ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 19
·28525-28537
·
IF 0
Qiu Rui,Chen Aiyin,Zhang Peng,Tang Xuejiao,Wang Cuiping,Sun Hongwen
Herein, novel catalysts of Fe-containing zeolite-A (Fe/zeolite-A) were synthesized by exchanging iron ions into zeolite-A framework, and short-chain organic acids (SCOAs) were employed as chelating agents. Reactive Brilliant Blue KN-R (KN-R) was used as a model pollutant to evaluate the performance of these catalysts based on the heterogeneous Fenton reaction. The results showed that Fe-OA/3A, which applied zeolite-3A as the supporter and oxalic as the chelating agent, presented the most prominent KN-R decolorization efficiency. Under the initial pH of 2.5, 0.4 mM KN-R could be totally decolorized within 20 min. However, the mineralization efficiency of KN-R was only 58.2%. Therefore, anthraquinone dyes were introduced to modify zeolite-3A. As a result, the mineralization efficiency of KN-R was elevated to 92.7% when using Alizarin Violet (AV) as the modifier. Moreover, the modified catalysts exhibited excellent stability, the KN-R decolorization efficiency could be maintained above 95.0% within 20 min after operating for nine cycles. The mechanism revealed that the Fe(II)/Fe(III) cycle was accelerated by AV-modified catalyst thus prompting the KN-R decolorization in Fenton-like system. These findings provide new insights for preparing catalysts with excellent activity and stability for dye wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Qiaoyuan Gao,Dagang Lin,Yongjie Fan,Qin He,Qi Wang
Visible-light-active Fe-2MI assemblies were prepared at room temperature using 2-Methylimidazole (2MI) as organic ligand to form complex with Fe(II) or Fe(III). TGA and XRD characterizations indicated that Fe(II) can form more stable complex and higher coordinating percentage with 2MI relative to Fe(III). Besides, Fe(II)-2MI displayed amorphous state with larger BET surface area and higher photocurrent response. At very low catalyst dosage (0.1 g/L), highest activity for Cr(VI) reduction can be achieved using Fe(II)-2MI as photocatalyst. The estimated pseudo-first-order rate constant (0.021 min −1 ) was 1.4 and 2.1 times that on Fe(III)-2MI and Fe(II)-NaOH, respectively. The well-known ZIF-67 (Co-2MI), ZIF-7 (Zn-2MI) and Fe-MOFs with other organic ligands (H 2 BDC, NH 2 -H 2 BDC or FA) were also used as control samples. Optimal activity for photocatalytic reduction of Cr(VI) was achieved by Fe(II)-2MI. The operating factors was optimized at acidic pH (2.0), higher catalyst dosage (0.3 g/L) and appropriate concentration of coexisting organics (2.0 mM) within the tested range. The stability of Fe(II)-2MI was investigated at different pH values (2, 3 and 4.64), which all displayed good stability. Mechanism study indicated that Fe(II)-2MI has adequate conduction and valence band positions for Cr(VI) reduction and organics oxidation, respectively. Therefore, the as-prepared amorphous Fe(II)-2MI assemblies may be cheap, stable and easy available candidate for the photocatalytic disposal of Cr(VI)-containing wastewaters.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Youyou Feng,Jing Qin,Yu Zhou,Qin Yue,Jing Wei
Nanozyme has been regarded as an efficient antibiotic to kill bacteria using the reactive oxygen species (ROS) generated by Fenton-like reaction. However, its activity is still unsatisfied and requires large amount of hydrogen peroxide with side effects toward normal tissues. Herein, spherical mesoporous Fe-N-C single-atom nanozyme (SAzyme) is designed for antibacterial therapy via photothermal treatment enhanced Fenton-like catalysis process. Due to the large pore size (4.0 nm), high specific surface area (413.9 m 2 g −1 ) and uniform diameter (100 nm), the catalytic performance of Fe-N-C SAzyme is greatly improved. The Michaelis-Menten constant ( K m ) is 4.84 mmol L −1 , which is similar with that of horseradish peroxidase (3.7 mmol L −1 ). Moreover, mesoporous Fe-N-C SAzyme shows high photothermal conversion efficiency (23.3 %) owing to the carbon framework. The catalytic activity can be enhanced under light irradiation due to the elevated reaction temperature. The bacteria can also be killed via physical heat effect. Due to the synergistic effect of nanozyme catalysis and photothermal treatment, the antibacterial performance is much higher than that using single antibacterial method. This work provides an alternative for combined antibacterial treatment via photothermal treatment assisted catalytic process using spherical mesoporous single-atom nanozyme as an antibiotic.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Xin Ding,Waqar Uddin,Hongting Sheng,Peng Li,Yuanxin Du,Manzhou Zhu
Recently, transition metal phosphides (TMPs) have been reported as a new kind of anode catalyst for oxygen evolution reaction (OER), and the composition of the material largely determines the performance of the catalysts. However, few reports explore how electrocatalytic performance of TMPs changed with the composition of the catalysts. We selected three different component Fe-based Prussian blue analogues (PBA) as precursors and transformed them into corresponding metal phosphides by simple heat treatment. By tuning the phosphidation temperature, a series of FeCoP, FeNiP, and FeMnP were obtained, in which FeCoP under a suitable phosphidation temperature at 400 °C exhibits most obviously porous structure and broadest distribution of pore size, which benefits for the mass transfer and oxygen release during OER. Besides, the charge-transfer resistance (R ct ) of TMPs has greatly decreased by introducing of Co in comparison of Ni and Mn, which accelerate the electron transport in OER. Due to the porous geometric structure and unique electronic structure, FeCoP-400 shows excellent and stable electrocatalytic activities of OER in 1 M KOH, with overpotentials of 261 mV at a current density of 10 mA cm −2 , superior to commercial RuO 2 and most OER electrocatalysts . Furthermore, FeCoP-400 exhibits outstanding stability with only 4% increase in potential during 24 h chronopotentiometry.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2022
·
IF 8.91
Xi Li,Xiao Zhang,Shiwen Wang,Peng Yu,Yanhua Xu,Yongjun Sun
To suppress the electron–hole recombination and enhance the electron transfer on carbon nitride , an Fe-doped porous carbon nitride catalyst (Fe/SCN) was synthesized via supramolecular self-assembly method and applied in heterogeneous Fenton activation for efficient tetracycline (TC) degradation. Various characterizations revealed that the catalyst exhibited excellent visible light capture performance and electron transfer capacity . The highest degradation efficiency and mineralization rate of TC (10 mg L −1 ) were achieved under neutral condition (90.3% and 61.2%, respectively) with the leaching of Fe less than 14 μg L −1 . Free radical quenching experiments and spin-resonance spectroscopy characterizations revealed the dominating role of OH in TC degradation, and density functional theory calculation confirmed the formation of Fe-N X and revealed the interaction between Fe sites and H 2 O 2 . Three possible pathways of TC degradation were proposed, and the biological inhibition test revealed the potential of Fe/SCN/H 2 O 2 system to reduce environmental risks caused by TC. This work provides a new insight into the design of metal-doped heterogeneous Fenton catalyst for the efficient degradation of antibiotic contaminants in water.
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ChemCatChem
·
2022
·Vol. 14
·期 13
·e202200253
·
IF 5.497
Mingsheng Luo,Tong Qin,Qinglong Liu,Zhi Yang,Fengli Wang,Hong Li
Graphical Promoting : A series of Fe-modified CeO 2 catalysts with nanoparticle, nanorod, nanocube and nano-octahedron morphologies were synthesized by the hydrothermal method. The Fe-modified CeO 2 nanorod catalysts exhibit a remarkably promoting effect on the formation of DMC from CO 2 and methanol. A series of Fe-modified CeO 2 catalysts with nanoparticle, nanorod, nanocube and nano-octahedron morphologies were synthesized and applied for direct synthesis of dimethyl carbonate (DMC) from CO 2 and methanol. The Fe-modification shows a remarkably promoting effect on the formation of DMC over Fe-modified CeO 2 nanorod. The DMC yield was improved from 0.202 to 2.568 mmol DMC per g cat by 2 %Fe-modification of CeO 2 nanorod. A synergistic effect among the moderate acid-basic sites, specific surface area and surface composition resulted from Fe-modification was proposed to be crucial to obtaining the high reactivity of DMC formation.
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ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Liping Sun,Chao Li,Yong Yan,Yue Yu,Hao Zhao,Zijue Zhou,Feng Wang,Yi Feng
Single atom nanozymes (SAzymes) represent the state-of-the-art technology in nanomaterial-based catalysis, which have attracted attentions in catalysis, cancer treatment, disinfection and biosensing fields. However, numerous SAzymes suffered from low aqueous dispersion and without recognition capacity, which impeded their applications in bioanalysis . Herein, we engineered DNA onto SAzymes to obtain the DNA/SAzymes conjugates , which significantly improved the aqueous dispersion and recognition ability of SAzymes. We synthesized iron SAzymes (Fe–N–C SAzymes) as the catalytic nanomaterials, and investigated the interactions between Fe–N–C SAzymes and DNA. We compared A 15 , T 15 and C 15 adsorption of Fe–N–C SAzymes in HEPES containing 2 mM MgCl 2 . We found that 50 μg mL −1 Fe–N–C SAzymes produced nearly 100% A 15 adsorption, 90% T 15 adsorption and only 69% C 15 adsorption, indicating that adenine and thymine had higher adsorption affinity on Fe–N–C SAzymes. More importantly, DNA modification did not affect the peroxidase-like activity of Fe–N–C SAzymes and the bioactivity of the adsorbed DNA. Taking the advantage of the diblock DNA with one DNA sequence (adenine) binding to Fe–N–C SAzymes and the other DNA sequence (i.e., aptamer) binding to cancer cells, we designed Apt/Fe–N–C SAzymes for colorimetric detection of cancer cells, which offered new insights for the use of SAzymes in biomedicine .
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ChemSusChem
·
2021
·Vol. 14
·期 16
·3382-3390
·
IF 8.928
Ting Feng,Jing Ding,Haiyan Li,Wei Wang,Bohua Dong,Lixin Cao
Graphical In hot water : CeO 2 /A−Fe(OH) 3 composites synthesized by a secondary water bath at 100 °C exhibit superior photocatalytic activity. A−Fe(OH) 3 increases specific surface area, passivates the surface of CeO 2 , and reduces the activation energy of water oxidation. This work provides a new insight into exploring amorphous cocatalysts to enhance photocatalytic O 2 evolution activity and augment the possibility of overall water splitting based on CeO 2 . Noble-metal-free composites with good photocatalytic property are of great interest. Here, CeO 2 nanorods composites loaded with amorphous Fe(OH) 3 cocatalyst were designed and prepared via a secondary water bath at 100 °C. The as-synthesized CeO 2 /amorphous Fe(OH) 3 composites exhibited superior light photocatalytic activities compared to pure CeO 2 , especially the sample with a loading time of 60 min. The photocatalytic oxygen generation rate could reach to 357.2 μmol h −1 g −1 , and the average apparent quantum yield (AQY) was 24.67 %, which was a 5.5-fold increase compared to the CeO 2 sample. The improvement of photocatalytic performance could be ascribed to three main reasons: First, loading the amorphous Fe(OH) 3 enlarged the specific surface area and passivated the surface of the pristine CeO 2 . Second, the amorphous Fe(OH) 3 ,which acted as a cocatalyst, provided many active sites, and reduced the reaction activation energy. Thirdly, the maximum interface with intimate contact between CeO 2 and amorphous Fe(OH) 3 cocatalyst accelerated the photogenerated charge separation efficiency and thus improved the photocatalytic performance of CeO 2 in photocatalytic water oxidation.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Ziyan Du,Jingxi Qin,Kang Zhang,Linwei Jia,Ke Tian,Junfeng Zhang,Haijiao Xie
Single atom catalysts with high-catalytic activity have been applied in many fields. In this work, single Fe atoms (FeSA) showed excellent catalytic performance on P-nitrophenol (PNP) degradation with high total organic carbon (TOC) removal rate and high turnover frequency (TOF). The high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) results show that Fe species in FeSA are mainly single Fe atom. X-ray absorption near-edge structure (XANES) and density functional theory (DFT) calculations show that each single Fe atom is anchored by four N atoms in the form of FeN 4 active site. This coordination environment enables FeSA possesses unique geometric configuration and highly uniform active sites, which is conducive to organic pollutant adsorption and peroxymonosulfate (PMS) activation. In addition, FeSA could maintained excellent catalytic activity in complex water bodies containing different anions and humic acids. The active species in the FeSA/PMS system were also investigated. It is found that the main oxidative active species in the system are O 2 •− and 1 O 2 . This work shows that FeSA was a highly efficient single atom catalyst for the degradation of organic pollutants and has a wide application prospect in advanced oxidation processes.
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RSC Advances
·
2023
·Vol. 13
·期 20
·13902-13910
·
IF 3.9
Jing Tian,Weixin Qian,Haitao Zhang,Hongfang Ma,Weiyong Ying
In this paper, catalysts with different aluminum contents were prepared by a co-precipitation method using LDHs (layered double hydroxides) as the precursors through the adjustment of Cu2+ : Fe2+, and the catalysts were named LDO catalysts. The effect of aluminum on CO2 hydrogenation to methanol was investigated by evaluating the characterization. With the addition of Al, Ar physisorption results showed an increase in BET-specific surface area, TEM demonstrated a decrease in catalyst particle diameter, XRD showed that Cu and Fe existed in the catalyst mainly in the form of CuFe2O4 and CuO, XPS demonstrated a decrease in electron cloud density and an increase in base sites and oxygen vacancies, and CO2-TPD and H2-TPD results indicated that Al promoted the dissociation and adsorption of CO2 and H2. When the reaction temperature was 230 °C, the pressure was 4 MPa, H2/CO2 = 2.5 and the space velocity was 2000 ml (h gcat)−1, the best conversion (14.87%) and the highest methanol selectivity (39.53%) of the catalyst were obtained at 30% aluminum content.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 25
·期 16
·15733-15742
·
IF 2.8
Fu Xiaori,Dionysiou Dionysios D.,Brusseau Mark L.,Zaman Waqas Qamar,Zang Xueke,Lu Shuguang,Qiu Zhaofu,Sui Qian
This study presents a performance comparison of Fe(II)-catalyzed sodium percarbonate (SPC), Fe(II)-EDDS-catalyzed SPC, and of the innovative hydroxylamine hydrochloride (HA)-Fe(II)-EDDS-catalyzed SPC for the degradation of trichloroethylene (TCE) in water. TCE degradation was greater in the Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-catalyzed SPC system, indicating the effectiveness of adding EDDS as an enhancement factor for the removal of TCE. Moreover, TCE degradation was faster in the HA-Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-EDDS-catalyzed SPC system, illustrating that HA can play a synergistic role in TCE degradation. Analysis of iron distribution in the three systems demonstrated that EDDS addition maintained iron in soluble form, and that the generation of soluble ferrous from ferric iron was expedited with addition of HA. Studies using nitrobenzene and carbon tetrachloride probes provided insights on the generation of hydroxyl radical (HO • ) and superoxide anion radical (O 2 •− ) in the three systems. A gradual increasing contribution of O 2 •− to TCE removal in Fe(II)-catalyzed SPC, Fe(II)-EDDS-catalyzed SPC, and HA-Fe(II)-EDDS-catalyzed SPC systems was verified through free-radical scavenger tests. Finally, monitoring of Cl − concentrations manifested the complete dechlorination of TCE. A possible mechanism of TCE degradation involving two pathways of HO • oxidation and O 2 •− reaction was proposed.
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Frontiers in Chemistry
·
2021
·
IF 5.221
Zhang Hui,Zhou Liang,Li Jing,Rong Sijia,Jiang Jianping,Liu Shengquan
Herein, we report a novel carboxymethyl cellulose (CMC)/MIL-101 (Fe)/poly(β-cyclodextrin) (β-CDP) hydrogel with high photocatalytic activity. β-CDP can significantly enhance the photoactivity of MIL-101(Fe) in the hydrogel prepared by a simple solvothermal method. The structure and property of this composite hydrogel were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. Tetracycline was selected as a model pharmaceutical antibiotic to evaluate the photocatalytic activity of the composite hydrogel under visible light irradiation and darkness, respectively. This composite hydrogel shows excellent activity for degrading pharmaceutical antibiotics under visible light irradiation. The increased photocatalytic activity can be attributed to β-CDP, which acts as a promoter and affords an efficient separation of photogenerated electron-hole pairs of MIL-101(Fe). Moreover, the composite hydrogel is shown to have good water retainability. The hydrogel is inexpensive and shows high photocatalytic activity. Hence, it can be used as an efficient photocatalytic material.
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