Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhengheng Yang,Xiaoming Ma,Hongbo Zhou,Jinxing Ma,Yuxin Ding,Di He
For more than a century, coagulation-precipitation using Fe(II) and Fe(III) are ubiquitous in wastewater treatment , however, a systematic understanding of the underlying mechanism and their performance toward chelated heavy metals (e.g. Cu II -EDTA) is still lacking. In this study, we therefore investigate the efficiency of Fe(II) and Fe(III) salts coagulation-precipitation, the properties (coagulation and crystallization behavior) of in-situ formed iron (oxy)hydroxides and explore the reaction mechanism using a suite of characterization techniques. Our results reveal that no matter Fe(II) and Fe(III) exhibited an exceptional removal performance for Cu(II) in terms of kinetics and iron dosage along with pH. Impressively, under optimal condition, over 95 % of chelated Cu(II) was removed within 10 min from Fe(II) while about 85 % from Fe(III) dosing. The highly reductive structural Fe(II) existing on mixed-valent iron bearing mineral results in reductive decomplexation of Cu II -EDTA in the Fe(II) coagulation-precipitation process in compare with replacement decomplexation in the Fe(III) coagulation-precipitation process, and then released free metal ions (Cu(I) and Cu(II)) can be removed by adsorption and coprecipitation . In addition, the in-situ formed Fe(III) (oxy)hydroxides were amorphous 2-line ferrihydrite with stable flocs and better sedimentation behavior than crystalline lepidocrocite from Fe(II) dosing, and these factors are crucial to the subsequent retention of heavy metals. The elucidation of this study has highlighted the great potential of using in-situ formed iron (oxy)hydroxides for cost-effective treatment of chelated heavy metal-bearing industrial wastewaters .
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Environmental Science-Nano
·
2023
·Vol. 10
·期 10
·2744-2753
·
IF 7.3
Jiaxin Lv,Ruixin Chen,Zhen Wu,Yang Bai,Han Song,Chen Tian,Mengye Wang,Zhang Lin
The enrichment of microplastics in polar ice is a typical phenomenon discovered in recent years. Thus, it is worthwhile to explore the degradation behavior of microplastics in frozen environments, which is crucial to evaluate their impact on polar ecosystems. Here, taking polystyrene (PS) as an example, the degradation behaviors of MPs in frozen anoxic Fe(II)-containing solutions were investigated. The results revealed that PS degradation rate in frozen solution was 14.6-fold higher than that in water. Mechanism study showed that freezing-induced aggregation and extrusion of PS enhanced the generation of environmentally persistent free radicals (EPFRs), which in turn contributed to the formation of H2O2. Moreover, freezing-induced enrichment of Fe(II) further interreacted with H2O2 to form Fe(IV) and OH free radicals at a pH of ∼6.5, and thus accelerated the degradation of PS. Such reaction was accompanied by the formation of Fe(III)-containing products, which would further react with aged PS to produce new EPFRs and Fe(II). Such cycles of aged PS/EPFRs and Fe(III)/Fe(II) continued to accelerate the degradation of PS in the frozen solution. This study provides an overlooked pathway for microplastic degradation in frozen Fe(II)-containing solutions, which would be of key importance to understand the degradation behaviors of microplastics in frozen environments.
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WATER RESEARCH
·
2023
·
IF 12.8
Tao Yang,Linqian An,Ge Zeng,Maoju Jiang,Juan Li,Changyu Liu,Jianbo Jia,Jun Ma
The widespread occurrence of p -arsanilic acid ( p -ASA) in natural environments poses big threats to the biosphere due to the generation of toxic inorganic arsenic (i.e., As(III) and As(V), especially As(III) with higher toxicity and mobility). Oxidation of p -ASA or As(III) to As(V) followed by precipitation of total arsenic using Fe-based advanced oxidation processes demonstrated to be a promising approach for the treatment of arsenic contamination. This study for the first time investigated the efficiency and inherent mechanism of p -ASA and As(III) oxidation by Fe(II)/peracetic acid (Fe(II)/PAA) and PAA processes. p -ASA was rapidly degraded by the Fe(II)/PAA process within 20 s at neutral to acidic pHs under different conditions, while it was insignificantly degraded by PAA oxidation alone. Lines of evidence suggested that hydroxyl radicals and organic radicals generated from the homolytic O O bond cleavage of PAA contributed to the degradation of p -ASA in the Fe(II)/PAA process. p -ASA was mainly oxidized to As (V), NH 4 + , and p -aminophenol by the Fe(II)/PAA process, wherein the aniline group and its para position were the most vulnerable sites. As(III) of concern was likely generated as an intermediate during p -ASA oxidation and it could be readily oxidized to As(V) by the Fe(II)/PAA process as well as PAA alone. The in-depth investigation demonstrated that PAA alone was effective in the oxidation of As(III) under varied conditions with a stoichiometric molar ratio of 1:1. Efficient removal (> 80%) of total arsenic during p -ASA oxidation by Fe(II)/PAA process or during As(III) oxidation by PAA process with additional Fe(III) in synthetic or real waters were observed, mainly due to the adsorptive interactions of amorphous ferric (oxy)hydroxide precipitates. This study systematically investigates the oxidation of p -ASA and As(III) by the Fe(II)/PAA and PAA processes, which is instructive for the future development of arsenic remediation technology.
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Sustainable Energy & Fuels
·
2019
·Vol. 3
·期 12
·3455-3461
·
IF 4.912
Bomin Feng,Xiuju Wu,Yanli Niu,Wei Li,Yunxi Yao,Weihua Hu,Chang Ming Li
Fe/N–C catalysts show great potential for the oxygen reduction reaction (ORR) but their catalytic activity should be further improved for practical application. Here, we report a high performance Fe/N–C hollow sphere with excellent ORR activity in both alkaline and acidic solutions. It is synthesized via pyrolysis of a melamine/Fe-incorporated polydopamine nanosphere precursor at 800 °C in an argon atmosphere. The N-rich melamine in the precursor affords abundant N dopants to form dense Fe–Nx active sites and also facilitates the formation of micropores in the catalyst via the gasification effect, together improving the ORR activity. The as-reported Fe/N–C catalyst outperforms the Pt/C catalyst in basic media (45 mV more positive half wave potential), approaches the Pt/C catalyst in acidic media (55 mV lower half wave potential), and exhibits impressive performance in Zn–air primary batteries.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Yanan Wei,Bingfeng Wang,Xinfang Cui,Yaseen Muhammad,Yanjuan Zhang,Zuqiang Huang,Xuesheng Li,Zhenxia Zhao,Zhongxing Zhao
MIL(Fe)/Fe-doped nanospongy porous biocarbon (Fe-SPC) composite was fabricated from MIL-100(Fe) via in situ growth on a unique Fe-doped nanospongy porous biocarbon (Fe-SPC) and was used as Fenton-like catalyst for advanced degradation of thiamethoxam (THIA). Fe was loaded on silkworm excrement and calcined to Fe-SPC with nanospongy and high sp2 C structure. The in situ growth strategy embedded the Fe-SPC into MIL-100(Fe) crystals and formed conductive heterojunctions with an intensified interface by Fe-bridging effect, which was confirmed by negative shift of Fe3+ binding energy in X-ray photoelectron spectroscopy. MIL(Fe)/Fe-SPC composites exhibited high degree of crystallinity and surface area (Brunauer–Emmett–Teller: 1730 m2/g). Liquid chromatography–mass spectrometry and density functional theory simulations demonstrated that THIA was converted to a relatively stable compound (C4H5N2SCl), which could be captured by MIL-100(Fe) with strong chemical bonding energy (Fe–N, −587 kJ/mol), followed by a significant geometric distortion, resulting in a thorough degradation. Efficient charge separation and synergistic chemisorption-catalysis strategy resulted in the high catalytic activity of MIL(Fe)/Fe-SPC. The composite catalyst concurrently exhibited high mineralization ratio with 95.4% total organic carbon removal (at 25 °C and 180 min) and good recycling ability under wider neutral/alkaline conditions. Endorsing to these intriguing properties, MIL(Fe)/Fe-SPC can be deemed an efficient contender for removal of hard-degradable pesticides and other environmental pollutants in practical applications.
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MOLECULES
·
2024
·Vol. 29
·期 9
·2078
·
IF 4.2
Yu Cao,Zeming Dai,Xuan Zhou,Yuting Lin,Jianhua Hou
The dyes in printing and dyeing wastewater are harmful to the human body and the environment. It is essential to develop practical and effective adsorbents to deal with them. In this study, an Fe-doped, ZIF-67 derived Fe/Co/C composite material with strong magnetism was successfully synthesized. The effects of pH, initial concentration, and adsorption time on the properties of the adsorbent were investigated. To further improve the removal efficiency and enhance the practicality, potassium peroxymonosulfate (PMS) was added to the system due to its Fenton-like effect. Then, an Fe/Co/C composite was used with PMS to remove Congo red (CR) with a 98% removal of 250 mg·L−1. Moreover, for its high saturation magnetization of 85.4 emu·g−1, the Fe/Co/C composite can be easily recovered by applying a magnetic field, solving the problem that powdery functional materials are difficult to recover and, thus, avoiding secondary pollution. Furthermore, since the composite material was doped before carbonization, this synthetic strategy is flexible and the required metal elements can be added at will to achieve different purposes. This study demonstrates that this Fe-doped, ZIF-67 derived magnetic material has potential application prospects for dye adsorption.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Xing Cao,Qianxi Dang,Huanhui Chen,Yubin Zhao,Ya Liu,Junrong Zeng,Qing Ma,Liubiao Zhong,Dayou Wang,Yejun Qiu
To address the severe carrier recombination in BiVO 4 -based Photoelectrochemical (PEC) water splitting, we developed Fe-doped Ni nanocrystals (Fe:Ni NCs) through an organic liquid phase synthesis as an efficient cocatalyst. Through a dip-coating and annealing modification process, the optimized Fe:Ni/BiVO 4 photoanode achieved a remarkable photocurrent density of 4.72 mA/cm 2 at 1.23 V vs. RHE, representing a 4.07-fold enhancement over pristine BiVO 4 . In-situ Raman characterization revealed that Fe:Ni NCs on BiVO 4 underwent in-situ surface reconstruction to form a unique Fe:Ni@Fe:NiOOH core–shell structure during PEC reaction. The presence of Fe accelerated the conversion of Ni to active NiOOH at lower potential (0.25 V vs. RHE) compared to pure Ni NCs modified BiVO 4 photoanode (0.30 V vs. RHE). Mechanistic studies identified a dual activation pathway involving both applied potential and BiVO 4 valence band oxidation. Meanwhile, Fe:Ni NCs cores with high conductivity accelerated the migration and accumulation of holes into Fe:NiOOH shells, resulting in improved carrier injection efficiency and water oxidation kinetics. This work not only elucidates fundamental differences between PEC and electrocatalytic water splitting mechanisms but also provides a reference for designing high-performance PEC photoanodes.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Feng Cheng,Peng Zhou,Yang Liu,Xiaowei Huo,Jian Zhang,Yue Yuan,Heng Zhang,Bo Lai,Yongli Zhang
Slow reduction of Fe(III) in iron-mediated Fenton-like systems strongly limits the decomposition of H 2 O 2 to produce hydroxyl radicals ( • OH). Here, we report that graphene oxide (GO) possesses excellent reactivity to enhance the Fe(III)/H 2 O 2 Fenton and photo-Fenton oxidation for degrading chloramphenicol (CAP). EPR analysis and quenching tests reveal that • OH is the primary oxidant for CAP degradation. The characterization analysis and iron species transformation experiments demonstrate that Fe(III) can combine with the functional groups on the GO surface to form GO-Fe(III) complexes. The chronopotentiometry and cyclic voltammogram suggest that GO can donate electrons to Fe(III) via intramolecular electron transfer and promote H 2 O 2 induced Fe(III) reduction by increasing the oxidation capability of Fe(III) due to the formation of GO-Fe(III) complexes, resulting in the strong promotion of the Fe(III)/Fe(II) cycle for producing OH. Moreover, the dark- and vis-GO/Fe(III)/H 2 O 2 systems can effectively degrade CAP at initial pH ranging from 2.0 to 4.7. The reusability and stability of GO were evaluated by performing the cyclic degradation experiments of CAP. The OH induced degradation pathway of CAP was proposed involving three stages, based on intermediates analysis of UPLC-QTOF-MS/MS system. Therefore, the GO/Fe(III)/H 2 O 2 system with or without visible light shows high potential for application in environmental remediation.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Xiang Li,Erbiao Cui,Zhen Xiang,Lunzhou Yu,Juan Xiong,Fei Pan,Wei Lu
Electromagnetic (EM) wave absorbing materials have been extensively applied in the electronic devices and wireless communication to solve the increasingly serious problems of electromagnetic pollution and radiation. In this work, Fe-MOFs/biomass cotton derived Fe@nanoporous carbon@carbon fiber (Fe@NPC@CF) composites were successfully obtained by means of in-situ synthesis and thermal decomposition processes. It was found that the Fe@NPC composites were uniformly distributed on the carbon fibers matrix. As a result, EM wave absorbing performances were greatly promoted via the synergic effects among Fe nanoparticles , nanoporous carbon and carbon fibers. A strong reflection loss ( RL ) of −46.2 dB and a wide absorbing bandwidth of 5.2 GHz ( RL < -10 dB) with a matching thickness of 2.5 mm were achieved for the Fe@NPC@CF composites with a low filling ratio of 25%. Therefore, this work not only paved the way for development of biomass as a green, low-cost and renewable high-performance carbon-based absorber, but also provided a good design and fabricating concept for the composite materials of EM wave absorber.
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Chemical Engineering Journal Advances
·
2021
·
IF 0
Kai Wei,Xiufan Liu,Shiyu Cao,Huijuan Cui,Yu Zhang,Zhihui Ai
In this study, we fabricated a micro-nano structured Fe 2 O 3 @FeB composites by treating commercial Fe 2 O 3 with sodium borohydride. The outside amorphous FeB alloy shell endowed the Fe 2 O 3 @FeB with remarkable Fenton-like performance in organic pollutants oxidation by efficient Fe(III)/Fe(II) cycle. For instance, the pseudo first-order rate constants of RhB degradation using Fe 2 O 3 @FeB as Fenton reagent was 74.6 times that of the Fe 2 O 3 counterpart, the hydroxyl radical generation rate of Fe 2 O 3 @FeB was 1-3 orders of magnitude larger than that of other heterogeneous Fenton reagent. Further mechanistic study unveiled that FeB was oxidized accompanying with Fe(0) and B(0) continuously donated electrons to Fe(III) to secure the efficient generation of surface Fe(II), which could generate additional H 2 O 2 by consecutive single-electron molecular oxygen activation (O 2 →•O 2 − →H 2 O 2 ), leading to enhance •OH production and Fenton-degradation toward typical pollutants. This study provides a facile route for efficient heterogeneous Fenton and strengthens the vital role of molecular oxygen activation on Fenton-like process.
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PHOSPHORUS SULFUR AND SILICON AND THE RELATED ELEMENTS
·
2019
·
IF 0.781
Xiaoling Yang,Ying Bai,Jiayun Li,Zinan Dai,Jiajian Peng
A novel iron-catalyzed hydrosilylation of alkenes process under solvent-free conditions has been reported. The influence of the amount of Fe catalyst, reaction temperature and various alkenes and silanes on the hydrosilylation were investigated. High yields of adduct were obtained in the hydrosilylation of octene with MeCl2H, Me2ClSiH and Ph2SiH2 by using 10 mol% iron powder as a signal catalyst.
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高影响因子
ADVANCED ENGINEERING MATERIALS
·
2024
·Vol. 26
·期 14
·2400527
·
IF 3.4
Rongjuan Zhang,Qi Hu,Shaobo Yang,Song Yan,Yaxin Gu,Jiawei Ji,Zheng Zhou,Chaoze Liu,Xinran Li,Zihao Wang,Chengchun Tang
The arrival of the 5 G era has brought great benefits to our lives, but it has also brought problems such as electromagnetic radiation. Therefore, the demand for lightweight, high-performance microwave absorbing materials with wide effective bandwidth is increasing. Herein, MIL-53/g-C 3 N 4 is first synthesized from precursors of ferric chloride, terephthalic acid, and g-C 3 N 4 , and then thermally annealed at different temperatures to generate MOF-Fe@C nanocomposites. Heat treatment can effectively carbonize g-C 3 N 4 to amorphous carbon and reduce iron in MIL-53 to magnetic Fe and Fe 3 O 4 nanoparticles through carbon-thermal reduction reaction. The synergistic effect of dielectric loss of amorphous carbon and magnetic losses of magnetic particles enhances attenuation and improves impedance matching, enhancing microwave absorption. The RL min of MOF-Fe@C(4)-700 is as low as -72.78 dB at 9.44 GHz at a thickness of 3.18 mm and its effective absorption bandwidth is as broad as 4.88 GHz, covering most of X-band frequency range. The research introduces a novel technique for synthesizing absorbers with controllable electromagnetic characteristics by incorporating g-C 3 N 4 as carbon sources into MOF materials.
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