Catalysis Science & Technology
·
2019
·Vol. 9
·期 20
·5712-5724
·
IF 5.726
Shuyuan Wang,Dan Xu,Jiaojiao Zhao,Wentao Zheng,Caixia Hu,Xiaodong Wen,Yong Yang,Yongwang Li
Hydrodeoxygenation (HDO) of lignin derivatives offers an effective approach to produce aromatics. In this work, phosphorus (P) modified Fe/SiO2 catalysts were prepared by a stepwise incipient wetness impregnation method. Influences of P on the physicochemical properties of Fe/P–SiO2 catalysts and their catalytic performance for the HDO of anisole were studied. Characterization results revealed that the addition of P into SiO2 reduced the sites for stepwise impregnated Fe species and FeOx particles could be isolated and prevented from aggregating by the optimized contents of P. The reduction of catalysts and the adsorption of H2 were inhibited with increasing the contents of P. In addition, the acidity increased linearly with the P loading pointing to coordinatively unsaturated Fe cations as the Lewis acidic centers in the catalysts. Evaluation results showed that P could tune the distribution of products from aromatics to methyl containing compounds. The aromatics selectivity was promoted to 76.5% with an optimized Fe/P atomic ratio in the 0.5PFS catalyst. Furthermore, an increasing concentration of Lewis acid sites resulted in the methyl transfer reaction (transalkylation). The CH4 selectivity (∼1.55%) was reduced with high contents of P in the catalysts, indicating a significant reduction of carbon loss. These findings provide useful information for the rational design of Fe-based catalysts, which improve the biomass conversion efficiency to platform chemicals.
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JOURNAL OF MEMBRANE SCIENCE
·
2019
·
IF 7.015
Atian Xie,Jiuyun Cui,Jin Yang,Yangyang Chen,Jihui Lang,Chunxiang Li,Yongsheng Yan,Jiangdong Dai
Membrane fouling is one of the major blockages toward the further sustained development of membrane technology . In this work, PVDF/NH 2 -MIL-88B(Fe) (PVDF/NM88B) membranes were prepared for the first time via one-step simple non-solvent induced phase conversion method. The PVDF/NM88B membrane shows an excellent separation performance (above 99.4%) and permeation flux (340–1970 L m −2 h −1 bar −1 ) towards different oil/water emulsions. Moreover, PVDF/NM88B membrane exhibits excellent antifouling performance with flux recovery ratio of almost 100% attributing to hydrophilicity and high photo-Fenton activity of NM88B. In addition, the membrane with good mechanical properties and recyclability shows great application potential in wastewater treatment . This work may shine a new light on the promising photo-Fenton self-cleaning prospect of Fe-based MOFs in constructing antifouling membranes for wastewater remediation and potential applications.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 22
·23162-23172
·
IF 2.914
Yu Jie,Wang Hongjie,Ji Qinghua
In aquatic environment, the existence of antibiotics including sulfadiazine (SDZ) has gain a huge attention. It is suggested that hydrous metal oxides have large potential to remove contaminants in water. The SDZ removal capability by ferric and manganese binary oxides (FMBO) was investigated, and the SDZ removal performance was compared with the ferric hydroxide (HFO) and manganese dioxide (HMO). Our results showed that SDZ removal was highly pH-dependent, but pH has less effect on uptake of SDZ on FMBO than that of the other two adsorbents. The surface acidity constant of FMBO was first calculated to be 6.31 and 8.48, respectively. The uptake process was successfully fitted for according to surface complex formation models (SCFM) and the results of modern surface analytical methods, such as FTIR and XPS, were also consistent with the surface complex uptake mechanism. The uptake of SDZ by FMBO ascribed to specific chemical interaction between the aniline group of SDZ and the hydroxyl groups from FMBO.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 10
·104502
·
IF 3.721
Guofeng Liang,Jilin Huang,Jiawang Li,Yinlong Wu,Guoju Huang,Yan Qi Jin,Hongbin Zeng,Hao Zhang,Jian Chen,Yanshuo Jin,Nan Wang,Fangyan Xie,Hui Meng
Transition metal and nitrogen co-doped carbon-based nanomaterial has been used as non-precious metal catalyst for oxygen reduction reaction (ORR). In this work, bamboo-like carbon nanotubes structured FeCo/N/C electrocatalyst is proved to show much enhanced performance compared with Co/N/C. MIL-53 (Fe) is used as iron source, MIL-53 (Co) is used as cobalt source and ZIF-8 as carbon source. The ball-milling procedure plays a significant role for the distribution of Fe and Co component and the formation of carbon nanotubes, which is believed to enhance the catalytic performance due to abundant electrocatalytic active sites and efficient mass transfer. The as prepared sample obtained by optimized preparation conditions exhibits outstanding ORR activity in acid solution with an onset potential of 0.96 V vs RHE (reversible hydrogen electrode), half-wave potential of 0.78 V, and a current density of 0.575 m A cm−2 at 0.7 V in a H2-O2 fuel cell test, which provides an ideal viewpoint to develop highly efficient catalyst for the oxygen reduction reaction. The high ORR performance could be attributed to the synergistic effect between Fe and Co and the high conductivity and mass transfer of the carbon nanotube.
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HIGH PERFORMANCE POLYMERS
·
2024
·
IF 1.8
Weihua Zhong,Jinwang Bai,Yunjun Luo,Dianbo Zhang,Chen Liang,Xiangdong Chen
Poly(p-phenylene-2,6-benzobisoxazole) (PBO) fiber is currently one of the best-performing organic fibers; however, its low UV aging resistance limits its use. To improve the UV aging performance of PBO fibers, a novel PBO-Fe-PDA fiber was created by depositing a biomimetic structure of polydopamine (PDA) on the surface of PBO fibers with the transition metal ion Fe3+ as the active center. The surface morphology and elemental composition of PBO-Fe-PDA fibers were investigated. It was revealed that Fe3+ formed a coordination bond structure with the oxazole ring, and PDA was successfully loaded onto the surface of PBO-Fe fibers. After UV aging, the crystallinity and crystallographic orientation of PBO fibers significantly decrease, microcrystals inside the fibers slip, and the size of microvoids in the fibers rises. As a result, the strength of PBO fibers was significantly decreased after UV aging. The anti-UV aging capacity of PBO-Fe-PDA fibers, on the other hand, has been enhanced, as evidenced by a slight drop in crystallinity and crystallographic orientation and a significant decrease in the size growth of internal microvoids in the fibers after UV aging. The tensile strength retention of PBO-Fe-PDA fibers after UV aging increased by 93.13% when compared to PBO fibers without altering the fibers’ initial strength. The testing results show that this surface modification method is simple to employ and extends the service life of PBO fibers significantly.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2019
·
IF 3.131
Tong Li,Pei Hu,Jiawei Li,Pintong Huang,Weijun Tong,Changyou Gao
Inspired by natural hemin structure, the fabrication of metal organic framework (MOF) nanomaterials constructed by metal ions and iron porphyrin for peroxidase mimicking has attracted extensive attention recently due to their high concentration of active sites and great channeling for substrate diffusion. Herein, by using benzoic acid as capping agent, we fabricated uniform PCN-224 nanoparticles (NPs), which were composed of Zr 6 cluster and tetrakis(4-carboxyphenyl)porphyrin (H 2 TCPP). Then Fe(Ⅲ) ions were incorporated into the center of H 2 TCPP producing iron porphyrin unit similar to hemin serving as catalytic active site. The procedure of iron incorporation didn't change the size and morphology of PCN-224 NPs. The newly formed Fe@PCN-224 NPs possessed peroxidase-like activity with much lower K m values and higher K cat values than most of peroxidase-like nanozymes as well as natural horseradish peroxidase (HRP), indicating their enhanced catalytic activity. Taking advantage of the excellent peroxidase-like activity of Fe@PCN-224 NPs, we successfully developed a colorimetric method for simple and sensitive detection of hydrogen peroxide and glucose in combination with glucose oxidase .
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CARBOHYDRATE POLYMERS
·
2020
·
IF 7.182
Lumin Chen,Houyong Yu,Christopher Deutschman,Ting Yang,Kam Chiu Tam
We report a facile method to prepare a novel composite based on Fe-Cu alloy decorated cellulose nanocrystals (Fe-Cu@CNC) via simple oxidation-reduction reaction. Spherical zero-valent iron nanoparticles (NZVI) and sheet-like copper nanoparticles were serially anchored on the CNC surface, and the generated composite exhibited excellent antibacterial activities and highly efficient Pb 2+ removal. The composites had high antibacterial ratios of 95.9 %–99.9 %, because superoxide radicals can cause irreversible damage to the bacteria, eventually leading to apoptosis and bacterial death. Meanwhile, the Fe-Cu@CNC composite showed quick Pb 2+ ion removal, reaching a 70.76 % removal within 5 min, a total removal of 93.98 % after 1 h, and excellent reusability (retaining removal efficiency of 80.41 % after six cycles). The adsorption kinetics demonstrated that the adsorption behavior can be described by pseudo-second-order kinetic model (R 2 >0.99). This study offers a new strategy to prepare a promising composite with advanced antibacterial and heavy metal removal properties for wastewater treatment.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 11
·113505
·
IF 4.316
Yapeng Kong,Yu Xiao,Xuemin Liang,Yuran Chen,Liqiang Wang
The availability of casting Ni–Fe alloy as inert anode for direct electro-reduction of V2O3 in molten Na3AlF6-K3AlF6-AlF3 was investigated. The electrochemical oxidation behavior of anode as well as microstructural evolutions of formed oxide scale were systematically studied. The electrochemical characterization and reaction mechanism of the cathode oxide were also investigated to evaluate the influence of alloy anode on cathodic reduction process. The in situ formed three-layered oxide scale is compact and coherent, which is composed of an outermost Fe2O3 + FeAl2O4 skin layer, a Fe2O3 middle layer and a FeAl2O4 inner layer. The skin layer has a continuous, smooth structure and shows electrochemical activity. The Fe2O3 layer with a compact structure prevents inward diffusion of electrolyte and outward migration of metal cations. The innermost FeAl2O4 layer shows a loose structure and functions as a buffer layer to improve the peeling resistance of oxide scale. With the continuous extension of polarization time, the inner FeAl2O4 layer is slowly oxidized and becomes thinner, simultaneously, the dense Fe2O3 layer becomes thicker. Ultimately, metal vanadium product with fine rod-like particles can be obtained and the oxygen content in the metal vanadium is below 0.3 mass% within electrolyzing time of 2 h. The corresponding current efficiency is around 63%.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Weirui Chen,Yixiang Bao,Xukai Li,Jun Huang,Jinxin Xie,Laisheng Li
Heterogeneous catalytic ozonation had met the bottlenecks when treating low concentration but high toxic pollutants: (i) the low mass transfer efficiency of ozone and pollutants to hydrophilic catalyst; (ii) the negative impact of coexisted water matrixes. Herein, to enhance the mass transfer efficiency of reactants toward hydrophilic Fe-MCM-41 as well as enhance the interfacial reaction, the fluoride planting Fe-MCM-41 (F-Fe-MCM-41) was synthesized and employed as catalyst in catalytic ozonation for nitrobenzene (NB). Both NB and TOC removal were promoted in F-Fe-MCM-41/O 3 with 99.0 % NB removal in 60 min and 88.6 % TOC removal in 120 min, which were superior to the degradation efficiency by O 3 and Fe-MCM-41/O 3 . FTIR, EPR, Mössbauer spectra, 29 Si NMR, 19 F NMR et al verified that the replacement of non-reactive silanols (-Si−OH) of Fe-MCM-41 with Si F groups could enhance its hydrophobicity, Lewis acidity and mass transfer effect. Comparative characterizations, experiments and theoretical calculations verified that interfacial reaction played the major role over liquid phase reaction for NB degradation in F-Fe-MCM-41/O 3 . Moreover, the strengthened interfacial reaction also reduced the OH scavenging effect of water matrix, such as humic acid and carbonate. The interfacial adjustment method proposed in this study provided a novel insight into catalyst design and water treatment process.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Lin Zhang,Yibing Sun,Zhichao Yang,Hongchao Li
MoO 2 has been extensively recognized as an efficient cocatalyst in Fe-based Fenton-like systems. However, current understanding has predominantly limited its functional role to that of a reducing agent. This study elucidates a previously unexplored mechanism involving surface interaction-mediated self-sustained Fe redox cycling in MoO 2 -cocatalytic Fe(III)/peroxymonosulfate (PMS) system. Experimental findings demonstrate the formation of multiple reactive species (i.e., free radicals and high-valent iron-oxo species (Fe IV =O), leading to differential degradation efficiencies for various pollutants (i.e., higher than 96.5 % for sulfamethoxazole, phenol, benzoic acid, atrazine, and carbamazepine, and 28.9 % for p -nitrobenzoic acid). Notably, the observed PMS decomposition efficiency exceeds the stoichiometric reduction capacity of MoO 2 , thereby challenging the conventional perception of its sole function as a sacrificial electron donor. Kinetic analyses further reveal that Fe(II), generated via the reduction of Fe(III) by MoO 2 , accounts for less than 27.8 % of the total PMS decomposition. Instead, the surface-adsorbed Fe(III) (Fe(III) sur ) on MoO 2 is identified as the dominant active site for PMS activation, preferentially yielding Fe IV O as the key reactive intermediate. Based on these observations, we propose that MoO 2 not only serves as a reducing agent but, more importantly, might play as a ‘solid ligand’ that regulates the reaction activity and pathway of Fe(III) with PMS. This work provides critical insights into the design of self-sustaining Fenton-like systems for wastewater treatment.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120613
·
IF 7.2
Xiao Feng,Qiqi Gan,Zhongliang Li,Yunhong Zhao,Tengfeng Xie,Dejun Wang,Yanhong Lin
Photocatalysis-coupled advanced oxidation rapidly mineralizes pollutants; here we engineer a Fe-CoS 2 /ZnIn 2 S 4 composite catalyst that activates peroxymonosulfate under visible light to eliminate tetracycline within minutes. The structure, morphology, composition, and optical properties of the photocatalyst were analyzed in detail. Fe-CoS 2 /ZnIn 2 S 4 exhibited markedly improved degradation performance, achieving 88 % TCH removal within 10 min and 94.6 % degradation efficiency within 30 min. The separation and transfer characteristics of photogenerated charges were investigated via surface photovoltage (SPV), transient photovoltage (TPV), photoluminescence (PL) spectroscopy, and UV–visible diffuse reflectance spectroscopy (UV-Vis DRS). Furthermore, the degradation of organic pollutants by sulfate radical-based advanced oxidation processes (SR-AOPs) assisted by photocatalysis was thoroughly studied. The test results demonstrate that the synergistic effects of metal nanoparticle loading and heterojunction construction enable the composite catalyst to achieve efficient photogenerated-carrier separation and rapid Co 3 + /Co 2+ cycling, thereby accelerating PMS activation and generating abundant radicals for pollutant removal. This study offers new insights for developing highly efficient PMS photo-activators for water treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Chiyu Wen,Chao Wang,Defang Liu,Zhuo Cheng,Jing Zhao,Hongli Zhang,Jun Wang,Guoxiang Zhu,Yongfa Zhu
Nitro-aromatic compounds constitute predominant explosive materials extensively utilized in military applications and industrial blasting operations. However, the manufacturing, consumption, and decommissioning of these explosives generate significant quantities of wastewater exhibiting both ecotoxicological hazards and explosive potential. Herein, an amino-functionalized MIL-100(Fe) (AFM) catalyst demonstrating simultaneously enhanced explosive capture and degradation is developed. The synergistic interplay of electrostatic attraction and hydrogen bonding between the amino groups of AFM and nitro groups of nitro-aromatic explosive confer exceptional binding affinity. The optimized AFM exhibits a remarkable 2,4,6-trinitrotoluene (TNT) adsorption of 14.93 mg/g, which is 3.6 times of unmodified MIL-100(Fe). In photo-Fenton reactions, the optimized AFM completely degrades TNT within 30 min, and achieves a mineralization efficiency as high as 96.7 %. Moreover, the AFM exhibits excellent stability, retaining a high TNT degradation efficiency of 97.7 % after five consecutive cycles. The currently designed AFM catalyst possessing fascinating explosive affinity and high explosive mineralization efficiency is expected to advance sustainable remediation of high-risk explosive wastewater.
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