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Simultaneous oxidation of Mn (Ⅱ) and As (Ⅲ) on cupric oxide (CuO) promotes As (Ⅲ) removal at circumneutral pH

Journal of Environmental Sciences 2023年第3期125卷 691-700页

作者： Lingqun Zeng Biao Wan Qian Wang Yupeng Yan Yuanzhi Tang xionghan feng State Environmental Protection Key Laboratory of Soil Health and Green Remediation College of Resources and EnvironmentHuazhong Agricultural UniversityWuhan 430070China School of Earth and Atmospheric Sciences Georgia Institute of TechnologyAtlantaGA 30332-0340USA Department of Environmental and Sustainable Engineering University at AlbanySUNY1400 Washington AvenueAlbanyNY 12222USA Geomicrobiology Center for Applied GeosciencesUniversity of Tuebingen72076 TuebingenGermany. Key Laboratory of Poyang Lake Watershed Agricultural Resources and Ecology of Jiangxi Province College of Land Resources and EnvironmentJiangxi Agricultural UniversityNanchang 330045China

Oxidation of Mn (Ⅱ) or As(Ⅲ) by molecular oxygen is slow at pH<9,while they can be catalytically oxidized in the presence of oxide minerals and then removed from contaminated ***,the reaction mechanisms on simultaneous oxidation of Mn(Ⅱ) and As (Ⅲ)on oxide mineral surface and their accompanied removal efficiency remain *** study compared Mn (Ⅱ) oxidation on four common metal oxides (γ-Al_(2)O_(3),CuO,α-Fe2O_(3)and ZnO) and investigated the simultaneous oxidation and removal of Mn (Ⅱ) and As (Ⅲ) through batch experiments and spectroscopic *** the tested oxides,CuO and α-Fe2O_(3)possess greater catalytic activity toward Mn (Ⅱ) *** and removal kinetics of Mn (Ⅱ) and As (Ⅲ) on CuO indicate that O_(2)is the terminal electron acceptor for Mn (Ⅱ) and As (Ⅲ) oxidation on CuO,and Mn (Ⅱ) acts as an electron shuttle to promote As (Ⅲ) oxidation and *** main oxidized product of Mn (Ⅱ) on CuO is high-valent MnO_(x)*** newly formed Mn (Ⅲ) or Mn (IV) phases promote As (Ⅲ) oxidation on CuO at circumneutral pH 8 and is reduced to Mn (Ⅱ),which may be then released into *** study provides new insights into metal oxide-catalyzed oxidation of pollutants Mn (Ⅱ) and As (Ⅲ) and suggests that CuO should be considered as an efficient material to remediate Mn (Ⅱ) and As(Ⅲ)contamination.

关键词： Simultaneous oxidation Mn(II) As(III) CuO Metal oxides

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Interactions of organic phosphorus with soil minerals and the associated environmental impacts: A review

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Pedosphere 2023年第1期33卷 74-92页

作者： Yupeng YAN Biao WAN Rui JIANG Xiaoming WANG Hui WANG Shuai LAN Qin ZHANG xionghan feng Key Laboratory of Poyang Lake Watershed Agricultural Resources and Ecology of Jiangxi Province College of Land Resources and EnvironmentJiangxi Agricultural UniversityNanchang 330045China Key Laboratory of Arable Land Conservation(Middle and Lower Reaches of Yangtze River) Ministry of Agriculture and Rural AffairsCollege of Resources and EnvironmentHuazhong Agricultural UniversityWuhan 430070China Geomicrobiology Center for Applied GeosciencesUniversity of TuebingenTuebingen 72076Germany Soil and Fertilizer Institute Anhui Academy of Agricultural SciencesHefei 230001China

As an important part of the soil phosphorus(P)pool,organic P(OP)is widely found in terrestrial and aquatic environments(e.g.,soils and sediments).The interfacial behavior of OP on natural minerals affects the transport,transformation,and bioavailability of P in the *** paper reviews the processes involving adsorption-desorption,dissolution-precipitation,and enzymatic/mineral-mediated hydrolysis of OP at the mineral-water interface,and their subsequent effects on OP speciation and mineral colloidal stability/*** sorption mechanisms of OP on natural minerals mainly include surface complexation and precipitation,which are controlled by factors such as mineral identity and crystallinity,the relative molecular weight of OP,reaction pH,ionic strength,temperature,and co-existing ligands or *** desorption amount and rate of OP from minerals are determined by the mineral identity,desorbent type,pre-sorption time,OP species,reaction pH,number of desorption cycles,and redox *** interactions between OP and minerals affect the sorption of co-existing metal ions and the stability of the *** effect of minerals on the enzymatic hydrolysis of OP sorbed on mineral surfaces depends on the mineral identity and OP *** minerals also exhibit catalytic activity to promote the cleavage of C–O–P bonds and OP *** provide an overview of state-of-the-art techniques currently applied in environmental OP *** main challenges and future research directions are also summarized to further explore OP interactions with natural minerals in complex environmental settings.

关键词： hydrolysis interfacial reactions natural minerals sorption surface complexation surface precipitation

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Structure and properties of Co-doped cryptomelane and its enhanced removal of Pb^(2+) and Cr^(3+) from wastewater

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Journal of Environmental Sciences 2015年第8期27卷 77-85页

作者： Hui Li Fan Liu Mengqiang Zhu xionghan feng Jing Zhang Hui Yin Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtse River) Ministry of AgricultureCollege of Resources and Environment Huazhong Agricultural University Department of Ecosystem Science and Management University of Wyoming Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences

Cryptomelane is a reactive Mn oxide and has been used in removal of heavy metal from wastewaters. Co-doped cryptomelane was synthesized by refluxing at ambient pressure and characterized by powder X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy and extended X-ray absorption fine structure spectroscopy, and its performances for removal of Pb^2＋ and Cr^3＋ from aqueous solutions were investigated. Co doping has a negligible effect on the structure and morphology of cryptomelane but increases the specific surface area and Mn average oxidation state. Mn and Co K-edge extended X-ray absorption fine structure spectroscopy（EXAFS） analysis shows that Co barely affects the atomic coordination environments of Mn, and distances of edge- and corner-sharing Co–Me（Me_Co, Mn） pairs are shorter than those of the corresponding Mn–Me pairs, implying the replacement of framework Mn（III） by Co（III）. These Co-doped cryptomelanes can quickly oxidize Cr3＋to be HCr O4-and remove 45%–66% of the total Cr in the reaction systems by adsorption and fixation, and they have enhanced Pb2＋adsorption capacities. Thus these materials are promising adsorbents for heavy metal remediation. The results demonstrate the design and modification of environmental friendly Mn oxide materials and can help us understand the interaction mechanisms of transition metals with Mn oxides.

关键词： Cryptomelane Co doping EXAFS Pb2+adsorption Cr^3+oxidation

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Roles of manganese oxides in degradation of phenol under UV-Vis irradiation:Adsorption,oxidation,and photocatalysis

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Journal of Environmental Sciences 2011年第11期23卷 1904-1910页

作者： Qin Zhang Xiaodi Cheng Chen Zheng xionghan feng Guohong Qiu Wenfeng Tan Fan Liu Key Laboratory of Subtropical Agriculture and Environment Ministry of Agriculture College of Resources ＆ Environment Huazhong Agricultural University Wuhan 430070 China College of Land Resource and Environment Jiangxi Agricultural University Nanchang 330045 China

Manganese oxides are known as one type of semiconductors,but their photocatalysis characteristics have not been deeply *** this study,photocatalytic degradation of phenol using several synthesized manganese oxides,i.e,acidic birnessite （BIR-H）,alkaline birnessite （BIR-OH）,cryptomelane （CRY） and todorokite （TOD）,were comparatively *** elucidate phenol degradation mechanisms,X-ray diffraction （XRD）,ICP-AES （inductively coupled plasma-atomic emission spectroscopy）,TEM （transmission electronic microscope）,N 2 physisorption at 77 K and UV-visible diffuse reflectance spectroscopy （UV-Vis DRS） were employed to characterize the structural,compositional,morphological,specific surface area and optical absorption properties of the manganese *** 12 hr of UV-Vis irradiation,the total organic carbon （TOC） removal rate reached 62.1%,43.1%,25.4%,and 22.5% for cryptomelane,acidic birnessite,todorokite and alkaline birnessite,*** to the reactions in the dark condition,UV- Vis exposure improved the TOC removal rates by 55.8%,31.9%,23.4% and 17.9%.This suggests a weak ability of manganese oxides to degrade phenol in the dark condition,while UV-Vis light irradiation could significantly enhance phenol *** manganese minerals exhibited photocatalytic activities in the order of：CRY BIR-H TOD *** may be three possible mechanisms for photochemical degradation：（1） direct photolysis of phenol;（2） direct oxidation of phenol by manganese oxides;（3） photocatalytic oxidation of phenol by manganese *** oxidation of phenol appeared to be the dominant mechanism.

关键词： manganese oxides adsorption oxidation photocatalysis degradation phenol

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Oxidation of As^Ⅲ by Several Manganese Oxide Minerals in Absence and Presence of Goethite

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Acta Geologica Sinica(English Edition) 2006年第2期80卷 249-256页

作者： feng xionghan TAN Wenfeng LIU Fan Huada Daniel RUAN HE Jizheng Key Lab of Subtropical Agriculture Resource ＆ Environment Ministry of Agiculture Huazhong Agricultural University Wuhan Hubei 430070 China Castco Testing Centre 29A On Chuen Street Fanling N. T. Hong Kong China Research Centre for Eco-Environmental Sciences Chinese Academy of Sciences 18 Shuangqing Road Beijing 100085 China

Oxidation of As^Ⅲ by three types of manganese oxide minerals affected by goethite was investigated by chemical analysis, equilibrium redox, X-ray diffraction （XRD） and transmission electron microscopy （TEM）. Three synthesized Mn oxide minerals of different types, birnessite, todorokite, and hausmannite, could actively oxidize As^Ⅲ to Asv, and greatly varied in their oxidation ability. Layer structured birnessite exhibited the highest capacity of As^Ⅲ oxidation, followed by the tunnel structured todorokite. Lower oxide hansmannite possessed much low capacity of As^Ⅲ oxidation, and released more Mn^2＋ than birnessite and todorokite during the oxidation. The maximum amount of Asv produced during the oxidation of As^Ⅲ by Mn oxide minerals was in the order： birnessite （480.4 mmol/kg）〉 todorokite （279.6 mmol/kg）〉 hansmannite （117.9 mmol/kg）. The oxidation capacity of the Mn oxide minerals was found to be relative to the composition, crystallinity, and surface properties. In the presence of goethite oxidation of As^Ⅲ by Mn oxide minerals increased, with maximum amounts of Asv being 651.0 mmol/kg for birnessite, 332.3 mmol/kg for todorokite and 159.4 mmol/kg for hansmannite. Goethite promoted As^Ⅲ oxidation on the surface of Mn oxide minerals through adsorption of the Asv produced, incurring the decrease of Asv concentration in solutions. Thus, the combined effects of the oxidation （by Mn oxide minerals）-adsorption （by goethite） lead to rapid oxidation and immobilization of As in soils and sediments and alleviation of the As^Ⅲ toxicity in the environments.

关键词： Mn oxide mineral goethite oxidation As^Ⅲ Asv

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Effects of Al^(3+)doping on the structure and properties of goethite and its adsorption behavior towards phosphate

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Journal of Environmental Sciences 2016年第7期28卷 18-27页

作者： Wei Li Longjun Wang Fan Liu Xiaoliang Liang xionghan feng Wenfeng Tan Lirong Zheng Hui Yin Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtse River) Ministry of Agriculture College of Resources and Environment Huazhong Agricultural University CAS Key Laboratory of Mineralogy and Metallogeny Guangzhou Institute of Geochemistry Chinese Academy of Sciences Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences

Al substitution in goethite is common in soils, and has strong influence on the structure and physicochemical properties of goethite. In this research, a series of Al-doped goethites were synthesized, and characterized by powder X-ray diffraction（XRD）, transmission electron microscopy（TEM）, X-ray photoelectron spectroscopy（XPS）, Fourier transform infrared spectroscopy（FT-IR） and extended X-ray absorption fine structure（EXAFS）spectroscopy. The adsorption behavior of these samples towards PO43-was also investigated. Characterization results demonstrated that increasing Al content in goethite led to a reduction in crystallinity, increase in specific surface area（SSA）, and morphology change from needle-like to granular. Rietveld structure refinement revealed that the lattice parameter a remained almost constant and b slightly decreased, but c was significantly reduced, and the calculated crystal density increased. EXAFS analysis demonstrated that the Fe（Al）–O distance in the structure of the doped goethites was almost the same, but the Fe–Fe（Al） distance decreased with increasing Al content. Surface analysis showed that, with increasing Al content, the content of OH groups on the mineral surface increased. The adsorption of phosphate per unit mass of Al-doped goethite increased, while adsorption per unit area decreased owing to the decrease of the relative proportion of（110） facets in the total surface area of the minerals. The results of this research facilitate better understanding of the effect of Al substitution on the structure and properties of goethite and the cycling of phosphate in the environment.

关键词： Goethite Al substitution XRD XAFS Adsorption

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Strategies for improving fertilizer phosphorus use efficiency in Chinese cropping systems

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Frontiers of Agricultural Science and Engineering 2019年第4期6卷 341-347页

作者： Gu feng Jingping GAI xionghan feng Haigang LI Lin ZHANG Keke YI Jialong LV Yiyong ZHU Li TANG Yilin LI College of Resources and Environmental Sciences China Agricultural UniversityBeijing 100193China College of Resources and Environment Huazhong Agricultural UniversityWuhan 430070China Key Laboratory of Plant Nutrition and Fertilizer Ministry of AgricultureInstitute of Agricultural Resources and Regional PlanningChinese Academy of Agricultural SciencesBeijing 100081China College of Natural Resources and Environment Northwest A&F UniversityYangling 712100China College of Resources and Environmental Sciences Nanjing Agricultural UniversityNanjing 210095China College of Resources and Environmental Sciences Yunnan Agricultural UniversityKunming 650201China State Key Laboratory of Soil and Sustainable Agriculture Institute of Soil ScienceChinese Academy of SciencesNanjing 210008China

A four-year project,entitled"The mechanisms of fraction transformation and high use efficiency of P fertilizer in Chinese cropping systems"commenced in *** project was established to answer three key questions and looked at 17 cropping systems on ten ***,we asked what are the dynamics of transformation,fixation and mobilization of P fertilizers in soil-cropping systems?Second,what are the mechanisms of soil-cropmicrobe interactions by which P fertilizer can be efficiently used?Third,how to manipulate the processes of P use in cropping systems?The targets of this project are(1)to explore the mechanisms of P fixation,the pathways of loss of P availability and the threshold of migration of fertilizer P in the field;(2)to uncover mechanisms by which soil legacy P is mobilized through root physiological and morphological processes and through arbuscular mycorrhizal fungi and P-solubilizing bacteria in rhizosphere and hyphosphere;(3)to estimate the biological potential of crops for high efficiency P absorption and use;(4)to innovate new approaches for improving the efficiency of P *** outcomes will provide theoretical support for setting standards for limitation of P fertilizer application rate in the main cropping zones of China.

关键词： fixation mobilization phosphorus fertilizer rhizosphere transformations utilization

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Relation of lead adsorption on birnessites with different average oxidation states of manganese and release of Mn^(2+)/H^+/K^+

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Journal of Environmental Sciences 2009年第4期21卷 520-526页

作者： ZHAO Wei, feng xionghan, TAN Wenfeng, LIU Fan, DING Shuwen Key Laboratory of Subtropical Agriculture Resource & Environment, Ministry of Agriculture of China, Huazhong Agricultural University, Wuhan 430070, China. Key Laboratory of Subtropical Agriculture Resource & Environment Ministry of Agriculture of China Huazhong Agricultural University Wuhan 430070 China

The characteristics of Pb^2＋ adsorption on the surface of birnessites with different average oxidation states （AOS） of Mn, synthesized under acidic and alkali conditions, were investigated. The results indicated that the amount of adsorbed Pb^2＋ increased with the increase of Mn AOS in birnessites. The amount of Pb〉 adsorbed positively correlated with the amount of released Mn^2＋, H^＋, and K^＋（r = 0.9962 〉 0.6614, n = 14, ct = 0.01）. The released Mn^2＋, H^＋, and K^＋ were derived mostly from the corresponding cations adsorbed on the vacant sites. The maximum amount of adsorbed Pb^2＋ increased with the increasing vacant cation sites, leading to an increase of the total amount of released Mn^2＋, H^＋, and K^＋, and the increased likelihood for two Pb^2＋ adsorbed in the region of one side of a vacant site.

关键词： pb^2+ adsorption birnessite vacant site cation release

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华中地区水旱轮作酸性土磷、铁形态转化及机理

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农业环境科学学报 2022年第9期41卷 1993-2003页

作者：崔宸阳严玉鹏王小明刘凡冯雄汉华中农业大学资源与环境学院武汉430000 江西农业大学国土资源与环境学院南昌330000

为探讨华中地区水旱轮作体系酸性土壤磷与铁的形态转化以及磷生物有效性变化,本研究于2018年和2019年水稻收获后采集该区域典型酸性红壤(低磷铁比)和黄棕壤(高磷铁比),采用张守敬-杰克逊无机磷分级方法和梯度扩散薄膜(DGT)技术,对干湿... 详细信息

为探讨华中地区水旱轮作体系酸性土壤磷与铁的形态转化以及磷生物有效性变化,本研究于2018年和2019年水稻收获后采集该区域典型酸性红壤(低磷铁比)和黄棕壤(高磷铁比),采用张守敬-杰克逊无机磷分级方法和梯度扩散薄膜(DGT)技术,对干湿交替培养样品磷形态、生物有效性磷(DGT-P)与铁(DGT-Fe)、Fe(Ⅱ)及无定形氧化铁(Fe)等进行定量分析。结果表明:淹水过程中黄棕壤和红壤pH逐渐升高趋于中性;二者氧化还原电势(Eh)在淹水期间降低,土壤环境呈明显的还原条件。淹水过程黄棕壤和红壤中Fe与Fe均增加,干燥后均明显降低。黄棕壤与红壤磷形态以铁结合态磷(Fe-P)与闭蓄态磷(Oc-P)为主,干湿交替过程中黄棕壤Oc-P向Fe-P转化,红壤Fe-P向Oc-P转化。在水-土界面以下120 mm土壤垂直剖面内,黄棕壤DGT-P和DGT-Fe释放水平先增加后减少;红壤DGT-Fe增加,DGT-P减少,黄棕壤P和Fe的同步释放相关性更显著。研究表明,干湿交替条件下酸性土壤磷形态主要是Fe-P与Oc-P之间转化,低P/Fe红壤以磷闭蓄化为主,高P/Fe黄棕壤Fe-P增加,以铁吸附磷为主;淹水导致DGT-P含量增加,生物有效性增加;干燥过程磷闭蓄化加深,但磷有效性并无明显降低,这与土壤磷水平有关。

关键词：磷氧化铁干湿交替磷铁比梯度扩散薄膜技术磷生物有效性

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不同环境条件下Mn(Ⅱ)在磁铁矿表面的催化氧化

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江西农业大学学报 2022年第4期44卷 1044-1056页

作者：秦张杰胡康生梁丰冯雄汉张嵚何小林兰帅江西农业大学国土资源与环境学院/江西省鄱阳湖流域农业资源与生态重点实验室江西南昌330045 华中农业大学资源与环境学院湖北武汉430070 江西省农业技术推广中心江西南昌330045

【目的】土壤中活性很强的铁和锰变价元素在水旱交替的环境下易形成不同的铁锰共生体,进而参与有机质氧化降解和污染金属离子形态及毒性变化等反应。其中锰在土壤溶液中主要以离子态Mn(Ⅱ)存在,其常在铁氧化物表面氧化沉淀,形成不同的... 详细信息

【目的】土壤中活性很强的铁和锰变价元素在水旱交替的环境下易形成不同的铁锰共生体,进而参与有机质氧化降解和污染金属离子形态及毒性变化等反应。其中锰在土壤溶液中主要以离子态Mn(Ⅱ)存在,其常在铁氧化物表面氧化沉淀,形成不同的铁锰共生体。磁铁矿是土壤中广泛存在的一种铁氧化物,但关于Mn(Ⅱ)在其表面的催化氧化途径与机制鲜少报道。【方法】以磁铁矿为研究对象,采用动力学氧化实验和长期老化实验,并结合X-射线衍射(XRD)光谱技术手段,阐述了不同环境中磁铁矿催化作用下Mn(Ⅱ)的氧化产物数量及类型,同时将其与具备不同带隙能的水铁矿和针铁矿的催化作用进行比较,探讨磁铁矿对Mn(Ⅱ)氧化的催化特性与两者的异同,进而阐明磁铁矿催化Mn(Ⅱ)氧化的途径和具体机制。【结果】Mn(Ⅱ)在磁铁矿催化作用下的主要产物为水锰矿和布塞尔矿,且腐殖质AQDS的加入可同时显著提高Mn(Ⅱ)氧化的速率和程度。其次,相较于Mn(Ⅱ)初始反应浓度为8 mmol/L的体系,Mn(Ⅱ)初始反应浓度增大到24 mmol/L时,其氧化产物的量增多,结晶度增强,尤其是含Mn(Ⅳ)的氧化物。另外,当pH由7增大到9,体系Mn(Ⅱ)的去除率显著增大,且产物除了布塞尔矿和水锰矿外还出现了大量的黑锰矿。最后,相较于60℃反应条件,常温反应温度更利于Mn(Ⅱ)催化氧化速率的提高、锰氧化物产量的增多和结晶的增强。【结论】Mn(Ⅱ)在磁铁矿表面的催化氧化应该具有界面催化、电化学催化和芬顿反应产物氧化催化3个途径。磁铁矿同时含有的Fe(Ⅱ)/Fe(Ⅲ)及其较强的半导体特性会使3个途径的实现都更加容易。上述结论为了解和预测富铁锰土壤环境下两者耦合的地球化学行为,以及与之共存物质的迁移转化和环境归趋奠定理论基础。

关键词：磁铁矿 Mn(Ⅱ) 催化氧化 AQDS pH 温度

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