SOIL BIOLOGY & BIOCHEMISTRY
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2022
·
IF 8.546
Jinzhi Yao,Shuping Qin,Ting Liu,Tim J. Clough,Nicole Wrage-Mönnig,Jiafa Luo,Chunsheng Hu,Tida Ge,Shungui Zhou
Poorly crystalline iron (Fe) oxides are commonly deposited on the surface of rice roots, forming an Fe plaque. This Fe plaque is an important area for Fe redox reactions because the poorly crystalline Fe is available for microbial transformations. However, it remains unclear what the mechanisms are that cause the root Fe plaque to affect CO 2 emissions from paddy soils . Thus, this study investigated the effects of Fe plaque on paddy soil CO 2 emissions and the associated mechanisms. Paddy soil with rice plant roots containing an Fe plaque-coating had 1.5-fold larger CO 2 emissions and higher expression levels of genes involved in soil carbon (C) degradation than Fe plaque-free roots, indicating that Fe plaque stimulated paddy soil derived CO 2 emissions. Fe plaque-coated rice roots, immersed in a 13 C-labeled glucose solution, emitted more CO 2 , with a higher abundance of 13 CO 2 , than the Fe plaque-free roots. These differences were not observed when the surfaces of the rice roots were sterilized. These results indicate that the Fe plaque-stimulated CO 2 emissions were due to soil microbial respiration , not autotrophic root respiration . Chelating the dissolved Fe on the root surface eliminated Fe plaque stimulation of CO 2 emissions, while Fe(III) supplementation correlated with enhanced CO 2 emissions. The stoichiometric mole ratio of the enhanced CO 2 emissions to the Fe(II) generated was comparable to the theoretical ratio of Fe(III) when used as an electron acceptor for organic C decomposition. These results showed that the Fe plaque enhancement of CO 2 emissions was coupled to Fe(III) reduction. Limiting the stimulating effects of Fe plaque on CO 2 emissions may be a potentially useful approach for mitigating organic C loss from paddy soils.
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2021
·Vol. 35
·期 8
·e6280
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IF 4.105
Jinzhong Guo,Zhuming Guo,Zhiyin Xiao,Jing Jin,Xiuqin Yang,Yi He,Xiaoming Liu
Four new monoiron (II) tricarbonyl complexes with the amine bound, fac -[Fe(CO) 3 I 2 (NH 2 R)] (R = Et, 1 ; n Pr, 2 ; n Bu, 3 ; n Pent, 4 ), were reported using cis -[Fe(CO) 4 I 2 ] as the precursor. All the complexes 1 – 4 were structurally confirmed by various techniques such as ultraviolet–visible (UV–vis), Fourier transform infrared (FTIR), and nuclear magnetic resonance (NMR) spectra and elemental analysis of which complexes 1 and 2 are crystallographically determined. The reaction of the precursor with alkylamines proceeded in two main parallel pathways to form both aminium salts of fac -[Fe(CO) 3 I 3 ] − and the amine-bound complexes ( 1 – 4 ). Their dominances altered with the reaction time. These complexes in DMSO undergo quick decomposition with complex 1 as the relatively most stable one ( t 1/2 = 7.3 min) although they are stable in solid status. Unlike the triiodo anion and pyridinyl analogs showing severe cytotoxicity due to the generation of iodine radical during the decomposition, no iodine radicals were detected from the fac -[Fe(CO) 3 I 2 (NH 2 R)] complexes. Therefore, the cell viability of RT112 cells was not affected by the presence of the amine-bound iron complex ( 1 ) up to 100 μmol L −1 .
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ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Xiangzhong Kong,Yong Yang,Siyuan Xu,Shi Li,Xi Chen,Lihua Wang,Zhongmin Wan
Phen strongly coordinates dissociative Fe ions to form active Fe-N X sites. • The strong coupling of Fe-F strengthens the poisoning resistance of the catalyst. • N,F co-doped network enhances ORR by lowering reaction energy barrier at Fe-N X sites. • Porous chain-bead framework prevents agglomeration, providing abundant sites and fast charge transfer. • AEMFCs with FeN X @Fe-F-CNF cathodes achieve a peak power density of 0.7 W cm −2 . Transition-metal-nitrogen-carbon (M-N-C) catalysts have garnered significant recognition as highly active non-precious metal catalysts for the oxygen reduction reaction (ORR) in anion exchange membrane fuel cells (AEMFCs), attributable to their low-cost, high atom-utilization and remarkable ORR performance. However, the primary drawback of conventional M-N-C catalysts lies in the suboptimal electronic structure of their metal centers (M-N 4 ), which results in excessively strong adsorption energy toward oxygen intermediates, thereby limiting their intrinsic activity and stability. Herein, the FeF 2 /Fe 3 N nanocrystalline decorated N, F co-doped chain-bead Fe-N-C fiber network (FeN X @Fe-F-CNF) has been fabricated by electrospinning strategy through utilizing 1,10-Phenanthroline monohydrochloride monohydrate (Phen) and NH 4 F as nitrogen/fluoride sources respectively. The six-membered heterocyclic in Phen allows for strong coordination with dissociative Fe ions, thus, promoting the formation of Fe-N X sites. Furthermore, co-doped N, F is able to tune the electronic structure of Fe active sites, whereas flexible chain-bead nanofibers guarantee considerable structural adaptation, thereby contributing to the enhancement of their catalytic activity and stability. The obtained FeN X @Fe-F-CNF exhibits enhanced ORR catalytic activity (with an E 1/2 of 0.863 V) and superior durability (with a current retention of 90.7 % after maintaining the ORR typical potential range for 100,000 seconds and a E 1/2 negative shift of 7 mV after 5000 continuous potential cycles). Furthermore, the assembled AEMFCs based on FeN X @Fe-F-CNF catalysts demonstrate excellent performance, with a peak power density of 0.7 W cm −2 , indicating its potential feasibility for commercial applications. Download: Download high-res image (293KB) Download: Download full-size image
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JOURNAL OF HAZARDOUS MATERIALS
·
2015
·
IF 4.529
Zhouwei Miao,Xiaogang Gu,Shuguang Lu,Mark L. Brusseau,Ni Yan,Zhaofu Qiu,Qian Sui
In this study, the effects of reducing agents on the degradation of tetrachloroethene (PCE) were investigated in the Fe(II)/Fe(III) catalyzed sodium percarbonate (SPC) system. The addition of reducing agents, including hydroxylamine hydrochloride, sodium sulfite, ascorbic acid and sodium ascorbate, accelerated the Fe(III)/Fe(II) redox cycle, leading to a relatively steady Fe(II) concentration and higher production of free radicals. This, in turn, resulted in enhanced PCE oxidation by SPC, with almost complete PCE removal obtained for appropriate Fe and SPC concentrations. The chemical probe tests, using nitrobenzene and carbon tetrachloride, demonstrated that HO was the predominant radical in the system and that O 2 − played a minor role, which was further confirmed by the results of electron spin resonance measurements. PCE degradation decreased significantly with the addition of isopropanol, a HO scavenger, supporting the hypothesis that HO was primarily responsible for PCE degradation. It is noteworthy that Cl − release was slightly delayed in the first 20 min, indicating that intermediate products were produced. However, these intermediates were further degraded, resulting in the complete conversion of PCE to CO 2 . In conclusion, the use of reducing agents to enhance Fe(II)/Fe(III) catalyzed SPC oxidation appears to be a promising approach for the rapid degradation of organic contaminants in groundwater.
研究领域:
环境化学
·
水处理
·
修复技术
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IONICS
·
2026
·
IF 3.4
Liu Zhuangzhuang,Yang Xiaobo,Li Shengting,Lu Guimin,Sun Ze
Iron impurities are among the most detrimental impurities in magnesium electrolysis because they can promote cathode passivation, reduce current efficiency, and contribute to Mg loss. This study systematically investigated the electrochemical reduction of Fe(Ⅲ) and the corresponding cathode passivation mechanism in an anhydrous carnallite melt composed of MgCl₂ and KCl with a molar ratio of 1:1 at 973 K. Based on cyclic voltammetry (CV), square wave voltammetry (SWV), chronoamperometry (CA), chronopotentiometry (CP), scanning electron microscopy (SEM), and energy-dispersive X-ray spectroscopy (EDS), the results show that Fe(Ⅲ) reduction is a single-step, diffusion-controlled, quasi-reversible process. Current reversal chronopotentiometry (CR-CP) measurements based on representative curves suggested a decrease in apparent current efficiency from 92.5% to 79.1% after 10 min of electrolysis. Morphological and electrochemical analyses further suggest the underlying passivation mechanism. During the initial stage of electrolysis, Fe(Ⅲ) is preferentially reduced and deposited on the cathode surface as a porous, sponge-like structure. The newly formed porous Fe deposits may adsorb MgO-containing species from the molten salt, suggesting the possible presence of an Fe/Mg/O-rich passivation layer on the cathode surface. Such a surface layer may reduce the wettability of the cathode toward liquid Mg and hinder the spreading and coalescence of Mg droplets, thereby promoting the deposition of Mg as fine, discrete, caviar-like particles with diameters below 1 mm. This process may contribute to Mg loss and the decrease in current efficiency during electrolysis. These findings provide fundamental insight into the role of Fe(Ⅲ) in cathode passivation during magnesium electrolysis.
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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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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xin Zhang,Qingling Fu,Hongqing Hu,Jun Zhu,Yonghong Liu
The co-oxidation of Fe(II) and As(III) occurs under aerobic conditions , and Fe(II) may largely determine the fate of As(III), but the effect of Fe(II) on the As(III) oxidation is barely explored. In this research, the limiting and driving roles of Fe(II) in As(III) oxidation were systematically studied through batch kinetic studies in combination with X-ray photoelectron spectroscopy (XPS) depth profiling, scanning electron microscopy and energy dispersive X-ray spectrometry (SEM-EDS), and quenching experiments. The results showed that As(III) oxidation efficiency increased with the increase of Fe/As molar ratio (from 63.1% to 98.3%), but decreased with the increase of pH (from 96.0% to 44.2%) and the increase of air flow rate (from 88.1% to 75.1%). The Fe(II) oxidation rate increased with the increase of pH and air flow rate. When Fe(II) was oxidized rapidly, As(III) was more likely to be immobilized in the “inner sphere” of formed Fe (hydr)oxides, limiting As(III) oxidation. On the other hand, Fe(II) was oxidized to produce Fe (hydr)oxides to adsorb or fix As(III); meanwhile, the ROS generated by Fenton-like reaction of Fe(II) promoted As(III) oxidation, especially, •O 2 − and H 2 O 2 were important ROS that drove the As(III) oxidation. These findings might provide a new insight for Fe(II) and As(III) geochemistry cycling in naturally occurring environment.
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PubMed
高影响因子
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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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Hongyan Zhang,Tao Yang,Hao Zhou,Yikai Wang,Xuehan Yang,Wenjie Liang,Dan Wu,Pan Yuan,Tingting Yu,Maoshuai He,Wenxian Wei
Ni phosphides have recently attracted considerable attention as promising catalysts for the oxygen evolution reaction (OER) and are generally promoted by Fe incorporation. However, the catalytic performance of nickel phosphide still does not meet the desired expectations. Additionally, the catalytic activity of iron (Fe) is insignificant and can be disregarded. In this study, we used C 3 N 4 as a carbon substrate to modulate the 3 d electron configurations and adsorption properties of Ni and Fe. Density functional theory (DFT) analysis reveals that the catalytic performance of Ni sites can be enhanced by utilizing the C 3 N 4 substrate. Surprisingly, the Fe sites can also be activated to catalyze OER through a direct O 2 mechanism and the catalytic activity of Fe is found to surpass that of Ni. As a result, the FeNi-C 3 N 4 -P catalyst demonstrated remarkable catalytic performance for OER. It exhibited a Tafel slope of 40.4 mV dec −1 , an overpotential of 235 mV at 100 mA cm −2 , and exhibited exceptional stability. This study highlights the activation of Fe and the enhancement of Ni by utilizing nitrogen-containing carbon substrates. This strategy offers promising prospects for the development of efficient Ni/Fe-based OER catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaomeng Zhang,Yang Zong,Longqian Xu,Yunfeng Mao,Deli Wu
Abiotic humification can be facilitated by iron-containing minerals or oxides, but most studies have focused on well-crystallized and stable iron phases, the catalytic effect of which is generally unremarkable. In the present study, we report an enhanced abiotic integrated polyphenol-Maillard humification reaction catalysed by Mg/Fe-layered double hydroxide (Mg/Fe-LDH) with high surface reactivity. The results demonstrated that Mg/Fe-LDH could effectively promote the humification reaction at a lower dosage compared with Fe 2 O 3 . As an iron-chelating ligand, catechol rapidly induced iron dissolution from Mg/Fe-LDH through the formation of an Fe(III)-catechol complex, which strengthened the catalytic effect of Fe(III). The photochemical behaviour of Fe(III)-catechol complex and its impact on the Fe(III)-catalysed humification process were investigated. Under light irradiation, environmentally persistent free radicals (EPFRs) originated from the Fe(III)-catechol complex were formed and stabilized in the presence of Mg/Fe-LDH particles, which inhibited the oxidation of catechol and the humification process. Hence, the formation of humic substances (HS) catalysed by Mg/Fe-LDH was more efficient under darkness. Iron redox cycling and generation of reactive oxygen species (ROS), HO• and O 2 •- , were also involved. According to transformation products (TPs) analysis, ortho -aminophenol was proposed to be a key product in the humification reaction. Self-coupling of catechol radical and ortho -aminophenol radical, ring cleavage were likely to occur in the Fe(III)-catalysed humification process. Higher relative abundance of CHO products was observed in the presence of Mg/Fe-LDH by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), suggesting that iron is effective on promoting C–C bonds formation. The above results provide more comprehensive insights into Fe(III)-catalysed humification and a guidance to improve the efficiency of HS formation and carbon sequestration in organic wastes utilization.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Usman Farooq,Jingguo Zhuang,Xinhai Wang,Shuguang Lyu
The removal of chlorinated hydrocarbons through heterogeneous catalysts from groundwater has become a valuable approach. However, the synthesis of a highly efficient and persistent material especially for trichloroethane (TCA) removal is still immature . In this study, we prepared polydopamine (PDA) embedded Fe/rGO nanocomposite via pH-induced polymerization of dopamine for the degradation of TCA in sodium percarbonate (SPC) system. The experimental outcomes revealed that PDA decorated Fe/rGO not only enhanced the TCA degradation (98%) more economically but also strengthened the stability and recyclability of catalyst compared to bare Fe/rGO. The TEM, XRD, FTIR, XPS and VSM analyses declared the successful preparation of magnetically separable PDA@Fe/rGO nanocomposite. Furthermore, a higher degradation rate of probe compounds in PDA@Fe/rGO/SPC system indicated that PDA decoration improved the formation of active species due to autoxidation of dopamine and reducing capability of PDA. The impact of solution matrix on PDA@Fe/rGO performance elucidated the effect of various species on degradation. The GCMS, TOC analysis and dechlorination experiments validated the formation of non-toxic products and reasonable TOC and chloride ions removal. The PDA@Fe/rGO catalyst can be recycled for six consecutive cycles retaining a 76% along with abundant availability of Fe 2+ and Fe 3+ species validated using XRD and XPS analysis. The enhanced remediation capacity and improved recyclability of PDA@Fe/rGO nanocomposite can serve as a shining star for the practical application of TCA removal in groundwater.
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