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Advances in Fe(III) bioreduction and its application prospect for groundwater remediation: A review

Yu Jiang, Beidou Xi, Rui Li, Mingxiao Li, Zheng Xu, Yuning Yang, Shaobo Gao

《环境科学与工程前沿（英文）》 2019年 第13卷 第6期 doi: 10.1007/s11783-019-1173-9

摘要： Microbial Fe(III) reduction is closely related to the fate of pollutants. Bioavailability of crystalline Fe(III) oxide is restricted due to thermodynamics. Amorphous Fe(III) (hydro)oxides are more bioavailable. Enrichment and incubation of Fe(III) reducing bacteria are significant. Microbial Fe(III) reduction is a significant driving force for the biogeochemical cycles of C, O, P, S, N, and dominates the natural bio-purification of contaminants in groundwater (e.g., petroleum hydrocarbons, chlorinated ethane, and chromium). In this review, the mechanisms and environmental significance of Fe(III) (hydro)oxides bioreduction are summarized. Compared with crystalline Fe(III) (hydro)oxides, amorphous Fe(III) (hydro)oxides are more bioavailable. Ligand and electron shuttle both play an important role in microbial Fe(III) reduction. The restrictive factors of Fe(III) (hydro)oxides bioreduction should be further investigated to reveal the characteristics and mechanisms of the process. It will improve the bioavailability of crystalline Fe(III) (hydro)oxides and accelerate the anaerobic oxidation efficiency of the reduction state pollutants. Furthermore, the approach to extract, culture, and incubate the functional Fe(III) reducing bacteria from actual complicated environment, and applying it to the bioremediation of organic, ammonia, and heavy metals contaminated groundwater will become a research topic in the future. There are a broad application prospects of Fe(III) (hydro)oxides bioreduction to groundwater bioremediation, which includes the in situ injection and permeable reactive barriers and the innovative Kariz wells system. The study provides an important reference for the treatment of reduced pollutants in contaminated groundwater.

关键词： Microbial Fe(III) reduction     Mechanism     Groundwater contamination     Remediation    

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Removal of Cu(II) and Fe(III) from aqueous solutions by dead sulfate reducing bacteria

Hong’en QUAN, He BAI, Yang HAN, Yong KANG, Jiao SUN

《化学科学与工程前沿（英文）》 2013年 第7卷 第2期   页码 177-184 doi: 10.1007/s11705-013-1324-7

摘要： The biosorption properties of dead sulfate reducing bacteria (SRB) for the removal of Cu(II) and Fe(III) from aqueous solutions was studied. The effects of the biosorbent concentration, the initial pH value and the temperature on the biosorption of Cu(II) and Fe(III) by the SRB were investigated. FTIR analysis verified that the hydroxyl, carbonyl and amine functional groups of the SRB biosorbent were involved in the biosorption process. For both Cu(II) and Fe(III), an increase in the SRB biosorbent concentration resulted in an increase in the removal percentage but a decrease in the amount of specific metal biosorption. The maximum specific metal biosorption was 93.25 mg?g at pH 4.5 for Cu(II) and 88.29 mg?g at pH 3.5 for Fe(III). The temperature did not have a significant effect on biosorption. In a binary metal system, the specific biosorption capacity for the target metal decreased when another metal ion was added. For both the single metal and binary metal systems, the biosorption of Cu(II) and Fe(III) onto a SRB biosorbent was better represented by a Langmuir model than by a Freundlich model.

关键词： sulfate reducing bacteria     biosorption     Cu(II)     Fe(III)    

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Concurrent adsorption and reduction of chromium(VI) to chromium(III) using nitrogen-doped porous carbon

《环境科学与工程前沿（英文）》 2022年 第16卷 第5期 doi: 10.1007/s11783-021-1491-6

摘要：

• A high-efficiency N-doped porous carbon adsorbent for Cr(VI) was synthesized.

关键词： Chromium(VI)     Nitrogen-doped porous carbon     Adsorption     Reduction     Loofah sponge    

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Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

《能源前沿（英文）》 2022年 第16卷 第5期   页码 812-821 doi: 10.1007/s11708-020-0669-0

摘要： The development of highly active nitrogen-doped carbon-based transition metal (M-N-C) compounds for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) greatly helps reduce fuel cell cost, thus rapidly promoting their commercial applications. Among different M-N-C electrocatalysts, the series of Fe-N-C materials are highly favored because of their high ORR activity. However, there remains a debate on the effect of Fe, and rare investigations focus on the influence of Fe addition in the second heat treatment usually performed after acid leaching in the catalyst synthesis. It is thus very critical to explore the influences of Fe on the ORR electrocatalytic activity, which will, in turn, guide the design of Fe-N-C materials with enhanced performance. Herein, a series of Fe-N-C electrocatalysts are synthesize and the influence of Fe on the ORR activity are speculated both experimentally and theoretically. It is deduced that the active site lies in the structure of Fe-N , accompanied with the addition of appropriate Fe, and the number of active sites increases without the occurrence of agglomeration particles. Moreover, it is speculated that Fe plays an important role in stabilizing N as well as constituting active sites in the second pyrolyzing process.

关键词： oxygen reduction reaction     Fe-N-C     active sites     Fe addition     second heat treatment    

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Comparison of different valent iron on anaerobic sludge digestion: Focusing on oxidation reduction potential, dissolved organic nitrogen and microbial community

《环境科学与工程前沿（英文）》 2022年 第16卷 第6期 doi: 10.1007/s11783-021-1514-3

摘要：

• ORP value from −278.71 to −379.80 mV showed indiscernible effects on methane yield.

关键词： Enhanced anaerobic sludge digestion     Different iron valence     Oxidation reduction potential     Dissolved organic nitrogen     Microbial community    

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Enhanced degradation of trichloroethene by calcium peroxide activated with Fe(III) in the presence of

Xiang ZHANG,Xiaogang GU,Shuguang LU,Zhouwei MIAO,Minhui XU,Xiaori FU,Muhammad DANISH,Mark L. BRUSSEAU,Zhaofu QIU,Qian SUI

《环境科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 502-512 doi: 10.1007/s11783-016-0838-x

摘要： Trichloroethene (TCE) degradation by Fe(III)-activated calcium peroxide (CP) in the presence of citric acid (CA) in aqueous solution was investigated. The results demonstrated that the presence of CA enhanced TCE degradation significantly by increasing the concentration of soluble Fe(III) and promoting H O generation. The generation of HO? and O ? in both the CP/Fe(III) and CP/Fe(III)/CA systems was confirmed with chemical probes. The results of radical scavenging tests showed that TCE degradation was due predominantly to direct oxidation by HO?, while O ? strengthened the generation of HO? by promoting Fe(III) transformation in the CP/Fe(III)/CA system. Acidic pH conditions were favorable for TCE degradation, and the TCE degradation rate decreased with increasing pH. The presence of Cl , HCO , and humic acid (HA) inhibited TCE degradation to different extents for the CP/Fe(III)/CA system. Analysis of Cl production suggested that TCE degradation in the CP/Fe(III)/CA system occurred through a dechlorination process. In summary, this study provided detailed information for the application of CA-enhanced Fe(III)-activated calcium peroxide for treating TCE contaminated groundwater.

关键词： calcium peroxide     trichloroethene (TCE)     citric acid     ferric ion     free radicals     oxidation    

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Effect of Fe loading quantity on reduction reactivity of nano zero-valent iron supported on chelating

Jialu SHI,Shengnan YI,Chao LONG,Aimin LI

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 840-849 doi: 10.1007/s11783-015-0781-2

摘要： In this study, nanoscale zero-valent iron (NZVI) were immobilized within a chelating resin (DOW 3N). To investigate the effect of Fe loading on NZVI reactivity, three NZVI-resin composites with different Fe loading were obtained by preparing Fe(III) solution in 0, 30 and 70% (v/v) ethanol aqueous, respectively; the bromate was used as a model contaminant. TEM reveals that increasing the Fe loading resulted in much larger size and poor dispersion of nanoscale iron particles. The results indicated that the removal efficiency of bromate and the rate constant ( ) were decreased with increasing the Fe loading. For the NZVI-resin composite with lower Fe loading, the removal efficiency of bromate declined more significantly with the increase of DO concentrations. Under acidic conditions, decreasing the pH value had the most significant influence on NZVI-R3 with highest Fe loading for bromate removal; however, under alkaline conditions, the most significant influence of pH was on NZVI-R1 with lowest Fe loading. The effects of co-existing anions , and were also investigated. All of the co-existing anions showed the inhibition to bromate reduction.

关键词： nanoscale zero valent iron     loading quantity     reduction     chelating resin     bromated    

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Process control factors for continuous microbial perchlorate reduction in the presence of zero-valent

ARTHUR Robert D.,TORLAPATI Jagadish,SHIN Kyung-Hee,CHA Daniel K.,YOON Yeomin,SON Ahjeong

《环境科学与工程前沿（英文）》 2014年 第8卷 第3期   页码 386-393 doi: 10.1007/s11783-013-0593-1

摘要： Process control parameters influencing microbial perchlorate reduction via a flow-through zero-valent iron (ZVI) column reactor were investigated in order to optimize perchlorate removal from water. Mixed perchlorate reducers were obtained from a wastewater treatment plant and inoculated into the reactor without further acclimation. Examined parameters included hydraulic residence time (HRT), pH, nutrients requirement, and perchlorate reduction kinetics. The minimum HRT for the system was concluded to be 8 hr. The removal efficiency of 10 mg·L influent perchlorate concentration was reduced by 20%–80% without control to the neutral pH (HRT= 8 hr). Therefore pH was determined to be an important parameter for microbial perchlorate reduction. Furthermore, a viable alternative to pH buffer was discussed. The microbial perchlorate reduction followed the first order kinetics, with a rate constant ( ) of 0.761 hr . The results from this study will contribute to the implementation of a safe, cost effective, and efficient system for perchlorate reduction to below regulated levels.

关键词： perchlorate     zero-valent iron (ZVI)     microbial reduction     hydrogen    

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Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 525-535 doi: 10.1007/s11705-022-2232-5

摘要： Fe–Nx nanoparticles-embedded porous carbons with a desirable superstructure have attracted immense attention as promising catalysts for electrochemical oxygen reduction reaction. Herein, we employed Fe-coordinated covalent triazine polymer for the fabrication of Fe–Nx nanoparticle-embedded porous carbon nanoflorets (Fe/N@CNFs) employing a hypersaline-confinement-conversion strategy. Presence of tailored N types within the covalent triazine polymer interwork in high proportions contributes to the generation of Fe/N coordination and subsequent Fe–Nx nanoparticles. Owing to the utilization of NaCl crystals, the resultant Fe/N@CNF-800 which was generated by pyrolysis at 800 °C showed nanoflower structure and large specific surface area, which remarkably suppressed the agglomeration of high catalytic active sites. As expect, the Fe/N@CNF-800 exhibited unexpected oxygen reduction reaction catalytic performance with an ultrahigh half-wave potential (0.89 V vs. reversible hydrogen electrode), a dominant 4e– transfer approach and great cycle stability (> 92% after 100000 s). As a demonstration, the Fe/N-PCNF-800-assembled zinc–air battery delivered a high open circuit voltage of 1.51 V, a maximum peak power density of 164 mW·cm–2, as well as eminent rate performance, surpassing those of commercial Pt/C. This contribution offers a valuable avenue to exploit efficient metal nanoparticles-based carbon catalysts towards energy-related electrocatalytic reactions and beyond.

关键词： Fe–Nx nanoparticles     hypersaline-confinement conversion     floret-like carbon     covalent triazine polymers     oxygen reduction reaction    

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One-step ball milling-prepared nano Fe

Xingguo Guo, Qiuying Wang, Ting Xu, Kajia Wei, Mengxi Yin, Peng Liang, Xia Huang, Xiaoyuan Zhang

《环境科学与工程前沿（英文）》 2020年 第14卷 第2期 doi: 10.1007/s11783-019-1209-1

摘要： • Nano Fe2O3 and N-doped graphene was prepared via a one-step ball milling method. • The maximum power density of Fe-N-G in MFC was 390% of that of pristine graphite. • Active sites like nano Fe2O3, pyridinic N and Fe-N groups were formed in Fe-N-G. • The improvement of Fe-N-G was due to full exposure of active sites on graphene. Developing high activity, low-cost and long durability catalysts for oxygen reduction reaction is of great significance for the practical application of microbial fuel cells. The full exposure of active sites in catalysts can enhance catalytic activity dramatically. Here, novel Fe-N-doped graphene is successfully synthesized via a one-step in situ ball milling method. Pristine graphite, ball milling graphene, N-doped graphene and Fe-N-doped graphene are applied in air cathodes, and enhanced performance is observed in microbial fuel cells with graphene-based catalysts. Particularly, Fe-N-doped graphene achieves the highest oxygen reduction reaction activity, with a maximum power density of 1380±20 mW/m2 in microbial fuel cells and a current density of 23.8 A/m2 at –0.16 V in electrochemical tests, which are comparable to commercial Pt and 390% and 640% of those of pristine graphite. An investigation of the material characteristics reveals that the superior performance of Fe-N-doped graphene results from the full exposure of Fe2O3 nanoparticles, pyrrolic N, pyridinic N and excellent Fe-N-G active sites on the graphene matrix. This work not only suggests the strategy of maximally exposing active sites to optimize the potential of catalysts but also provides promising catalysts for the use of microbial fuel cells in sustainable energy generation.

关键词： Microbial fuel cells     Air cathodes     Nano Fe2O3 and nitrogen-doped graphene     Oxygen reduction reaction    

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Approaching the commercial threshold of solar water splitting toward hydrogen by III-nitrides nanowires

《能源前沿（英文）》 doi: 10.1007/s11708-023-0870-z

摘要： Approaching the commercial threshold of solar water splitting toward hydrogen by III-nitrides nanowires

关键词： threshold solar water     splitting hydrogen III    

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Self-assembled bright luminescent hierarchical materials from a tripodal benzoate antenna and heptadentate Eu(III) and Tb(III) cyclen complexes

Aramballi J. Savyasachi, David F. Caffrey, Kevin Byrne, Gerard Tobin, Bruno D'Agostino, Wolfgang Schmitt, Thorfinnur Gunnlaugsson

《化学科学与工程前沿（英文）》 2019年 第13卷 第1期   页码 171-184 doi: 10.1007/s11705-018-1762-3

摘要：

The europium heptadentate coordinatively unsaturated (Eu(III)) and the terbium (Tb(III)) 1,4,7,10-tetraazacyclododecane (cyclen) complexes 1 and 2 were used in conjunction with ligand 3 (1,3,5-benzene-trisethynylbenzoate) to form the supramolecular self-assembly structures 4 and 5; this being investigated in both the solid and the solution state. The resulting self-assemblies gave rise to metal centered emission (both in the solid and solution) upon excitation of 3, confirming its role as a sensitizing antenna. Drop-cased examples of ligand 3, and the solid forms of 4 and 5, formed from both organic and mixture of organic-aqueous solutions, were analyzed using Scanning Electron Microscopy, which showed significant changes in morphology; the ligand giving rise to one dimensional structures, while both 4 and 5 formed amorphous materials that were highly dense solid networks containing nanoporous features. The surface area (216 and 119 m2·g−1 for 4 and 5 respectively) and the ability of these porous materials to capture and store gases such as N2 investigated at 77 K. The self-assembly formation was also investigated in diluted solution by monitoring the various photophysical properties of 3–5. This demonstrated that the most stable structures were that consisting of a single antennae 3 and three complexes of 1 or 2 (e.g., 4 and 5) in solution. By monitoring the excited state lifetimes of the Eu(III) and Tb(III) ions in H2O and D2O respectively, we showed that their hydration states (the q-value) changed from ~2 to 0, upon formation of the assemblies, indicating that the three benzoates of 3 coordinated directly to the each of the three lanthanide centers. Finally we demonstrate that this hierarchically porous materials can be used for the sensing of organic solvents as the emission is highly depended on the solvent environment; the lanthanide emission being quenched in the presence of acetonitrile and THF, but greatly enhanced in the presence of methanol.

关键词： self-assembly     supramolecular chemistry     lanthanides     Eu(III) and Tb(III) complexes     luminescence     metallostars    

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New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan GAO, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Ming HOU, Zhigang SHAO

《能源前沿（英文）》 2021年 第15卷 第2期   页码 421-430 doi: 10.1007/s11708-021-0727-2

摘要： In recent years, Fe-N-C catalyst is particularly attractive due to its high oxygen reduction reaction (ORR) activity and low cost for proton exchange membrane fuel cells (PEMFCs). However, the durability problems still pose challenge to the application of Fe-N-C catalyst. Although considerable work has been done to investigate the degradation mechanisms of Fe-N-C catalyst, most of them are simply focused on the active-site decay, the carbon oxidation, and the demetalation problems. In fact, the 2e pathway in the ORR process of Fe-N-C catalyst would result in the formation of H O , which is proved to be a key degradation source. In this paper, a new insight into the effect of potential on degradation of Fe-N-C catalyst was provided by quantifying the H O intermediate. In this case, stability tests were conducted by the potential-static method in O saturated 0.1 mol/L HClO . During the tests, H O was quantified by rotating ring disk electrode (RRDE). The results show that compared with the loading voltage of 0.4 V, 0.8 V, and 1.0 V, the catalysts being kept at 0.6 V exhibit a highest H O yield. It is found that it is the combined effect of electrochemical oxidation and chemical oxidation (by aggressive radicals like H O /radicals) that triggered the highest H O release rate, with the latter as the major cause.

关键词： proton exchange membrane fuel cells (PEMFCs)     oxygen reduction reaction (ORR)     Fe-N-C catalyst     potential     H2O2     degradation    

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ion-exchanged K on the low-temperature hydrothermal stability of Cu/SAPO-34 and its synergic application with Fe

Chen Wang, Jun Wang, Jianqiang Wang, Meiqing Shen

《环境科学与工程前沿（英文）》 2021年 第15卷 第2期 doi: 10.1007/s11783-020-1322-1

摘要： Abstract • K+ hinder the structural degradation of Cu/SAPO-34 under humid condition<100°C. • K+ on Cu/SAPO-34 brings lower acidity and inferior SCR activity at high temperature. • Fe/Beta was used to compensate the low activity of Cu/SAPO-34 at high temperature. • The hybrid catalysts with KCu/SAPO-34 and Fe/Beta show a great potential for using. K ions were introduced onto Cu/SAPO-34 catalysts via the ion-exchange process in order to improve their stability under low-temperature hydrothermal aging. The changes in structure and copper-species contents of these catalysts upon hydrothermal aging were probed in order to investigate their effects on selective catalytic reduction (SCR) activity. For the fresh Cu/SAPO-34 catalysts, K ions had little influence on the chabazite framework but effected their acidities by exchanging with acid sites. After hydrothermal aging, the structural integrity and amount of active sites decreased on pure Cu/SAPO-34. While the K-loaded catalysts showed improved chabazite structure, acidity, and active site conservation with increasing K loading. However, although the 0.7 wt% K catalyst maintained the same crystallinity, active site abundance, and low-temperature SCR activity as the fresh catalyst upon aging, an apparent decrease in SCR activity at high temperature was observed because of the inevitable decrease in the number of Brönsted acid sites. To compensate for the activity disadvantage of K-loaded Cu/SAPO-34 at high temperature, Fe/Beta catalysts were co-employed with K-loaded Cu/SAPO-34, and a wide active temperature window of SCR activity was obtained. Thus, our study reveals that a combined system comprising Fe/Beta and K-loaded Cu/SAPO-34 catalysts shows promise for the elimination of NOx in real-world applications.

关键词： Selective catalytic reduction     Cu/SAPO-34 catalyst     Ion-exchanged K     Low-temperature hydrothermal stability     Fe/Beta catalyst    

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III族氮化物材料和设备的未来技术及用途

Shuji Nakamura

《工程（英文）》 2015年 第1卷 第2期   页码 161-161 doi: 10.15302/J-ENG-2015059

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标题 作者 时间 类型 操作

Advances in Fe(III) bioreduction and its application prospect for groundwater remediation: A review

Yu Jiang, Beidou Xi, Rui Li, Mingxiao Li, Zheng Xu, Yuning Yang, Shaobo Gao

期刊论文

Removal of Cu(II) and Fe(III) from aqueous solutions by dead sulfate reducing bacteria

Hong’en QUAN, He BAI, Yang HAN, Yong KANG, Jiao SUN

期刊论文

Concurrent adsorption and reduction of chromium(VI) to chromium(III) using nitrogen-doped porous carbon

期刊论文

Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

期刊论文

Comparison of different valent iron on anaerobic sludge digestion: Focusing on oxidation reduction potential, dissolved organic nitrogen and microbial community

期刊论文

Enhanced degradation of trichloroethene by calcium peroxide activated with Fe(III) in the presence of

Xiang ZHANG,Xiaogang GU,Shuguang LU,Zhouwei MIAO,Minhui XU,Xiaori FU,Muhammad DANISH,Mark L. BRUSSEAU,Zhaofu QIU,Qian SUI

期刊论文

Effect of Fe loading quantity on reduction reactivity of nano zero-valent iron supported on chelating

Jialu SHI,Shengnan YI,Chao LONG,Aimin LI

期刊论文

Process control factors for continuous microbial perchlorate reduction in the presence of zero-valent

ARTHUR Robert D.,TORLAPATI Jagadish,SHIN Kyung-Hee,CHA Daniel K.,YOON Yeomin,SON Ahjeong

期刊论文

Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer

期刊论文

One-step ball milling-prepared nano Fe

Xingguo Guo, Qiuying Wang, Ting Xu, Kajia Wei, Mengxi Yin, Peng Liang, Xia Huang, Xiaoyuan Zhang

期刊论文

Approaching the commercial threshold of solar water splitting toward hydrogen by III-nitrides nanowires

期刊论文

Self-assembled bright luminescent hierarchical materials from a tripodal benzoate antenna and heptadentate Eu(III) and Tb(III) cyclen complexes

Aramballi J. Savyasachi, David F. Caffrey, Kevin Byrne, Gerard Tobin, Bruno D'Agostino, Wolfgang Schmitt, Thorfinnur Gunnlaugsson

期刊论文

New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan GAO, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Ming HOU, Zhigang SHAO

期刊论文

ion-exchanged K on the low-temperature hydrothermal stability of Cu/SAPO-34 and its synergic application with Fe

Chen Wang, Jun Wang, Jianqiang Wang, Meiqing Shen

期刊论文

III族氮化物材料和设备的未来技术及用途

Shuji Nakamura

期刊论文