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dc.description.abstract植物從土壤中攝取養分受到植物根系與土壤之物理、生物化學性質交互作用的複雜過程影響。單子葉禾本科植物的根分泌可鉗合三價鐵且對鐵親和力高的載鐵物質 (phytosiderophores, PSs) 來溶解土壤中的鐵,進而影響磷等其他營養元素在土壤中的移動。本研究目的為:探討載鐵物質之一的去鐵胺 (desferrioxamine-B, DFO-B) 與含鐵、鋁或磷礦物 (紅磷鐵礦 (strengite, FePO4∙2H2O) 、磷酸鋁石 (variscite, AlPO4∙2H2O)) 與已吸附磷的針鐵礦 (goethite, α-FeOOH)、水鋁礦 (gibbsite, α-Al(OH)3)、赤鐵礦 (hematite, α-Fe2O3) 交互作用下礦物表面溶出的情形,進而來瞭解載鐵物質在植物吸收磷可能扮演的角色。實驗結果顯示:擬一級速率方程式適合用於說明DFO-B促進含鐵、鋁或磷礦物的溶解情形,其中溶解的速率常數與DFO-B被吸附的量有相關性。在 pH 4 下,DFO-B隨著針鐵礦、水鋁礦與赤鐵礦表面所吸附磷含量的增加而加速礦物的溶解速率。然而,在 pH 9下,礦物表面磷吸附量的增加卻抑制礦物表面的溶出,可能是因 pH 9 環境下,磷酸根在礦物表面形成了較穩定的結構,使DFO-B不易溶解礦物表面。根據 Arrhenius 方程式,在不同溫度與 pH 下,DFO-B與不同礦物反應之活化能 (activation energies, Ea) 也顯示:在 pH 9 下的反應之活化能高於 pH 4 下的活化能,表示磷酸根與礦物表面在 pH 9 下形成了DFO-B難以鉗合的形式,進而抑制了礦物表面的溶解。針對含鐵磷或鋁磷的礦物研究發現:DFO-B的存在促進紅磷鐵礦與磷酸鋁石溶解的現象。其中,因為磷酸鋁石表面吸附較多的DFO-B,造成磷酸鋁石溶解速率較紅磷鐵礦溶解速率快。zh_TW
dc.description.abstractNutrient uptake of plants from soil is a complex process determined by the interactions of the plant roots with the soil and the combination of physical and biochemical properties of the soil. The roots of graminaceous monocots secrete phytosiderophores (PSs), which are chelating agents with a high affinity for Fe(III), to dissolve Fe(III) in soil. The release of PSs can potentially mobilize nutrients, such as P, associated with Fe in soil. To understand the potential role of PSs in regulating the P acquisition of plants, this study investigated the interactions of desferrioxamine-B (DFO-B) siderophore with some major Fe, Al and P - containing minerals, including strengite (FePO4∙2H2O), variscite (AlPO4∙2H2O), and phosphate-loaded goethite (α-FeOOH), gibbsite (α-Al(OH)3) and hematite (α-Fe2O3). The pseudo-first-order rate constant was determined for the DFO-B – promoted dissolution of each mineral and subsequently normalized to the corresponding amount of adsorbed siderophore to calculate the mass-normalized dissolution rate. Apparent activation energies (Ea) were calculated from the mass-normalized dissolution rates of each mineral obtained at different temperatures using the Arrhenius equation. Increasing the loading of adsorbed P on all three oxides (i.e., goethite, hematite and gibbsite) resulted in an increase in the dissolution rates of the minerals but a decrease in dissolution rates at pH 9. The rate inhibition at pH 9 is attributed to the presence of binuclear surface complexes, in which much more energy is required to remove simultaneously two center atoms from the crystalline lattice than it is to remove solely one center (i.e. in the case of mononuclear complexes at pH 4). Higher Ea values at pH 9 than at pH 4, supports our hypothesis that the existence of stronger adsorbed phosphate complexes hinder the smooth release of the metal-ion-center. DFO-B -promoted dissolution of strengite and variscite studies show that dissolution was enhanced in the presence of DFO-B. Higher dissolution rates for variscite than strengite is attributed to the higher adsorbed concentrations of DFO-B on variscite than on strengite.en_US
dc.description.tableofcontents摘要 i ABSTRACT ii ACKNOWLEDGMENTS iv TABLE OF CONTENTS vi LIST OF TABLES ix LIST OF FIGURES xiii 1. INTRODUCTION 1 1.1 Background 1 1.2 Objectives 5 2. LITERATURE REVIEW 7 2.1 Metal Oxides in Soil 7 2.2 The Structures of the Applied Minerals 9 2.2.1 Goethite 9 2.2.2 Hematite 10 2.2.3 Gibbsite 12 2.2.4 Strengite and Variscite 13 2.3 Phosphate 14 2.3.1 Uncomplexed Phosphate in Aqueous Solution 15 2.3.2 Adsorption of Phosphate on Metal Oxides 16 2.3.3 pH Dependency 18 2.4 Siderophores 19 2.4.1 Chemistry of Siderophores 23 2.5 Mineral Dissolution 26 2.5.1 Rate Laws 27 2.5.2 Temperature Dependence 28 3. MATERIALS AND METHODS 31 3.1 Chemicals 31 3.2 Mineral phases Synthesis/ Mineralogical Samples synthesis 31 3.2.1 Goethite (α-FeOOH) 31 3.2.2 Hematite (α–Fe2O3) 32 3.2.3 Variscite (AlPO4 ‧ 2H2O) 32 3.2.4 Strengite (FePO4‧2H2O) 33 3.2.5 Gibbsite [γ-Al (OH)3] 33 3.3 X-ray Diffraction Analyses 34 3.4 Adsorption Experiments 34 3.4.1 Maximum Phosphorus Adsorption Capacities of Minerals 34 3.4.2 Adsorption of DFO-B on Mineral Surfaces 38 3.5 Steady-State Ligand-promoted Dissolution of Minerals in the Presence of DFO-B 38 3.6 Analysis Methods 39 4. RESULTS 41 4.1 Mineral Characterization 41 4.2 Adsorption of Phosphates on Oxides 43 4.3 Dissolution Kinetics 46 4.4 Dissolution of Strengite and Variscite 60 4.5 Phosphate Desorption Kinetics 66 4.6 Effect of Adsorbed Phosphate on Dissolution 72 4.7 Temperature Effect 74 4.8 Temperature dependence of DFO-B - promoted dissolution of strengite and variscite. 88 5. DISCUSSION 90 5.1 Phosphate Adsorption 90 5.2 DFO-B Adsorption and –promoted Dissolution 91 5.3 pH-Dependence and the Influence of Phosphate 92 5.4 Dissolution of Strengite and Variscite. 98 5.5 Temperature Dependence of Dissolution 99 6. CONCLUSIONS 108 REFERENCES 109 APPENDIX 132zh_TW
dc.subjectDesferrioxamine-B (DFO-B)en_US
dc.subjectligand-promoted dissolutionen_US
dc.subjectactivation energyen_US
dc.title載鐵物質 (DESFERRIOXAMINE-B) 與含磷鐵鋁礦物之間的化學反應機制zh_TW
dc.typeThesis and Dissertationzh_TW
item.openairetypeThesis and Dissertation-
item.fulltextno fulltext-
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