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Enhancing microbial superoxide generation and conversion to hydroxyl radicals for enhanced bioremediation using iron-binding ligands

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Journal of Environmental Sciences 2025年第1期147卷 597-606页

作者： Yuhan Wang Xue Ning Jinsong Liang Aijie Wang jiuhui qu School of Civil and Environmental Engineering Harbin Institute of TechnologyShenzhen 518055China SFI MaREI Centre for Energy Climate and MarineEnvironmental Research InstituteUniversity College CorkCorkIreland Center for Water and Ecology Tsinghua UniversityBeijing 100084China

Harnessing bacteria for superoxide production in bioremediation holds immense promise,yet its practical application is hindered by slow production rates and the relatively weak redox potential of *** study delves into a cost-effective approach to amplify superoxide production using an Arthrobacter strain,a prevalent soil bacterial *** research reveals that introducing a carbon source along with specific iron-binding ligands,including deferoxamine(DFO),diethylenetriamine pentaacetate(DTPA),citrate,and oxalate,robustly augments microbial superoxide ***,our findings suggest that these iron-binding ligands play a pivotal role in converting superoxide into hydroxyl radicals by modulating the electron transfer rate between Fe(Ⅲ)/Fe(Ⅱ)and ***,among the tested ligands,only DTPA emerges as a potent promoter of this conversion process when complexed with Fe(Ⅲ).We identify an optimal Fe(Ⅲ)to DTPA ratio of approximately 1:1 for enhancing hydroxyl radical production within the Arthrobacter *** research underscores the efficacy of simultaneously introducing carbon sources and DTPA in facilitating superoxide production and its subsequent conversion to hydroxyl radicals,significantly elevating bioremediation ***,our study reveals that DTPA augments superoxide production in cultures of diverse soils,with various soil microorganisms beyond Arthrobacter identified as contributors to superoxide *** emphasizes the universal applicability of DTPA across multiple bacterial *** conclusion,our study introduces a promising methodology for enhancing microbial superoxide production and its conversion into hydroxyl *** findings hold substantial implications for the deployment of microbial reactive oxygen species in bioremediation,offering innovative solutions for addressing environmental contamination challenges.

关键词： Superoxide Hydroxyl radical Iron-binding ligand Bioremediation DTPA

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Research progress of novel adsorption processes in water purification: A review

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Journal of Environmental Sciences 2008年第1期20卷 1-13页

作者： qu jiuhui State Key Laboratory of Environmental Aquatic Chemistry Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China

As an effective, efficient, and economic approach for water purification, adsorbents and adsorption processes have been widely studied and applied in different aspects for a long time. In the recent years, a lot of novel adsorption processes have been developed for enhancing the efficiency of removing the organic and inorganic contaminants from water. This article reviews some new adsorbents and advanced adsorption methods that specialize in their compositions, structures, functions, and characteristics used in water treatment. The review emphasizes adsorption/catalytic oxidation process, adsorption/catalytic reduction process, adsorption coupled with redox process, biomimetic sorbent and its sorption behaviors of POPs, and modified adsorbents and their water purification efficiency.

关键词： adsorbents adsorption pollutants water purification

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Review on heterogeneous oxidation and adsorption for arsenic removal from drinking water

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Journal of Environmental Sciences 2021年第12期33卷 178-188页

作者： Ruiping Liu jiuhui qu Key Laboratory of Drinking Water Science and Technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution ControlSchool of EnvironmentTsinghua UniversityBeijing 100084China

The long term exposure of arsenic via drinking water has resulted in wide occurrence of arsenisim globally, and the oxidation of the non-ionic arsenite(As(Ⅲ)) to negatively-charged arsenate(As(Ⅴ)) is of crucial importance for the promising removal of arsenic. The chemical oxidants of ozone, chlorine, chlorine dioxide, and potassium permanganate may achieve this goal;however, their application in developing countries is sometimes restricted by the complicate operation and high cost. This review paper focuses on the heterogeneous oxidation of As(Ⅲ) by solid oxidants such as manganese oxide, and the adsorption of As(Ⅴ)accordingly. Manganese oxide may be prepared by both chemical and biological methods to achieve good oxidation performance towards As(Ⅲ). Additionally, manganese oxide may be combined with other metal oxides, e.g., iron oxide, to improve the adsorption capability towards As(Ⅴ). Furthermore, manganese oxide may be coated onto porous materials of metal organic frameworks to develop novel adsorbents for arsenic removal. To achieve the application in engineering works, the adsorbents granulation may be achieved by drying and calcination, agglomeration, and the active components may also be in situ coated onto the porous materials to maintain the oxidation and adsorption activities as much as possible. The novel adsorbents with heterogeneous oxidation and adsorption capability may be carefully designed for the removal of arsenic in household purifiers, community-level decentralized small systems, and the large-scale drinking water treatment plants(DWTPs).This review provides insight into the fundamental studies on novel adsorbents, the development of innovative technologies, and the demonstration engineering works involved in the heterogeneous oxidation and adsorption, and may be practically valuable for the arsenic pollution control globally.

关键词： Arsenic Heterogeneous oxidation Adsorption Manganese oxide Drinking water

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The progress of catalytic technologies in water purification:A review

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Journal of Environmental Sciences 2009年第6期21卷 713-719页

作者： LI Dapeng qu jiuhui National Natural Science Foundation of China Beijing 100085 China Research Center for Eeo-Envrionmental Sciences Chinese Academy of Sciences Beijing 100085 China

Catalytic technologies have been paid increasing attention in refractory pollutants abatement due to its practical and potential values in water purification. As effective and efficient approaches for water purification, Fenton＇s reagent, ozonation, electrochemical and photocatalytic methods have been widely studied and applied in different aspects and have been reviewed by several articles. In recent years, some novel catalytic processes based on above processes have been developed for enhancing the efficiency of removing the organics from water. This review emphasized on the recent development of heterogeneous catalytic ozonation, electrocatalysis in respect of novel electrodes and electro-Fenton method, photoelectrocatalysis process and photoelectron-Fenton in water purification. It was also an attempt to propose general ideas about mechanism and principle enhancing the catalytic efficiency for the degradation and the mineralization of organics in water.

关键词： catalytic technology water purification heterogeneous catalytic ozonation electrocatalysis electro-Fenton photoelectro- catalysis photoelectro-Fenton

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Pathways toward a pollution-free planet and challenges

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Frontiers of Environmental Science & Engineering 2024年第6期18卷 3-8页

作者： jiuhui qu Jiaping Chen School of Environment Tsinghua UniversityBeijing 100084China College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China

The mission of“Establishment of Zero-Pollution Earth”defined by United Nations Environment Programme aims at creation of a clean,safe and prosperous home for all human *** is of rational choice from each individual to protect our environment and demonstrates our great ambition to achieve our *** key message given in this article is that,zero pollution does not mean no discharge of pollutants and instead it can be achievable through optimizing and controlling a sound balance between pollutants discharge and capacities of decontamination through treatment and natural environmental accumulation,which can be termed as“Principle of Equilibrium”between pollution and *** on this principle,we propose and illustrate several key factors and synergistic pathways toward a pollution-free planet:quantitative determination on purification and wastewater;source control through green measures;minimization of negative side-effects;precise management through digitalized systems;and keeping sound balance between pollutants and natural *** should be noted that we would face a series of difficulties and challenges in moving forward to“Zero-Pollution Earth”.We should further develop theories,principles and tools to achieve the balance between quantity of pollutants and decontamination *** should work together to break through the bottleneck limited by“Principle of equilibrium”to establish new environmental remediation systems leading to“Zero-Pollution Earth”.

关键词： Wastewater treatment Resources Recovery Greenhouse gases Energy Pollution-free

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Optimum conditions for the formation of Al_(13) polymer and active chlorine in electrolysis process with Ti/RuO_2-TiO_2 anodes

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Journal of Environmental Sciences 2012年第2期24卷 297-302页

作者： Chengzhi Hu Huijuan Liu jiuhui qu State Key Laboratory of Environmental Aquatic Chemistry Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China.

A polyaluminum containing a high concentration of Al13 polymer and active chlorine（PACC） was successfully synthesized by a new electrochemical reactor using Ti/RuO2-TiO2 *** can potentially be used as a dual-function chemical reagent for water *** obtained results indicated that the formation of Al13 polymer and active chlorine,were the most active components in PACC responsible for coagulation and disinfection *** components were significantly influenced by electrolyte temperature,current density,and stirring *** was observed that high electrolyte temperature favored the formation of *** current density and stirring rate resulted in high current efficiency of chlorine evolution,thus favoring the generation of Al13 and active chlorine in *** the PACC（AlT = 0.5 mol/L,basicity = 2.3） was prepared at the optimum conditions by electrolysis process,the Al13 polymer and active chlorine in product reached above 70% of AlT and 4000 mg/L,*** the pilot scale experiment with raw polyaluminum chloride used as an electrolyte,PACC was successfully prepared and produced a high content of Al13 and active chlorine *** pilot scale experiment demonstrated a potential industrial approach of PACC preparation.

关键词： Al13 polymer coagulation pre-oxidation electrolysis water treatment

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Removal of pharmaceutical in a biogenic/chemical manganese oxide system driven by manganese-oxidizing bacteria with humic acids as sole carbon source

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Journal of Environmental Sciences 2023年第4期126卷 734-741页

作者： Tingming Ye Huijuan Liu Weixiao Qi jiuhui qu Key Laboratory of Drinking Water Science and Technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution ControlSchool of EnvironmentTsinghua UniversityBeijing 100084China University of Chinese Academy of Sciences Beijing 100049China

Bioaugmented sand filtration has attracted considerable attention because it can effectively remove contaminants in drinking water without additional chemical reagent *** this study,a synthesized chemical manganese dioxide (MnO_(2)) -coated quartz sand(MnQS) and biogenic manganese oxide (BioMnOx) composite system was proposed to simultaneously remove typical pharmaceutical contaminants and Mn_(2)+.We demonstrated a manganese-oxidizing bacterium,Pseudomonas ***-1,could oxidize Mn_(2)+to generate BioMnOxusing humic acids (HA) as sole carbon *** coaction of MnQS,QJX-1,and the generated BioMnOxin simultaneously removing caffeine and Mn_(2)+in the presence of HA was *** found a synergistic effect between *** and BioMnOxtogether significantly increased the caffeine removal efficiency from 32.8%(MnQS alone) and 21.5%(BioMnOxalone) to 61.2%.Meanwhile,Mn_(2)+leaked from MnQS was rapidly oxidized by QJX-1 to regenerate reactive BioMnOx,which was beneficial for continuous contaminant removal and system *** degradation intermediates of caffeine oxidized by MnQS and BioMnOxwere detected by LC-QTOF-MS analysis,which implied that caffeine was oxidized by a different ***,this work promotes the potential application of bioaugmented sand filtration in pharmaceutical removal in the presence of natural organic matter in drinking water.

关键词： Bioaugmentation MnO_(2)-coated quartz sand Manganese-oxidizing bacteria Humic acid Caffeine

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Preparation and evaluation of Zr-β-FeOOH for efficient arsenic removal

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Journal of Environmental Sciences 2013年第4期25卷 815-822页

作者： Xiaofei Sun Chun Hu jiuhui qu State Key Laboratory of Environmental Aquatic Chemistry Research Center for Eco-Environmental SciencesChinese Academy of Sciences

A Zr-β-FeOOH adsorbent for both As（Ⅴ） and As（Ⅲ） removal was prepared by a chemical co-precipitation method. Compared with β-FeOOH, the addition of Zr enhanced the adsorption capacities for As（Ⅴ） and As（Ⅲ）, especially As（Ⅲ）. The maximum adsorption capacities for As（Ⅲ） and As（Ⅴ） were 120 and 60 mg/g respectively at pH 7.0, much higher than for many reported adsorbents. The adsorption data accorded with Freundlich isotherms. At neutral pH, for As（Ⅴ）, adsorption equilibrium was approached after 3 hr, while for As（Ⅲ）, adsorption equilibrium was approached after 5 hr. Kinetic data fitted well to the pseudo second-order reaction model. As（Ⅴ） elimination was favored at acidic pH, whereas the adsorption of As（Ⅲ） by Zr-β-FeOOH was found to be effective over a wide pH range of 4-10. Competitive anions hindered the adsorption according to the sequence： phosphate 〉 silicate 〉 bicarbonate 〉 sulfate 〉 nitrate, while Ca2＋ and Mg2＋ increased the removal of As（Ⅲ） and As（Ⅴ） slightly. The high adsorption capability and good performance in other aspects make Zr-β-FeOOH a potentially attractive adsorbent for the removal of both As（Ⅲ） and As（Ⅴ） from water.

关键词： arsenic adsorbent adsorption kinetic Zr-β-FeOOH

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The Phragmites Root-Inhabiting Microbiome: A Critical Review on Its Composition and Environmental Application

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Engineering 2022年第2期8卷 42-50页

作者： Donglin Wang Yaohui Bai jiuhui qu Key Laboratory of Drinking Water Science and Technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China College of Resource and Environment University of Chinese Academy of SciencesBeijing 100049China

As widespread wetland plants,Phragmites play a vital role in water purification and are widely utilized in constructed wetlands(accounting for 15.5%of applied wetland plants)as a natural alternative to wastewater ***,despite such common applications,current understanding of the basic composition of the Phragmites root-inhabiting microbiome and the complex functions of each member of this microbiome remains incomplete,especially regarding pollution *** review summa-rizes the advances that have been made in ecological and biochemical research on the Phragmites root microbiome,including bacteria,archaea,and *** on next-generation sequencing,microbial com-munity compositions have been profiled under various environmental ***,culture-based methods have helped to clarify the functions of the microbiome,such as metal iron stabilization,organic matter degradation,and nutrient element *** unique community structure and functions are highly impacted by Phragmites lineages and environmental factors such as *** on the current understanding of the Phragmites root microbiome,we propose that synthetic microbial com-munities and iron–manganese plaque could be applied and intensified in constructed wetlands to help promote their water purification performance.

关键词： Phragmites Rhizosphere microbiome Microbial community composition Pollution remediation Constructed wetlands

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Mechanism and kinetics of 2-chlorophenol degradation in drinking water by photo-electrochemical synergic effect

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Science China Chemistry 2003年第3期46卷 259-270页

作者： SONG Qiang (宋强) qu jiuhui (曲久辉) State Key Laboratory of Environmental Aquatic Chemistry Research Center for Eco-Environmental Science Chinese Academy of Sciences Beijing 100085 China State Key Laboratory of Environmental Aquatic Chemistry Research Center for Eco-Environmental Science Chinese Academy of Sciences Beijing 100085 China

The synergic effect mechanism of photo-electrochemical oxidation is investigated in detail through reaction products and kinetics analysis in a photo-electric integral reactor with 2-chlorophenol (2-CP) as the model pollutant. A kinetics model is constructed for the combinatorial photo-electrochemical (CPE) degradation. A remarkable synergetic effect, which can significantly enhance the mineralization rate of the CPE process, is verified by the comparison of apparent kinetic constants. In the CPE process, complemental effects with multi-level and multi-pathway for pollutants degradation under our experimental conditions are speculated. It is proved that the degradation pathways are not only the simple summation of that of photolysis and electrolysis, but the formation of synergic effect through combination of several new acting approaches. The degradation efficiency is enhanced considerably by three factors, control of electrode poisoning by the UV irradiation, control of excitation and reaction trend of pollutants molecules by the UV irradiation, and control of activation effect and transfer trend by the oriented direct current (DC) electric field. An advanced oxidation system is set up through manifold of free radicals chain reactions in the CPE reactions, so that the aqueous organics can be mineralized fast and completely. It is proven by the kinetics analysis that the mineralization of organic pollutants is mainly attributed to the generation of very active hydroxyl radicals (OH@) in bulk solution from the CPE synergetic effect.

关键词： 2-chlorophenol, photo-electrochemical synergic effect, kinetics model, drinking water, microelectrolysis, UV.

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