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Synthesis of todorokite by refluxing process and its primary characteristics

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Science china Earth Sciences 2004年第8期47卷 760-768页

作者： feng xionghan1, liu fan1, tan wenfeng1, liu Xiangwen2 & HU Hongqing1 1. college of resources and environment, huazhong agricultural university, wuhan 430070, china 2. Testing Center, china university of Geosciences, wuhan 430074, china 1. college of resources and environment Huazhong Agricultural University 430070 Wuhan China 2. Testing Center China University of Geosciences 430074 Wuhan China

Single phase and well-crystallined todorokite were synthesized by heating and refluxing process from birnessite as a precursor. The average chemical composition of the synthesized todorokites by refluxing for 8 h and for 24 h was Mg0.19MnO2.11(H2O)1.15 and in0.17-MnO2.10(H2O)0.88, respectively. The crystallinity of the todorokite increased and no other phase was produced with increasing refluxing period. The synthesized todorokites have the same morphologies and the similar structural characteristics with the natural todorokites and hydro-thermally synthesized samples. The chemical compositions of the synthetic tordorokites by refluxing process are close to those of todorokites synthesized by hydrothermal process, except a higher average oxidation state of Mn for the former.

关键词： todorokite,birnessite,manganese oxide,refluxing,hydrothermal,synthesis.

Pathways of birnessite formation in alkali medium

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Science china Earth Sciences 2005年第9期48卷 1438-1451页

作者： feng xionghan1, tan wenfeng1, liu fan1, HUANG Qiaoyun1 & liu Xiangwen2.1. college of resources and environment, huazhong agricultural university, wuhan 430070, china 2. Testing Center, china university of Geosciences, wuhan 430074, china 1. college of resources and environment Huazhong Agricultural University 430070 Wuhan China 2. Testing Center China University of Geosciences 430074 Wuhan China

Birnessite is a common weathering and oxidation product of manganese-bearing rocks. An O2 oxidation procedure of Mn(OH)2 in the alkali medium has been used to synthesize birnessite. Fast and powder X-ray diffraction (XRD), transmission electron microscopy (TEM), electron diffraction (ED), energy dispersed X-ray analysis (EDAX), infrared spectroscopy (IR) techniques and chemical composition analysis, Eh-pH equilibrium diagram approaches were employed to investigate the reaction process and pathways of birnessite formation. Results showed that the process of the birnessite formation could be divided into four stages: (1) forma- tion stage for hausmannite and feitknechtite, (2) stage of transformation of hausmannite and feitknechtite to buserite, (3) buserite crystal growing stage, and (4) stage of conversion of buser- ite into birnessite. Mn(OH)2 was mainly present as amorphous state only for a short initial time of oxidation reaction. In the oxidation process, buserite formed following two pathways by recrys- tallization after dissolution of the intermediates, and the transformations of the minerals de- pended on the Eh determined by the dissolved O2 concentration on their surfaces. The results are fundamental in further exploration on the mechanism of birnessite formation in the alkali medium. A great practical significance would also be expected with respect to the areas of mate- rial sciences.

关键词： birnessite, pathway of formation, reaction process, Eh-pH diagram, hausmannite, feitknechtite.

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

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

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

As(V)浓度和环境因子对硫酸盐绿锈转化的影响及其机制

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化学学报 2017年第6期75卷 608-616页

作者：王小明彭晶徐欢欢谭文峰刘凡黄巧云冯雄汉华中农业大学资源与环境学院农业部长江中下游耕地保育重点实验室武汉430070 华中农业大学农业微生物国家重点实验室武汉430070

绿锈与As(V)可共存于土壤、沉积物和地下水等缺氧环境,但As(V)如何影响绿锈转化过程和机制了解甚少.本工作通过溶液化学和光谱学方法,系统研究了As(V)浓度、pH、温度和空气流速对硫酸盐绿锈(GR)转化的影响.GR转化过程中通过吸附和共沉... 详细信息

绿锈与As(V)可共存于土壤、沉积物和地下水等缺氧环境,但As(V)如何影响绿锈转化过程和机制了解甚少.本工作通过溶液化学和光谱学方法,系统研究了As(V)浓度、pH、温度和空气流速对硫酸盐绿锈(GR)转化的影响.GR转化过程中通过吸附和共沉淀作用对As(V)有极强的去除能力,同时As(V)增强了GR的稳定性,显著影响转化产物的结晶度、矿物类型和生成机制.随As(V)浓度增加,GR氧化转化由溶解-氧化-沉淀机制向固态氧化机制过渡,产物由针铁矿和纤铁矿混合相向纯纤铁矿向纤铁矿、水铁矿和高铁绿锈混合相转变;高As(V)浓度时形成无定形FAsO_4表面沉淀.Fe/As=24时,pH 6.5~9、温度(5~45℃)和空气流速(0~0.05 m3/h)条件下纤铁矿均为主要产物,随pH和空气流速增加或温度减小纤铁矿结晶度逐渐减弱;高pH或高空气流速或低温有利于高铁绿锈和水铁矿形成,高温有利于针铁矿形成.上述结果对深入理解环境中各种铁氧化物的形成转化机制和As(V)的环境行为有重要意义.

关键词：绿锈 As(V) pH 温度空气流速转化

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2.18年和2.19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2.18年和2.19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

基于不同分析方法研究磷酸根在矿物表面吸附机制的进展

同方期刊数据库博看期刊评论

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土壤学报 2020年第1期57卷 22-35页

作者：严玉鹏王小明熊娟王慧胡震刘凡谭文峰冯雄汉华中农业大学资源与环境学院农业农村部长江中下游耕地保育重点实验室武汉430070 安徽省农业科学院土壤料研究所合肥230001

磷素是植物生长必需的营养元素,也是联系生态系统中生物与非生物作用的关键元素。对磷酸根在矿物表面吸附反应机制的深入认识,有助于了解其在陆地和水环境中的形态、迁移、转化和生物有效性。本文主要综述了磷酸根在常见(土壤)矿物表面... 详细信息

磷素是植物生长必需的营养元素,也是联系生态系统中生物与非生物作用的关键元素。对磷酸根在矿物表面吸附反应机制的深入认识,有助于了解其在陆地和水环境中的形态、迁移、转化和生物有效性。本文主要综述了磷酸根在常见(土壤)矿物表面吸附机制的研究进展。各种分析技术或方法,如OH–释放量分析、Zeta电位分析(电泳迁移率测试)、等温滴定量热法、原子力显微镜、X射线光电子能谱、红外光谱、核磁共振波谱、X射线吸收光谱、表面络合模型、量子化学计算等,均以不同方式揭示磷酸根在不同矿物体系的吸附机制。磷酸根在矿物(尤其是铁、铝氧化物)表面的吸附通常伴随着水基和羟基的交换。一般认为磷酸根在矿物表面主要形成双齿双核、单齿单核内圈络合物,且受pH的影响较大。pH以及磷酸根在矿物表面的吸附密度影响内圈络合物的质子化状态。在低pH、高磷浓度、较高反应温度、较长吸附时间,以及弱晶质矿物吸附等条件下矿物表面吸附的磷可在矿物表面转化形成含磷的表面沉淀,造成矿物溶解转化以及磷生物有效性的进一步降低。最后展望了磷酸盐在矿物-水界面吸附有关的研究热点和方向。

关键词：磷酸根矿物表面吸附表面沉淀机制

有机磷与土壤矿物相互作用及其环境效应研究进展

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土壤学报 2019年第6期56卷 1290-1299页

作者：严玉鹏王小明刘凡冯雄汉华中农业大学资源与环境学院农业农村部长江中下游耕地保育重点实验室

土壤有机磷是土壤环境中重要的磷组分,其在环境中的界面反应影响着磷素的迁移、转化、生物有效性以及环境行为。本文主要总结了土壤中典型有机磷在矿物表面的吸附-解吸、溶解-沉淀等反应特性和微观机制,以及有机磷-矿物相互作用对有机... 详细信息

土壤有机磷是土壤环境中重要的磷组分,其在环境中的界面反应影响着磷素的迁移、转化、生物有效性以及环境行为。本文主要总结了土壤中典型有机磷在矿物表面的吸附-解吸、溶解-沉淀等反应特性和微观机制,以及有机磷-矿物相互作用对有机磷形态、金属离子界面反应行为,以及矿物胶体化学稳定性与溶解转化的影响等环境效应。土壤有机磷可含多个磷酸基团,相对分子质量大,电荷密度高,通过界面反应与环境矿物发生强烈的相互作用,并影响矿物的电荷性质、共存金属离子的吸附特性、以及胶体化学稳定性。有机磷界面反应特性和机制受矿物类型和结晶度、有机磷相对分子质量、pH、温度和共存离子等因素的影响。有机磷在矿物表面的吸附密度一般随着体系pH、矿物结晶度和有机磷相对分子质量的升高而降低。有机磷一般可在矿物表面形成内圈络合物,某些情况下还存在氢键作用,甚至转化形成表面沉淀。有机磷和金属离子在矿物表面的吸附一般存在协同效应(尤其是在低pH条件下),即金属离子促进了有机磷的吸附,有机磷也促进金属离子的固定;吸附机制因反应体系而异,主要包括形成三元表面络合物和表面沉淀等,多数时候存在多种机制的共同作用。最后讨论了环境中有机磷与矿物相互作用的主要研究热点和方向。

关键词：有机磷吸附-解吸铁铝氧化物黏土矿物金属离子内圈络合物