displays superior electrochemical stability at high current density . An appropriate Fe dopant level facilitates the in-situ transformation of Ni–Fe phosphides into active NiFeOOH during alkaline OER. This work simplifies the synthesis procedure of metal phosphides.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Cheng Zeng,Yan Wang,Tong Xiao,Zhicheng Yan,Jinquan Wan,Quanmo Xie
To improve the efficacy of organic pollutant removal using sulfate radicals, we designed MIP@C-Fe-Nx, a molecularly imprinted material capable of targeting the degradation of tetrabromobisphenol A (TBBPA), which can be used as both adsorbent and catalyst to recognize and degrade Tetrabromobisphenol A (TBBPA) accurately, and the final removal rate of TBBPA can reach 104.6 mg·g −1 . Based on the synergistic effects of MIP@C-Fe-Nx on the excellent organic pollutant recognition and catalytic performance, low concentrations of TBBPA can be pre-targeted, concentrated, and fixed on the surface of MIP, and degraded simultaneously in-situ by·OH and SO 4 •- which are produced by activating PS with C-Fe-Nx. Recognition experiments demonstrated that MIPs had perfect performance in recognizing and adsorbing TBBPA and debromination intermediates. The DFT calculations and HPLC-MS analysis indicated that MIP@C-Fe-Nx had a targeted recognition and accumulation for TBBPA and debromination intermediates, for example, dibromobisphenol A, monobromobisphenol A, and bisphenol A, thus avoid the formation of toxic intermediates causing secondary contamination.
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JOURNAL OF SOLID STATE CHEMISTRY
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2021
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IF 3.498
Falong Wang,Yaqiang Dong,Liang Chang,Yan Pan,Qiang Chi,Mengji Gong,Jiawei Li,Aina He,Xinmin Wang
In this paper, a novel type of nano-CaCO 3 /epoxy nanocomposites insulating layer for the FeSiCr/carbonyl-iron soft magnetic composites (SMCs) has been successfully developed. The novel inorganic/resin nanocomposites can greatly reduce the core loss of the SMCs while maintain other excellent magnetic properties . By optimizing the content of insulating layer, the FeSiCr/carbonyl-iron SMCs exhibits the lowest core loss of 466.5 mW/cm 3 at a maximum magnetic induction of 50 mT and frequency of 100 kHz, which is greatly reduced by 24.2%, compared with the sample only coated by epoxy resin . Meanwhile, the effective permeability and quality factor remains high. In addition, the production process of the novel nano-CaCO 3 /epoxy nanocomposites insulating layer exhibits the advantages of simplicity, convenience and low cost compared with other ceramic coatings (Al 2 O 3 , MgO , SiO 2 , etc.) and surface nitride coatings, which is more suitable for the industrialization of molded inductors, and therefore has a variety of industrial application prospects.
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JOURNAL OF CATALYSIS
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2021
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IF 7.92
Junhui Wang,Shimin Yin,Qinhua Zhang,Fengliang Cao,Yicheng Xing,Qingshan Zhao,Yang Wang,Wengang Xu,Wenting Wu,Mingbo Wu
Polymeric carbon nitride materials show intriguing prospects in numerous light-to-energy conversion applications, but seldom studies focus on their triplet energy transfer, leading to the insufficient lifetime for the photochemical process. Inspired by the porphyrin molecular photocatalyst, single-atom sites (Fe-N 4 ) as triplet sensitizing sites were fabricated in g-C 3 N 4 for the preparation of Fe-g-C 3 N 4 , which processes a long-lived triplet emissive state (τ PH = 4.93 μs). But under realistic condition for the large-scale production of catalyst, single atoms are inevitable to sinter, resulting in the formation of other metal species. Therefore, the photooxidation of 1,5-dihydroxynaphthalene (1,5-DHN) and the photocatalytic E-Z Isomerization of stilbene were selected as the model reactions to evaluate the influence of various Fe species on the triplet energy transfer. It was found that Fe-N 4 sites promote the triplet energy transfer process, while Fe nanoclusters (Fe 0 ) promote the electron transfer and inhibit triplet energy transfer. This finding provides guidance for the rational design of photocatalysts to efficiently improve triplet energy transfer process and its application.
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