SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Chengcheng Xu,Jing Deng,Shijun Zhu,Xiao Ling,Songtu Shen,Hongguang Guo,Qiongfang Wang,Xueyan Li
The introduction of ascorbic acid (AA) into Fe(III)/PS system exhibited extremely high activity on the removal of N,N-diethyl- meta -toluamide (DEET) and other pollutants. The removal efficiency of DEET within 30 min reached 90.13%, its dynamic curve obeyed second-order kinetic model and the k obs was calculated to be 0.150 L·mg −1 ·min −1 . Compared with other reducing agents, AA was tested to be the most suitable. The optimal dosages of Fe(III), PS and AA were tested to be 0.1, 1.0 and 0.5 mM, respectively. Furthermore, the introduction of AA extended the working pH to 2.5–9.3. Common anions posed different degrees of inhibition on DEET degradation at relatively high concentration, while a small dosage of HCO 3 − (<1 mM) abnormally exerted a positive role. In terms of reaction mechanism, scavenger experiment and EPR observation illustrated that ·OH and ·SO 4 − dominated DEET degradation, yet slight Fe(Ⅳ) was also found during the reaction, which indicated that Fe(Ⅳ) may also contribute to DEET removal. Different from the rapid consumption of Fe(II) in Fe(II)/PS system, Fe(II) in Fe(III)/PS/AA system entered a dynamic equilibrium state in the later stage of the reaction, which can decompose PS to form ·SO 4 − continuously. Furthermore, the reduction and chelation ability of AA both functioned a key role. According to the degradation intermediates identified by LC-MS analysis, the degradation pathways of DEET could be divided into two directions, which covered opening benzene ring and removing side chain.
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APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Cong Wang,Jingyu Zhao,Congmei Chen,Ping Na
In this study, we compared the differences between bimetallic oxides FeCo 2 O 4 catalyzing the oxidation of phenol by peroxydisulfate (PS) and peroxymonosulfate (PMS) under near neutral and alkaline conditions. Phenol could be completely oxidized and removed in both PMS and PS systems. X-ray photoelectron spectroscopy (XPS) analysis and density functional theory (DFT) calculations showed that there was a synergistic mechanism between Co and Fe on the catalyst surface. Although the PMS-FeCo 2 O 4 system reached the fastest reaction rate of 1.5 × 10 −1 min −1 , it showed a higher oxidants consumption and more residual total organic carbon (TOC) (36%) in solutions after reactions. Quenching experiments and electron paramagnetic resonance (EPR) analysis showed that sulfate radical (SO 4 − ), hydroxyl radical ( OH) and singlet oxygen ( 1 O 2 ) played important roles in the oxidation of phenol in PMS system. While in the PS-FeCo 2 O 4 system, in addition to free radical reactions, the non-radical mechanisms between PS and the catalyst surface played a major role in phenol oxidation, and the soluble organic matter in the PS system could be completely removed. Thus, PS has a better application prospect in the treatment of phenol. This discovery has certain guiding significance for catalyst modification and doping to improve catalyst activity and the choice of oxidant.
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CHEMOSPHERE
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2021
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IF 7.086
Zeyu Wang,Luyao Dai,Jiachao Yao,Tianjiao Guo,Dzmitry Hrynsphan,Savitskaya Tatsiana,Jun Chen
Multi walled carbon nanotubes (MWCNTs) have attracted more and more attention as adsorbents due to their excellent adsorption properties. By loading metal particles on MWCNTs, the chemical reduction ability of adsorbed pollutants could be provided, so as to achieve the purpose of adsorption and degradation of pollutants. Therefore, the removal process of NO 3 − -N by Fe–Pd–Fe 3 O 4 /MWCNTs was studied, including rapid adsorption of initial pollutants, gradual reduction of intermediate products and re-adsorption of final products. The results showed that Fe–Pd–Fe 3 O 4 /MWCNTs completely removed NO 3 − -N within 2 h, 39% and 25% of which were converted into NO 2 − -N and NH 4 + -N. The adsorption efficiency, kinetics, capacity and adsorption energy all followed the order of NH 4 + -N > NO 2 − -N > NO 3 − -N. With the recoverability and reusability of Fe–Pd–Fe 3 O 4 /MWCNTs having been confirmed in 5 consecutive cycles, the removal rate of NO 3 − -N still reached 43%. It has been shown that MWCNTs prolonged the reducing power for NO 3 − -N, due to avoiding the aggregation of metal particles. The rapid adsorption of initial pollutants, effective stepwise reduction and convenient recovery processes were of great value for the rehabilitation of polluted water.
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PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Hongwei Luo,Chenyang Liu,Ying Cheng,Yifeng Zeng,Dongqin He,Xiangliang Pan
The biggest problem with Fe/PMS (peroxymonosulfate) system is the slow generation rate of SO 4 − due to inefficient Fe 3+ /Fe 2+ cycle and the low decomposition efficiency of PMS . Here, we report the Fe 3+ -enhanced decomposition of PMS by a two-dimensional transition metal dichalcogenide WS 2 for pollutant degradation and E. coli disinfection. Experimental results showed that the removal rates of six representative pollutants were all above 90% under various pH conditions. Over a wide range of pH values (2–9), the removal rate of carbamazepine (CBZ) in PMS/WS 2 /Fe 3+ system almost reached 100% within 10 min, and E. coli could be inactivated by 97.3% within 1 min. WS 2 in the system accelerated the Fe 3+ /Fe 2+ cycle and participated in the activation of PMS. Electron paramagnetic resonance (EPR) measurements and scavenging experiments demonstrated that the SO 4 − and HO radicals were the main active oxidative species. The degradation pathway of CBZ was revealed based on its intermediates as determined by liquid chromatograph-mass spectrometer (LC-MS). The presence of common anions such as Cl − and HCO 3 − in PMS/WS 2 /Fe 3+ system noticeably affected the CBZ degradation. The characterization results verified the structural stability and the reusability of WS 2 . These research findings suggest that the combination of Fe 3+ and WS 2 is a promising method for PMS activation to remove organic pollutants and inactivate pathogenic bacteria during the process of wastewater treatment .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Hongbo Lu,Chunli Wang,Xueming Liu,Jing Zhang,Zhang Lin,Zhengping Hao,Gang Pan
Arsenic sulfide sludge (ASS) is a typical precipitation product of acid smelting wastewater. Previous study reported that when exposed to sunlight, the release and oxidation of As(III) in ASS were markedly accelerated. However, the key factor to trigger the photocatalytic transformation of ASS is still unclear. Herein, we revealed that the coexisting Fe(II)/Fe(III) ions were critical to promote the photo-oxidation of released As(III) under visible light. We further validated that Fe(II)-stimulated photo-oxidation mechanism of As(III) in ASS was pH-dependent. In acid conditions, OH and SO 4 − were promoted by Fe(II)/Fe(III) cycling catalysis with the assistance of the reductive sulfur species from ASS, e.g. S 2− and SO 3 2− , and thus accelerated the oxidation of As(III). While in neutral conditions, the nascent ferric hydroxide colloids enhanced the oxidation rate of As(III) via photo-induced ligand-to-metal-charge transfer (LMCT) mechanism. These findings help in predicting and controlling the fate of real arsenic-containing sludge in sunlit environments.
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CERAMICS INTERNATIONAL
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2021
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IF 4.527
Yurun Feng,Xue Guo,Junbin Lu,Jie Liu,Guantong Wang,Hongyu Gong
The SiCN(Fe) fibers with excellent one-dimensional microstructure and electromagnetic wave (EMW) absorption performance were synthesized by combining polymer-derived ceramics (PDCs) method and electrospinning. The in-situ generation of Fe 3 Si and CNTs by adding ferric acetylacetonate (FA) into the raw materials effectively improved the dielectric properties , magnetic properties and the impedance matching performance of the SiCN(Fe) fibers. The EMW absorption performance of SiCN(Fe) fibers were mainly based on dipole polarization loss, interface polarization loss and eddy current loss. The RL min value of SiCN(Fe) fibers reached −47.64 dB at 1.38 mm and the effective absorption band (EAB, RL ≤ −10 dB) reached 4.28 GHz (13.72–18 GHz, 1.35 mm).
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Zhuo-Yu Li,Yu-Lei Liu,Pei-Nan He,Xin Zhang,Lu Wang,Hai-Teng Gu,Hao-Chen Zhang,Jun Ma
Hydroxylamine is commonly known to enhance the performance of Fe(II)-based advanced oxidation processes (AOPs) by promoting Fe(II) regeneration from Fe(III). Recently, ferryl ion (Fe(IV)) was found as an important reactive specie in Fe(II)/peroxydisulfate (PDS) system, while the interaction between hydroxylamine and Fe(IV) in Fe(II)/hydroxylamine/PDS system was still ambiguous. Therefore, the role of hydroxylamine, especially in interaction with reactive species, was systematically studied therein. With methyl phenyl sulfoxide (PMSO) as a probe compound, an original function of hydroxylamine to transform the major reactive species from Fe(IV) to radicals (SO 4 - and OH) for potential pollutants oxidation was clarified. Experimental results combined with Density Functional Theory (DFT) calculations showed that SO 4 - , OH and Fe(IV) all contributed to PMSO oxidation. Hydroxylamine showed the greatest promotional effect on the production of SO 4 - , while the production of Fe(IV) was inhibited with concentrations of hydroxylamine increasing from 0.2 to 1.4 mM. Compared with PMSO, hydroxylamine showed stronger scavenging ability towards Fe(IV) than SO 4 - and OH. Thus, more than 50% of radicals was consumed by PMSO and Fe(IV) mainly reacted with hydroxylamine to regenerate Fe(II). In a word, hydroxylamine played a dual role during potential pollutants oxidation in Fe(II)/hydroxylamine/PDS system, namely (1) transforming the major reactive species from Fe(IV) to radials (SO 4 - and OH) and (2) regenerating Fe(II) from both Fe(IV) and Fe(III). This study provides an insight into the role of hydroxylamine and its interactions with Fe(IV), which advances our understanding on similar Fe(II)/reductants/PDS systems.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Yuzhou Wu,Xubin Zhang,Fumin Wang,Yi Zhai,Xianbao Cui,Guojun Lv,Tao Jiang,Jiaqi Hu
Direct hydroxylation of benzene to phenol is an effective and environment-friendly route to obtain phenol. Herein, Fe-doped and cupric acetylacetonate [Cu(acac)2]-grafted mesoporous silica (Cu/Fe-SBA-15) with highly dispersed metallic sites has been synthesized and used as a heterogeneous catalyst in the hydroxylation of benzene. The physiochemical properties of the synthesized materials as well as the reciprocity between iron and copper sites were analyzed by several characterization techniques including nitrogen adsorption–desorption, X-ray diffraction, transmission electron microscopy, UV–vis diffuse reflectance spectroscopy, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. In direct hydroxylation of benzene with H2O2 as the oxidant, the prepared Cu/Fe-SBA-15 material showed great catalytic activity. Moreover, the synergistic effect between doped Fe sites and grafted Cu sites was also investigated. In this catalyst, Fe and Cu species both played the role of active sites. Excessive activity of iron would lead to benzene peroxidation, while the presence of copper sites could effectively hinder benzene peroxidation.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Yunjin Yao,Huanhuan Hu,Hongda Zheng,Hongwei Hu,Yinghao Tang,Xiaoyan Liu,Shaobin Wang
Bimetallic Fe- and Mo-embedded N-enriched porous biochar (Fe-Mo@N-BC) is developed and serves as a cost-effective and highly efficient catalyst for mineralization of non-biodegradation organic contaminants . Fe-Mo@N-BC was prepared by pyrolysis of complex Fe/Mo -containing precursors. Transmission electron microscopy and elemental mapping suggested that Fe and Mo are uniformly dispersed in nitrogen-doped biochar with hierarchical mesopores . In comparison to Fe@N-BC and Mo@N-BC, Fe-Mo@N-BC exhibited a superior activity for activating peroxymonosulfate (PMS). The stable activity was ascribed to N-doping and synergistic effect of Fe and Mo species, where both Fe-N x and Mo-N x can simultaneously serve as the active sites and N-BC can act as a carrier and an activator as well as an electron mediator. Electron paramagnetic resonance and quenching experiments indicated that H O • , O 2 • − and 1 O 2 were responsible for organic degradation . The effects of PMS dosage, initial Orange II concentration, temperature, solution pH, coexisting anions and humic acids on organic degradation were also investigated. With the assistance of an external magnet, Fe-Mo@N-BC can be easily separated after reaction and remains stable in the reusability tests. This work demonstrates a feasible strategy towards the fabrication of Fe, Mo-embedded N-enriched porous biochar catalysts for the detoxification of organic contaminants.
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Chen Zhe-qin,Zhong Xiao-cong,Xie Yong-min,Liu Jia-ming,Xu Zhi-feng,Wang Rui-xiang
Metal–air batteries have shown tremendous potential as devices for electrical energy storage and conversion; however, their commercial applications are limited owing to the high costs of precious metal catalysts. In this study, urea was employed as a dispersant and as an additional nitrogen source to synthesize zeolitic imidazolate framework-derived iron-nitrogen-carbon catalysts (ZIF-8-derived Fe-NCs). The fabricated nitrogen-rich catalyst was found to have a high specific surface area and numerous surface defects, while maintaining the original ZIF-8 morphology. Electrochemical analysis with a rotating ring-disk electrode revealed that the onset potential of nitrogen-rich Fe-NC was 0.91 V at 1600 rpm with a limiting current density of 5.38 mA·cm −2 , which indicated a high catalytic activity for the oxygen reduction reaction. Additionally, the decent stability of the catalyst was confirmed by a 2 h cycle test.
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高影响因子
ACS Omega
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2021
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IF 3.512
Binbin Jin,Ligang Luo,Longfei Xie
The utilization of CO2, as a cheap and abundant carbon source to produce useful chemicals or fuels, has been regarded as one of the promising ways to reduce CO2 emissions and minimize the green-house effect. Previous studies have demonstrated that CO2 (or HCO3–) can be efficiently reduced to formic acid with metal Fe under hydrothermal conditions without additional hydrogen and any catalyst. However, the pathways and kinetics of the autocatalytic CO2 reduction remain unknown. In the present work, the reaction kinetics were carefully investigated according to the proposed reaction pathways, and a phenomenological kinetic model was developed for the first time. The results showed that the hydrothermal conversion of HCO3– into formic acid with Fe can be expressed as the first-order reaction, and the activation energy of HCO3– is 28 kJ/mol under hydrothermal conditions.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Weifeng Li,Tao Zhang,Li Lv,Yanxiao Chen,Wenxiang Tang,Shengwei Tang
A novel strategy of room-temperature synthesis of MIL-100(Fe) with organic amine as deprotonating agent was proposed. The as-prepared solid product was denoted as R-MIL-100(Fe). The material was systematically characterized via XRD , FT-IR, XPS and SEM. The effects of operation parameters such as initial fluoride concentration, reaction time, initial pH and co-existing anions on the fluoride adsorption performance of the synthesized R-MIL-100(Fe) were studied. The maximum fluoride adsorption capacity of R-MIL-100(Fe) was as high as 23.53 mg/g at 298 K in the fluoride solution. The results indicate that the adsorption process of fluorine on R-MIL-100(Fe) belongs to surface adsorption and intraparticle diffusion . An excellent fluoride adsorption performance of R-MIL-100(Fe) was observed in a wide pH range of 4–10. The co-existing anions including Cl - , NO 3 - and SO 4 2- almost had no negative effects on the adsorption performance of R-MIL-100(Fe). However, the present of CO 3 2- or HCO 3 - brought an obvious reduction of F - adsorption capacity of R-MIL-100(Fe). Thermodynamic study results illustrate that the adsorption process was an exothermic chemisorption . Chemical combination of iron and fluorine was confirmed by FT-IR and XPS. The strong combination brings the excellent F - adsorption performance of MIL-100(Fe). R-MIL-100(Fe) was successfully regenerated and recycled five cycles with an excellent regeneration ability and recyclability.
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