礦業發展過程中所產生之廢礦經風化作用可進一步衍生出酸性礦山排水（acid mine drainage; AMD），其所含高濃度有毒元素及後續形成之大量含水氧化鐵沉澱皆可能對環境生態及人體健康造成影響。瞭解AMD及其沉澱物之特性、危害性及再利用性有助於對其之預防與整治外，也有利於環境之永續發展。本研究以Ｘ光繞射、傅利葉轉換紅外線光譜、電子顯微鏡和感應藕合電漿放射光譜等方法分析金瓜石酸性礦山排水（pH = 2.8）及其與溪水（pH = 6.0）和海水（pH = 8.0）混染過程中之水化學特性以及所沉澱物質之礦物學特徵，以探討其中之元素遷移行為與微奈米硫酸氫氧氧化鐵物質沉澱作用之關係，並考量瀑布地形與季節變化之影響。
金瓜石黃金瀑布、濂洞溪下游河床和本山七坑坑口及其溝渠流徑之表層沉澱物以具刺蝟狀形貌之四方硫酸纖鐵礦（schwertmannite）球粒集合體為主要組成。酸性礦山排水中鐵和砷濃度由上游往下游相對其他金屬離子濃度大幅減少，顯示四方硫酸纖鐵礦為現地沉澱，並且具有顯著之砷吸收能力。酸性礦山排水受瀑布曝氣效應影響可加速其二價鐵氧化速率，使得瀑布段之二價鐵氧化速率及模式速率常數（0.5-2.0×10-7 mol L-1 sec-1和1.1-5.7×10-3 sec-1）及鐵（四方硫酸纖鐵礦）沉澱作用之速率及模式速率常數（1.5-7.3×10-7 mol L-1 sec-1和1.9-2.4×10-7 mol L-1 sec-1）較下游溪流段快或高出1至2個量級，並具有高砷吸收率（4.7-6.3×10-9 mol L-1 sec-1）。溪流段夏季之速率受溫度影響比冬季高出4至5倍，但瀑布段冬季之速率與夏季差異不大，可歸因於冬季水流量大時瀑布曝氣效應可增強鐵沉澱速率。
草酸銨溶樣分析結果顯示黃金瀑布表層四方硫酸纖鐵礦之平均化學式為Fe16O16(OH)11(SO4)2.5•16H2O，並含有2794 ppm砷、439 ppm鋁、115 ppm銅及23 ppm鉻。隨著沉澱深度增加，四方硫酸纖鐵礦先逐漸轉變成低結晶度針鐵礦，再轉變成較高結晶度針鐵礦。同時沉澱物整體之Al/Fe、Cr/Fe與S/Fe莫耳比值減少，As/Fe無顯著變化，Cu/Fe增加，顯示四方硫酸纖鐵礦轉變過程中，鋁、鉻與硫酸根被釋放至溶液中，砷可被保留，銅則被富集。低結晶度針鐵礦之形成對相轉變過程中元素之遷移及滯留行為有顯著影響。
四方硫酸纖鐵礦之沉澱可使金瓜石酸性礦山排水中砷及金屬濃度往下游衰減，但仍約有每年3235公噸鐵、737公噸鋁、191公噸銅及2.4公噸砷排放至濂洞灣中，並且在海水表層沉澱大量懸浮粒。入海口海水（酸鹼值小於4）所形成短柱狀懸浮奈米微粒，乃是四方硫酸纖鐵礦及少量針鐵礦所組成；而濂洞灣近岸海水（酸鹼值大於5.5）所形成球狀懸浮奈米微粒，屬非晶質水合氧化鐵、鋁，並含有微量四方硫酸纖鐵礦。隨著水體酸鹼值升高，海水懸浮粒之組成從相對富含砷、鉻、鉛、鐵及硫轉而相對富含鋁、矽、銅、鋅、錳、鎳、鈷及鎘。金瓜石酸性礦山排水之水體化學及沉澱物組成變化主要受控於（硫酸）氫氧氧化鐵、鋁物質沉澱與水體酸鹼值之改變，以及中和過程中金屬元素逐步於不同階段共沉澱或被吸附作用。這些過程可延緩或降低金瓜石地區酸性礦山排水對環境污染之影響，然而富含重金屬之海水懸浮粒的後續脫附、轉變或溶解作用值得追蹤和關注。

Acid mine drainage (AMD) often occurs as a result of weathering of mine wastes in mining areas. Migration of high concentrations of toxic elements and subsequent precipitation of hydrous iron oxides in AMD areas could pose great threats on environmental quality, ecosystem, and human health. Analyzing the characteristics and reactions of AMDs and their precipitates is fundamentally important for understanding geochemical reactions in such an environment. It can also provide parameters essential for contamination assessment and remediation crucial to environmental sustainability.
Variations of water chemistry and precipitate mineralogy during mixing of acid mine drainage (AMD) (pH = 2.8) with a creek (pH = 6.0) and seawater (pH = 8.0) were investigated by XRD, SEM, TEM, IR, ICP analysis to discuss the relationships between metal mobility and precipitation of micro-nanometric iron oxyhydroxysulfate minerals in the Chinkuashih AMD area in consideration of reaction kinetics, waterfall effects, and seasonal variations. In terms of Fe(II) oxidation and Fe(III) precipitation in the creek section, the summer rates were 4-5 times higher than the winter rates, largely attributed to a temperature effect. In contrast, the seasonal differences in rate and rate constant were small in the waterfall section due to waterfall aeration which enhanced the Fe precipitation rate when the flow rate was large in the winter.
Radiating aggregates of schwertmannite with an overall hedgehog morphology occurred as a principal constituent of the surface precipitates on the bedrocks of Golden Falls and downstream Lian-Dong Creek and a channel at the Penshan 7th adit. Remarkable downstream reduction of Fe and As concentrations with respect to other metals in the water suggested in-situ precipitation of schwertmannite associated with an arsenate sorption process. Under the influence of water aeration, the waterfall section showed up to 1-2 orders of magnitude faster rates and higher model rate constants of Fe(II) oxidation (6.1-6.7×10-6 mol L-1 sec-1and 2.7-2.9×10-2 sec-1) and Fe (schwertmannite) precipitation (1.7-2.1×10-6 mol L-1 sec-1and 3.5-4.1×10-7 mol L-1 sec-1) than the creek section, and had a high As sorption rate (4.7-6.3×10-9 mol L-1 sec-1).
The schwertmannite in the surface precipitate at Golden Falls had an chemical formula of Fe16O16(OH)11(SO4)2.5•16H2O, and contained 2794 ppm As, 439 ppm Al, 115 ppm Cu, and 23 ppm Cr on average. With increasing depth, a transformation from schwertmannite, poorly crystalline goethite, to better crystallized goethite was characterized. In addition, bulk analyses indicated decreases of Al/Fe, Cr/Fe and S/Fe molar ratios and an increase of Cu/Fe and with rather small variations in As/Fe as the sample depth increased. The data suggested that Al, Cr and sulfate were released, As was retained, and Cu was accumulated, and that the formation of poorly crystalline goethite had a strong effect on the mobility and attenuation of elements during the transformation.
Schwertmannite precipitation was the main cause for downstream attenuation of As and metal concentrations in the Chinkuashih AMD and creek waters. However, there were still about 3235 metric tons per year (t yr-1) of Fe, 737 t yr-1 Al, 191 t yr-1 Cu, and 2.4 t yr-1 As discharged into Lian-Dong Bay, which produced abundant suspended particulates in the surface seawater near the estuary. The estuarine suspended particulates formed at pH < 4 were short nanorods consisting of schwertmannite and subordinate goethite, and the inshore suspended particulates formed at pH > 5.5 were composed of non-crystalline hydrous iron and aluminum oxides (HFO and HAO) with a trace of schwertmannite, in a form of nanoballs. As the pH increased in the water, the suspended particulates were enriched in Al, Si, Cu, Zn, Mn, Ni, Co, and Cd relative to As, Cr, Pb, Fe, and S.
The water chemistry and precipitate constituents in areas affected by AMDs at Chinkuashih were mainly influenced by the formation of iron oxyhydroxysulfate minerals and HFO/HAO and sequential co-precipitation or adsorption of trace elements interrelated to changes in solution pH at various stages of water mixing and neutralization. These processes may have reduced and/or deferred environmental impacts made by the Chinkuashih AMDs. However, further investigations and continuous monitoring of the potential influences of desorption, transformation, and/or dissolution of the suspended particulates in Lian-Dong Bay are apparently important.

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