ACS ES&T Water
·
2020
·
IF 0
Mingyue Zhao,Zhicheng Cui,Liang Fu,Fabrice Ndayisenga,Dandan Zhou
The slow reduction of Fe(III) to Fe(II) in electro-Fenton technology limits pollutant removal and causes Fe sludge production. This study hypothesizes that Shewanella, a dissimilatory iron-reducing bacteria, can accelerate the iron reduction of the Fenton reaction. A Shewanella biofilm coupled with Fe2O3 coated electrode (F/S) was used to drive the electro-Fenton reaction, and compared the results with the singlet Fe2O3 (F) anode and Shewanella biofilm anode (S). Meanwhile, dissolved oxygen (DO) is studied as an important influencing factor. The suitable DO was verified at ∼2 mg/L, phenol removal of F/S was 67% higher than that of the sum of three other singlet systems. The chemical oxygen demand (COD) removal was 72% and 50% higher than that of F and S, respectively. F/S corrosion current (Icorr) was 6.3 times higher than F, and induced hematite to transform into Fe2PO5 and FeOOH on the anode. Long-term operation showed that phenol was almost 100% removed for F/S; COD removal was generally 20% higher than F; thus, the toxicity of the effluent could be significantly decreased. The total Fe loss did not exceed 10% at the end of operation. This paper provides a feasibly novel method for electro-Fenton reaction, by employing Fe-reducing bacteria.
研究领域:
环境科学
·
微生物学
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产品关联
DOI
SCIENCE OF THE TOTAL ENVIRONMENT
·
2013
·
IF 3.258
Yan Xu,Yan He,Xiaoli Feng,Luyi Liang,Jianming Xu,Philip C. Brookes,Jianjun Wu
A novel Fe(III) reducing bacterium, Clostridium beijerinckii Z, was isolated from glucose amended paddy slurries, and shown to dechlorinate pentachlorophenol (PCP). Fifty percent of added PCP was removed by C. beijerinckii Z alone, which increased to 83% in the presence of both C. beijerinckii Z and ferrihydrite after 11 days of incubation. Without C. beijerinckii Z, the surface-bound Fe(II) also abiotically dechlorinated more than 40% of the added PCP. This indicated that the biotic dechlorination by C. beijerinckii Z is a dominant process causing PCP transformation through anaerobic dechlorination, and that the dechlorination rates can be accelerated by simultaneous reduction of Fe(III). A biochemical electron transfer coupling process between sorbed Fe(II) produced by C. beijerinckii Z and reductive dehalogenation is a possible mechanism. This finding increases our knowledge of the role of Fe(III) reducing genera of Clostridium in dechlorinating halogenated organic pollutants, such as PCP, in anaerobic paddy soils.
研究领域:
环境微生物学
·
生物修复
·
土壤科学
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产品关联
DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2011
·
IF 1.77
Jiang Xue Dong,Wei Wen,Nian Bing Li,Hong Qun Luo
In pH 2.6 HCl solution, dopamine (DA) could reduce Fe(III) to Fe(II), which further reacted with [Fe(CN) 6 ] 3− to form a Fe 3 [Fe(CN) 6 ] 2 complex. By virtue of hydrophobic force and Van der Waals force, the complex aggregated to form Fe 3 [Fe(CN) 6 ] 2 nanoparticles with the average diameter of about 20 nm. This resulted in a significant enhancement of resonance Rayleigh scattering (RRS). The maximum wavelength of the ion-association complex was located at about 350 nm. The increment of scattering intensity (Δ I RRS ) was directly proportional to the concentration of DA in the range of 0.06–1.0 μg/mL. This method has high sensitivity and the detection limit (3 σ ) for DA was 3.43 ng/mL. In this work, the characteristics of absorption and RRS spectra of this reaction have been studied. The optimum reaction condition and influencing factors have been investigated. The method was applied to the determination of DA in pharmaceutical samples with satisfactory results. Furthermore, the reaction mechanism and the reasons of RRS enhancement have been explored.
研究领域:
分析化学
·
生物医学
·
药物分析
✓ 已验证
DOI
PubMed
高影响因子
Sustainable Materials and Technologies
·
2024
·
IF 8.6
Yijun Chen,Meina Cheng,Hailiang Yang,Sanjian Ma,Long Jin,Zixia Lin,Xin Liu
The traditional Fenton process has two issues that hinder its further application and promotion. One is the generation of large amounts of iron sludge. The other is the safe storage and transport of explosive H 2 O 2 . The problems could be solved by accelerating to regenerate Fe(II) and realizing to self-generate H 2 O 2 . The key to the solution lies in the use of reducing active hydrogen [H] to supply electrons. The effect of different loading methods of Pd 0 nanoparticles (NPs), active centres for [H] generation, on the catalytic performance is unknown. Herein, the Pd/UiO-66(Zr) (Pd 0 NPs loaded on the surface of UiO-66(Zr)) and Pd@UiO-66(Zr) (Pd 0 NPs confined into the pores of UiO-66(Zr)) were synthesized. It confirmed that the [H] could be used to promote to regenerate Fe(II) and self-generate H 2 O 2 . Using only a trace amount of ferrous (25 μM) and without H 2 O 2 , the trimethoprim (20 mg·L −1 ) could be thoroughly removed within 90 min. Moreover, the stability of Pd@UiO-66(Zr) was slightly superior to that of Pd/UiO-66(Zr) because of the confinement effect of pore wall on Pd 0 NPs, as well as the interception effect on the intermediate products that can be complexed with Pd 0 NPs.
研究领域:
环境科学
·
催化化学
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产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Shu Wang,Nanqi Ren,Danhui Liang,Jifei Chang,Xin Wang,Jiaguo Yan,Xiang Cheng,Lili Dong,Nan Li
Vivianite is an important bio-induced product of dissimilated iron reduction (DIR), which exists widely in activated sludge and digested sludge of wastewater treatment plants (WWTPs). Extracellular polymeric substances (EPS) surrounding dissimilatory iron-reducing bacteria (DIRB) were reported to be transient media for microbial extracellular electron transfer (EET) and DIR. However, what happens when a layer of EPS envelops microbial cells during vivianite recovery? This study tried to assess the relationship between iron reduction and electron transfer by stripping EPS layer-by-layer, then clarified the delamination of different EPS layers on the performance of vivianite recovery. After stripping total EPS (PC-EPS batches) of DIRB, the Fe (III) reduction efficiencies ( R Fe ), Fe (III) reduction rate ( V Fe ), and vivianite formation efficiency ( R V ) decreased by 33%, 37%, and 30%, respectively. Tightly bound-EPS (TB-EPS) was confirmed to play a crucial role in vivianite formation, which contributed 28–51% to vivianite recovery and 34–55% to iron reduction. Electronic shuttle substances were contained in TB-EPS, which enhanced the EET rate and efficiency between cells and Fe (III). The polysaccharide content of TB-EPS was positively related to adhesiveness between cells and mineral, as well as the iron reduction efficiency. Furthermore, redox proteins (PpcA, OmcB) were embedded in EPS, which shortened the distance of electron hopping to across the EPS layer and further accelerated vivianite recovery from wastewater. Long-term operation of anaerobic reactors confirmed that TB-EPS played critical roles in bio-induced vivianite formation.
研究领域:
环境科学
·
微生物学
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污水处理
·
生物地球化学
✓ 已验证
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Xing Yan,Jie Bu,Xiong Chen,Ming-Jun Zhu
Microbial extracellular respiration is an important energy metabolism on earth, which is significant for the elemental biogeochemical cycle. Herein, extracellular Fe(III) and electrode respiration were confirmed in Thermoanaerobacterium thermosaccharolyticum MJ2 . The intra/extracellular electron transfer (IET/EET) mechanism of MJ2 was investigated by comparative genomic analysis for the first time. Morphological characterization and electrochemical properties of anode illustrated that MJ2 generated bio-electricity by forming a biofilm. The respiration chain inhibition and enzyme activity tests showed that hydrogenase with cytochrome c (Cyt- c ) was involved in IET of MJ2 . Noteworthily, the exogenous Cyt- c increased hydrogenase activity to promote bio-electricity generation by 92.84 %. The Cyt- c gene synteny between MJ2 and another well-known exoelectrogen ( Thermincola potens JR ) indicated that Cyt- c bound to the outer membrane mediated the formation of biofilm involved in EET of MJ2 . This study broadened the understanding of microbial extracellular respiration diversity and provided new insights to explore the electron transfer pathways of exoelectrogens.
研究领域:
微生物学
·
基因组学
·
电化学
·
生物地球化学
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Meiling Chen,Lin Ding,Shijun Zhu,Xiuqin Xiong,Xinkai Yuan,Yanhua Peng,Liming Yang,Hui Shi,Penghui Shao,Xubiao Luo
The slow Fe(II)/Fe(III) cycle during the Fenton reaction process strongly impedes oxidation efficiency in practical applications. In this study, an activated carbon (AC) assisted Fenton reaction system was used to treat electroplating wastewater containing Ni-ethylenediaminetetraacetic acid (Ni-EDTA). AC was found to enhance the removal of Ni-EDTA in Fenton/Fenton-like reactions. The reported results revealed that AC could effectively promote the regeneration of Fe(II) from Fe(III) species via electron transfer to improve the reaction rather than directly enhancing the H 2 O 2 decomposition to accelerate the production of hydroxyl radicals (•OH). Quenching experiments and EPR also demonstrated that •OH and •O 2 − took part in the radical oxidation process, in which the contribution of •OH was dominant. XPS and FT-IR analysis further confirmed that the carbonyl group (C O) on the surface of AC could indeed act as the dominant active site and an electron donor to directly reduce Fe(III). In addition, electrochemical tests indicated that AC could increase the oxidation potential of Fe(III) to boost the reaction between Fe(III) and H 2 O 2 , thus enabling the transfer of electrons from H 2 O 2 to Fe(III) to facilitate the Fe(II)/Fe(III) cycle. This study might contribute to a new insight into the mechanisms of AC-catalyzed Fenton oxidation processes for the decomplexation heavy metal-EDTA.
研究领域:
环境科学
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化学工程
·
废水处理
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产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Zhang Xiang,Tang Jingjing,Wang Lingling,Wang Chuan,Chen Lei,Chen Xinqing,Qian Jieshu,Pan Bingcai
Heterogeneous Fenton reaction represents one of the most reliable technologies to ensure water safety, but is currently challenged by the sluggish Fe(III) reduction, excessive input of chemicals for organic mineralization, and undesirable carbon emission. Current endeavors to improve the catalytic performance of Fenton reaction are mostly focused on how to accelerate Fe(III) reduction, while the pollutant degradation step is habitually overlooked. Here, we report a nanoconfinement strategy by using graphene aerogel (GA) to support UiO-66-NH 2 -(Zr) binding atomic Fe(III), which alters the carbon transfer route during phenol removal from kinetically favored ring-opening route to thermodynamically favored oligomerization route. GA nanoconfinement favors the Fe(III) reduction by enriching the reductive intermediates and allows much faster phenol removal than the unconfined analog (by 208 times in terms of first-order rate constant) and highly efficient removal of total organic carbon, i.e., 92.2 ± 3.7% versus 3.6 ± 0.3% in 60 min. Moreover, this oligomerization route reduces the oxidant consumption for phenol removal by more than 95% and carbon emission by 77.9%, compared to the mineralization route in homogeneous Fe 2+ +H 2 O 2 system. Our findings may upgrade the regulatory toolkit for Fenton reactions and provide an alternative carbon transfer route for the removal of aqueous pollutants.
研究领域:
环境科学
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催化
·
水处理
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Hongwei Zhu,Xu Yin,Yi Wang,Kajia Wei,Liankai Gu,Yonghao Zhang,Zhenshan Duan,Zhen Huang,Haoming Chen,Weiqing Han
This study developed a self-supported MOF/FeOOH heterojunction cathode without binders for boosted Fe(Ⅲ) reduction in heterogeneous electro-Fenton (EF) processes. The electron transport channels from FeOOH to in-situ grown NH 2 -MIL-88B(Fe) were established through the spontaneous formation of an internal electric field (IEF), which enhanced the electrical conductivity and disrupted the chemical inertness of the Fe(Ⅲ) reduction. The MOF/FeOOH cathode increased sulfamethazine (SMT) removal up to 95.76 %, 2.5 times better than using PTFE as binders. After ten-consecutive degradation experiments, the Fe(Ⅱ) content at cathode surface increased from 39.23 % to 56.73 %. Density functional theory (DFT) calculations and advanced characterization techniques demonstrated the efficient Fe(Ⅲ) reduction and H 2 O 2 activation during the reaction. These results elucidate the promoting effect of modulating the “contact” between the catalyst and current collectors, as to provide a feasible and promising strategy for the development of efficient heterogeneous EF cathodes.
研究领域:
环境科学
·
材料科学
·
电化学
·
催化
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产品关联
DOI
高影响因子
Biochar
·
2024
·Vol. 6
·期 1
·1-14
·
IF 13.1
Wang Shengsen,Li Wenjing,Ding Chengyu,Zhang Jian,Zhang Ni,Li Yuncong C.,Gao Bin,Wang Bing,Wang Xiaozhi
Arsenic (As) detoxification in polluted soils by iron-based materials can be mediated by the endogenous soil organic matter (SOM), nevertheless the mechanisms remain unclear. Herein, endogenous SOM in a paddy soil was substantially removed to understand its roles on As immobilization by biochar-supported zero-valent iron (ZVI/BC). The results demonstrated that ZVI/BC application significantly decreased As bioavailability by 64.2% compared with the control soil under the anaerobic condition. XPS and HR-TEM suggested As immobilization by ZVI/BC mainly invoked the formation of ternary complexes (i.e., As-Fe-SOM). However, SOM depletion compromised the efficacy of ZVI/BC for As immobilization by 289.8%. This is likely because SOM depletion increased the fulvic acid and OH − contents in soils. Besides, ZVI/BC increased the proportion of As(III) in available As fraction, but SOM depletion altered the mechanisms associated with As(V) reduction. That is, As(V) reduction resulted from the reductive capacity of ZVI in the pristine soil, but the As(V)-reducing bacteria contributed greater to As(V) reduction in the SOM-depleted soil. Additionally, SOM depletion boosted the abundances of Fe(III)- and As(V)-reducing bacteria such as Bacillus and Ammoniphilus in soils, which enhanced the dissimilatory arsenate reduction. Thus, this work highlighted the importance of SOM in the remediation of As-contaminated soils by ZVI/BC. Graphical Abstract
研究领域:
环境科学
·
土壤化学
·
微生物学
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产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Yanping Zhu,Qingru Xie,Runliang Zhu,Ying Lv,Yunfei Xi,Jianxi Zhu,Jian Fan
As the heterogeneous Fenton reactions are always restricted by the unsatisfied reduction efficiency of Fe(III) and ineffective consumption of H 2 O 2 , many strategies have been developed. In this work, we prepared hydrothermal carbons (HTC) with different graphitization degrees using glucose under different hydrothermal times, and then they were combined with ferrihydrite (Fh). Interestingly, although 30%HTC/Fh has much better BPA degradation efficiency than Fh (26 times larger of calculated degradation rate constants), the decomposition rate of H 2 O 2 in the former system is lower. The generated Fe(II) of HTC/Fh is much higher than that of Fh during the heterogeneous Fenton reactions , and the degradation of BPA is almost unaffected by p -benzoquinone (scavenger of superoxide radicals (O 2 •− )) while greatly inhibited by isopropanol (scavenger of hydroxyl radicals (HO • )). These results indicate that HTC act as electron donors due to the abundant carbon-centered persistent free radicals (PFRs) to directly reduce Fe(III) to Fe(II) and therefore decrease the H 2 O 2 consumption by Fe(III), which subsequently inhibits the generation of less active O 2 •− and promote the utilization efficiency of H 2 O 2 . HTC with a low graphitization degree contain more PFRs for Fe(III) reducing, significantly enhancing the Fenton catalytic activity of Fh.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Sciences
·
2024
·
IF 5.9
Yujiang Huang,Tong Hu,Sichen Li,Wenjun Zhou
Harnessing the redox potential of biochar to activate airborne O 2 for contaminant removal is challenging. In this study, ferrihydrite (Fh) modified the boron (B), nitrogen (N) co-doped biochars (BCs) composites (Fh/B(n)NC) were developed for enhancing the degradation of a model pollutant, tetracycline (TC), merely by airborne O 2 . Fh/B(3)NC showed excellent O 2 activation activity for efficient TC degradation with a apparent TC degradation rate of 5.54, 6.88, and 22.15 times that of B(3)NC, Fh, and raw BCs, respectively, where 1 O 2 and H 2 O 2 were identified as the dominant ROS for TC degradation. The B incorporation into the carbon lattice of Fh/B(3)NC promoted the generation of electron donors, sp 2 C and the reductive B species, hence boosting Fe(III) reduction and 1 O 2 generation. O 2 adsorption was enhanced due to the positively charged adsorption sites (C- B + and N C + ). And 1 O 2 was generated via Fe(II) catalyzed low-efficient successive one-electron transfer (O 2 → O 2 ·− → 1 O 2 , H 2 O 2 ), as well as biochar catalyzed high-efficient two-electron transfer (O 2 → H 2 O 2 → 1 O 2 ) that does not involve . O 2 − as the intermediate. Moreover, Fh/B, N co-doped biochar showed a wide pH range, remarkable anti-interference capabilities, and effective detoxification. These findings shed new light on the development of environmentally benign BCs materials capable of degradading organic pollutants.
研究领域:
环境科学
·
材料科学
·
化学工程
·
污染控制
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产品关联
DOI
PubMed
高影响因子
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