SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Dongping Zhang,Yongdi Liu,Yanyu Song,Xianbo Sun,Wen Liu,Jun Duan,Zhengqing Cai
A Fe-doped CeO 2 was fabricated for catalytic ozonation of Amoxicillin (AMX), and the catalytic mechanisms were explored in this study. Under optimal conditions (the initial solution pH of 7.0, FC-0.3 dosage of 0.5 g/L, O 3 dosage of 4 mg/min), the AMX and TOC removal by the optimal material (FC-0.3, at Fe/Ce atomic ratio of 0.3) reached 98.1 % at 24 min and 55.2 % at 36 min, respectively. Improved the AMX mineralization efficiency by 3.7 times. The experiments and theoretical calculation reveal the mechanisms of promoted catalytic ozonation by FC-0.3: 1) Highly abundant surface-active sites (i.e., –OH) enabled the adsorption of H 2 O and O 3 , which was favorable to the generation of reactive oxygen species (ROS) and improved the reaction probability for ROS and contaminants. 2) The synergistic effect between Ce 4+ /Ce 3+ and Fe 3+ /Fe 2+ redox couples accelerated the electron transfer and formation of ROS. More than 42 % of •OH was generated in the presence of FC-0.3, and the •OH, •O 2 − and 1 O 2 were the main ROS that contributed to AMX degradation. The surface OH groups played a key role in the catalytic ozonation. The oxygen vacancies (OVs) played an important role in electron transfer, Ce and Fe were the active sites of electrons transfer following the sequence of (Ce 3+ + Fe 2+ ) → (Ce 4+ + Fe 3+ ) → (Ce 3+ + Fe 2+ ) redox reaction. The degradation pathway investigation and toxicity evaluation revealed that some more toxic intermediates were generated during the ozonation process, and sufficient mineralization is required to meet safe discharge. This study provides reference for the synthesis of new catalysts and insight into the reaction mechanisms in the heterogeneous catalytic ozonation process.
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高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Zibin Pan,Zhengxian Chen,Gary Owens,Zuliang Chen
Biosynthesis strategies are promising methods for the sustainable preparation of nanoparticles because they are less toxic to living organisms and the environment. However, there are still several knowledge gaps concerning the exact mechanisms involved in the biosynthesis of bimetallic composites when used for the removal of arsenic species. Thus, this work focused on the biosynthesis mechanism involved in the formation of a Fe/Cu bimetallic bio-composite (Fe/Cu-OC), and determination of the specific biomolecules in tea extract involved in biosynthesis, and identification of the reactive sites involved in the removal of As(V). FTIR , XPS, GC-MS, and LC-MS analysis of the main components of the tea extract proved that the surface of Fe/Cu-OC contained many different functional groups, including -OH, Fe/Cu-O, and O C-OH, which were mainly associated with theanine and caffeine complexes. SEM and TEM analyses indicated that Fe/Cu-OC had both crystalline and amorphous features with an average particle size of 366 ± 10 nm. A 97 % removal efficiency for As(V) was obtained by Fe/Cu-OC, suggesting that the surface contained numerous reactive sites, including unsaturated Fe and Cu complexes, as well as saturated benzene rings. Moreover, DFT calculations indicated that the Gibbs free energy changes for the preparation of Fe/Cu-OC were < 0, suggesting that in the composites biosynthesis was a thermodynamically favored spontaneous reaction. A biosynthetic mechanism for the formation of Fe/Cu-OC was proposed, involving a series of spontaneous coordination, redox, and organic adsorption reactions.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Yanjing Wang,Minglei Song,Jianrong Wei,Jie You,Siping Chen,Shuangyin Wang,Yanyong Wang
Electrochemically mediated Fe(II)/Fe(III) redox-coupled uranium extraction can efficiently reduce the cell voltage of electrochemical uranium extraction (EUE). How to regulate the surface structure to enhance the uranium acyl ion adsorption capacity and strengthen the Fe(II)/Fe(III) redox cycle process is crucial for EUE. In this work, we developed surface sulfated nanoreduced iron (S-NRI) for EUE and exhibited improved properties for EUE at an ultralow cell voltage (−0.1 V). Compared with a nanoreduced iron (NRI) adsorbent, S-NRI displayed faster electrochemical extraction kinetics properties and higher extraction efficiency and capacity for uranium. In a more complex seawater electrolyte containing uranyl ion concentration ranging from 1 to 20 ppm, the removal efficiency could reach almost ∼100% after EUE for 24 h. At a higher 50 ppm uranium acyl ion concentration in a seawater electrolyte, S-NRI exhibited higher extraction capacity (755.03 mg/g), which is better than 528.53 mg/g of NRI at a cell voltage of −0.1 V. Outstanding EUE property could be attributed to the fact that sulfate species (M–SO42–) on the S-NRI surface not only enhanced selective adsorption of uranyl ions but also strengthened the Fe(II)/Fe(III) redox cycle, which accelerated electron transfer between Fe(II) and U(VI), promoted the regeneration of Fe(II) active sites, and finally enhanced the EUE property.
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PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 9
·092522
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IF 4.386
Jian-Ru Li,Cun-Ying Xu,Jing-Ling Lu,Shu-Xian Wang,Xiao Chen,Qin-Qin Xiang,Yi-Xin Hua
The electrodeposition behavior of Fe was studied in phenyltrimethylammonium chloride-ethylene glycol eutectic-based ionic liquids (TMPAC-EG EILs) containing FeCl2 through electrochemical measurement and the deposit characterization. Some kinetic parameters (standard rate constants, transfer coefficients and activation energy for standard rate constants) as well as transport properties were obtained and discussed as function of temperature. The values of transfer coefficient (0.32–0.39) are significantly lower than conventional value (0.5). Electrodeposition of Fe follows three-dimensional progressive nucleation and growth mode, which is unaffected by temperature. Besides, it is found that deposition temperature plays a central role in controlling surface morphology and structure of the resultant Fe coatings. At low temperature (333–353 K), smooth and dense iron coating can be obtained. The phase structure changes from a nanocrystalline α-Fe to amorphous phase (metallic glass) as the deposition temperature increases from 333 K to 353 K.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Ziyi Xiao,Rui Wu,Tingting Shu,Yingxi Wang,Ling Li
In order to further improve the catalytic performance of MIL-101, cobalt-doped MIL-101(Fe,Co) was synthesized by solvothermal method. By adjusting the ratio of cobalt doping, the MIL-101(Fe,Co 20% ) with the best catalytic activity was obtained. The activation performance of MIL-101(Fe,Co 20% ) for peroxymonosulfate (PMS) was studied using Rhodamine B (RhB) as a pollutant model. The experimental results proved MIL-101(Fe,Co 20% ) with much better catalytic performance than MIL-101(Fe), which can degrade more than 99% of RhB within 15 min. The effects of initial solution pH and coexisting anions in water on the degradation of RhB were further discussed. The results showed that MIL-101(Fe,Co 20% ) was with excellent stability and degradation efficiency can still keep above 90% after five cycles. The free radical quenching experiments were further studied to explore the degradation mechanism. It can be concluded that SO 4 - · was the main active free radical for the degradation of RhB. The possible intermediate products in the degradation process of RhB were analyzed by LC-MS. Combined with the comparison of XPS before and after the reaction, the possible reaction mechanism of RhB degradation process was inferred.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Guolong Lu,Xin Men,Ruoqi Tang,Zhida Wang,Hao Cui,Tongxi Zheng,Mi Wang,Haoqi Yang,Zhenning Liu
Transition metal and nitrogen co-doped carbon electrocatalysts are promising candidates to replace the precious metal platinum (Pt) in oxygen reduction reactions (ORR). Unfortunately, the electrochemical performance of existing electrocatalysts is restricted due to limited accessibility of active sites. Inspired by jellyfish tentacles, we design an efficient ORR micro-reactor called Fe-N x /HC@NWs. It features abundant exposed Fe-N x active sites dispersed on nitrogen-doped cubic carbon cages, which have a hierarchically porous and hairy structure. The accessible, atomically dispersed Fe-N x sites and the elaborate substrate architecture synergize to provide the catalyst withremarkable ORR catalytic activity, extraordinary long-term stability, and favorable methanol tolerance in an alkaline electrolyte ; overall, its performance is comparable to that of commercial carbon-supported Pt. Our synthesis is facile and controllable, paving a new avenue toward advanced non-precious metal-based electrocatalysts for energy storage and conversion .
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高影响因子
Advanced Science
·
2021
·Vol. 8
·期 22
·2101824
·
IF 16.806
Jun Wang,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Wenchao Peng
Fenton-like reactions with persulfates as the oxidants have attracted increasing attentions for the remediation of emerging antibiotic pollutions. However, developing effective activators with outstanding activities and long-term stabilities remains a great challenge in these reactions. Herein, a novel activator is successfully synthesized with single iron atoms anchored on porous N-doped carbon (Fe-N-PC) by a facile chemical vapor deposition (CVD) method. The single Fe atoms are coordinated with four N atoms according to the XANES, and the Fe-N 4 -PC shows enhanced activity for the activation of peroxymonosulfate (PMS) to degrade sulfamethoxazole (SMX). The experiments and density functional theory (DFT) calculations reveal that the introduction of single Fe atoms will regulate the main active sites from graphite N into Fe-N 4 , thus could enhance the stability and tune the PMS activation pathway from non-radical into radical dominated process. In addition, the N atoms connected with single Fe atoms in the Fe-N 4 -C structure can be used to enhance the adsorption of organic molecules on these materials. Therefore, the Fe-N 4 -C here has dual roles for antibiotics adsorption and PMS activation. The CVD synthesized Fe-N 4 -C shows enhanced performance in persulfates based Fenton-like reactions, thus has great potential in the environmental remediation field.
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Chemical Engineering and Processing-Process Intensification
·
2021
·
IF 4.237
Dicka Ar Rahim,Wei Fang,Gaojun Zhu,Haryo Wibowo,Dwi Hantoko,Qing Hu,Herri Susanto,Zengliang Gao,Mi Yan
Before syngas from gasification of biomass could be used as synthesis fuel or chemical feedstock, it requires the removal of hydrogen sulfide (H 2 S) to meet the purity standard level of those applications. In this study, Zn-Fe/Al 2 O 3 were successfully synthesized by a microwave-assisted wet incipient impregnation technique for use as adsorbent for H 2 S removal. The characterization of synthesized adsorbents showed that the oxide form of Zn and Fe present on the surface of adsorbents were zinc oxide (ZnO), magnetite (Fe 3 O 4 ), and zinc ferrite (ZnFe 2 O 4 ). While the reduction of adsorbent was mostly due to that of iron oxide . The reduced adsorbents might consist of ZnO/Fe 3 O 4 /FeO/Fe on alumina as support. At relatively high space velocity (26,000 h −1 ) the adsorbents were able to reduce the H 2 S concentration from 250 ppm at the inlet to around 45 ppm, 35 ppm, and 25 ppm at the outlet by adsorbent 1ZnFe, 2ZnFe, and 3ZnFe; respectively. The removal efficiency for adsorbent 1ZnFe, 2ZnFe, and 3ZnFe were 82%, 86%, and 90%; respectively. Results also shown an increase in adsorbent lifetime with the increase of the Zn to Fe ratio.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2017
·
IF 2.714
Xiaoqin Huang,Yanli Niu,Weihua Hu
Heterogeneous Fenton catalyst with high activity and excellent durability is highly demanded for efficient removal of organic pollutants via well-known Fenton reaction. In this work Fe/Fe 3 C nanoparticles loaded on iron/nitrogen-doped graphene (Fe/Fe 3 C @ Fe/N-Graphene) were synthesized via spontaneous oxidative polymerization of dopamine (DA) on graphene oxide (GO) surface in the presence of iron (III) chloride, followed by thermal annealing. The Fenton catalytic performance of as-prepared Fe/Fe 3 C @ Fe/N-Graphene was evaluated by degrading rhodamine 6G (Rh 6G) as a model organic pollutant. It is found that as-prepared catalyst demonstrates good activity with a rate constant of 0.080 min −1 under optimal hydrogen peroxide (H 2 O 2 ) concentration and catalyst dosage. Moreover, its catalytic activity shows negligible decrease even after 13 successive cycles, exhibiting excellent catalytic durability. The possible mechanism behind the improved Fenton catalytic activity and durability was further discussed.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Xiaolin Shi,Guo Yang,Bo Xing,Caiyi Jiang,Hangdao Qin,Min Li,Fuping Zhang,Yi Wang,Dongzheng Wang,Xingyong Liu
Fluorine-containing wastewater seriously threatens human health due to the wide application of sodium p -perfluorous nonenoxybenzenesulfonate (OBS). Herein, a novel Fe-Co bimetallic biochar (Fe-Co@BC) with abundant pore structure, functional groups and quickly electron transfer capability was prepared using hydrothermal method. Meanwhile, Fe-Co@BC-Ⅰ exhibited a superior catalytic capacity for degradation of OBS in PMS system, and the removal efficiency of OBS reached to 94.1 % within 60 min. After three cycles, the removal efficiency of OBS still up to 80 % and the Fe-Co had almost no leaching (Fe: 0.006 mg/L; Co: 0.023 mg/L). Further mechanistic insights were verified that high catalytic capacity and stability ascribed to the synergistic effects of Fe and Co, where Fe-Co mutual interaction promoted the formation of Fe 2+ and Co 2+ and accelerated electron transfer of catalyst. In addition, the quenching experiments and electron paramagnetic resonance (EPR) proved that the degradation of OBS can be mainly ascribed to indirect oxidation of SO 4 −• , O 2 −• and •OH, and the possible degradation pathway of OBS was proposed in the Fe-Co@BC/PMS system. This study provides an insight into bimetallic prepared and activation PMS degradation fluorinated wastewater.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yanyu Song,Xianbo Sun,Long D. Nghiem,Jun Duan,Wen Liu,Yongdi Liu,Zhengqing Cai
Building a heterojunction is a fascinating option to guarantee sufficient carrier separation and transfer efficiency, but the mechanism of charge migration at the heterojunction interface has not been thoroughly studied. Herein, MIL-53(Fe)/Bi 4 O 5 I 2 photocatalyst with a Z-scheme heterojunction structure is constructed, which achieves efficient photocatalytic decontamination under solar light. Driven by the newly-built internal electric field (IEF), the formation of Fe-O-Bi electron migration channel allows for rapid separation and transfer of charge carriers at the heterojunction interface, confirmed by the material characterization and density functional theory (DFT) calculation. The narrower band gap and improved visible light response also contribute to the enhanced photocatalytic activity of composite materials. With levofloxacin as the target pollutant, the optimal MIL-53(Fe)/Bi 4 O 5 I 2 achieves complete removal of pollutant within 150 min, the photocatalysis rate of which is ca. 4.4 and 26.0 times that of pure Bi 4 O 5 I 2 and MIL-53(Fe), respectively. Simultaneously, the optimal composite material exhibits satisfactory photodegradation of seven fluoroquinolones, and the photocatalysis rates are as follows: lomefloxacin > ciprofloxacin > enrofloxacin > norfloxacin > pefloxacin > levofloxacin > marbofloxacin. DFT calculations reveal a positive relationship between degradation rate and Fukui index (ƒ 0 ) of main carbon atoms in seven fluoroquinolones. This study sheds light on the existence of electron migration channels at Z-scheme heterojunction interface to ensure sufficient photoinduced carrier transfer, and reveals the influence of pollutant structure on photolysis rate.
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Tao Zhao,Dazhong Zhong,Qiang Fang,Xin Zhao,Runxin Du,Genyan Hao,Guang Liu,Jinping Li,Qiang Zhao
The rational design of metal-organic frameworks (MOFs) provides potential opportunities for improving energy conversion efficiency. However, developing efficient MOF-based electrocatalysts remains highly challenging. Herein, a strategy involving strain engineering is developed to promote the electrocatalytic performance of MOFs by optimizing electronic configuration and improving the active site. As expected, the optimized CoFe–BDC NO 2 exhibits a low overpotential of 292 mV at 10 mA cm –2 and a small Tafel slope of 31.6 mV dec –1 as oxygen evolution reaction (OER) electrocatalyst. Notably, when CoFe–BDC NO 2 is prepared on Nickel foam (NF), the overpotential is only 345 mV at 1 A cm –2 , which ensures efficient water oxidation properties. Integrating CoFe–BDC NO 2 /NF anode in membrane electrode assembly (MEA) for overall water splitting and CO 2 reduction reaction (CO 2 RR) tests, the results show that the cell voltages of CoFe–BDC NO 2 /NF are 3.14 and 3.09 V at 300 mA cm –2 (25 °C), respectively, indicating that MOFs have various practical application prospects. The research of the structure-performance relationship reveals the lattice oxygen oxidation mechanism (LOM) where the Co-O-Fe bond is formed during the OER process by changing the electronic environment and coordination structure of CoFe–BDC NO 2 , and with high valence Co as active center, which provides a deep understanding of the structure design of MOFs and their structural transformation during OER.
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