現代水泥工業面臨的挑戰主要在於「開發替代原料來源」與「降低製程CO2排放」兩大方面。許多產業廢棄物皆具有作為水泥替代原料之潛力，且積極的廢棄物管理策略應以再利用途徑優先於傳統處理與處置，藉以促進資源循環並降低環境負荷。另一方面，為了減少水泥製造之CO2排放，節能型水泥（low-energy cements）成為近年的研究重點課題，其中富貝萊土水泥（belite-rich cement，BRC）除可大量降低製程CO2排放之外，更具有優越的機械與化學特性，因此在各類節能型水泥中受到矚目。然而，燒製富貝萊土水泥熟料的難題在於必須避免貝萊土（belite，Ca2SiO4，C2S）於降溫過程由β相轉變為無水化活性的γ相結構，故需進一步探究相關燒製條件與晶相轉變之控制方法。有鑑於此，本研究嘗試以無機產業廢棄物（包含牡蠣殼灰、稻殼灰、淨水污泥、轉爐石與電鍍污泥）作為替代原料燒製富貝萊土水泥熟料，並探討重金屬對C2S相轉變之影響及富貝萊土水泥之水化特性。此外，本研究亦嘗試建立晶相定量分析方法，用於測定水泥熟料中矽酸鹽類之含量，以作為檢討生料最適組成及探討重金屬影響之基礎指標。
在晶相定量分析方法建立方面，研究結果發現噴霧乾燥（spray drying）技術可有效提升晶相定量結果之精確度（precision）與再現性（reproductivity），另比對定量結果與標準水泥熟料之矽酸鈣晶相含量，亦顯示此晶相定量方法具有良好的準確性（accuracy）。而上述無機廢棄物可全取代水泥生料用於熟料燒製，藉由熟料游離石灰含量可知，艾萊土（alite，Ca3SiO5，C3S）與貝萊土之最適燒結溫度分別為1400 °C與1250 °C。當生料之石灰飽和度（lime saturation factor，LSF）為1.00～1.05且矽氧係數（silica ratio，SR）為3.0～4.0時，燒成熟料含有最高量的C3S晶相；而當生料LSF為0.74、SR為4.0時，燒成熟料中C2S晶相含量則可達到最大值，故將其擇定為富貝萊土水泥之最適生料組成參數。
在重金屬對於C2S相轉變之影響方面，鎳、鋅、鉻對β-C2S之穩定具有正面的效果（Cr3+ > Ni2+ > Zn2+），然而銅則具有負面的影響。以電鍍污泥燒製富貝萊土水泥時，其含有的重金屬亦可將熟料中C2S穩定於β相；當5.0 wt.%以上電鍍污泥取代水泥生料時，可發現燒成熟料中無水化活性的γ-C2S幾乎消失。另由熟料之重金屬殘留量及穿透式電子顯微鏡（transmission electron microscope，TEM）之微結構觀察可知，以電鍍污泥燒製之熟料中β-C2S之穩定應可歸因於鎳與鉻之作用。
對於富貝萊土水泥水化特性而言，雖然水泥漿體之早期強度（28天內）隨富貝萊土水泥比例提高而降低，但其晚期強度皆可比擬普通卜特蘭水泥。當富貝萊土水泥含量達40 wt.%時，漿體之抗壓強度仍可符合台灣與美國對於第I型水泥之標準規範。此外，含80 wt.%富貝萊土水泥之漿體於養護晚期有較高的水化活性，此階段應導因於β-C2S的水化反應，而於90天與180天水化後可觀察到結構交錯且緻密的水化產物。經由核磁共振（magic angle spinning/nuclear magnetic resonance，MAS/NMR）分析29Si光譜可得知，在高含量的富貝萊土水泥（40 wt.%與80 wt.%）漿體中，晚期矽酸鈣水化物具有較長的鍵結長度，此應為其晚期抗壓強度提升之主要原因。上述富貝萊土水泥之水化特性應可提供相關工程應用設計之參考。
關於富貝萊土水泥漿體之溶出特性，鈣離子為溶出液中主要可溶出金屬，其濃度變化趨勢則與漿體水化反應進展相符。此外，鎳、鋅、銅、鉛等重金屬皆未溶出，而僅於試驗初期有微量的鉻離子存在於溶出液中，故由此可知富貝萊土水泥漿體中重金屬具有良好的穩定性，應可大部分釋除其環境影響之疑慮。

The exploration of alternative materials and the reduction of CO2 emissions are currently the main challenges of the modern cement industry. Many industrial wastes have potential to be cement raw materials, and this recycling method deserves priority attention in waste management, rather than the traditional treatment and disposal methods. In recent years, low-energy cements, such as the alinite cement, the sulfoaluminate cement, and the belite-rich cement (BRC), have been developed to reduce the CO2 emissions in cement manufacturing. Of these, BRC is more attractive because it not only leads to a considerable reduction in CO2 emissions, but also has superior mechanical and chemical properties. However, the major difficulty in producing BRC is preventing belite (Ca2SiO4, C2S) from transforming to the non-hydraulic γ phase during clinker cooling.

Accordingly, the purpose of this study was to use inorganic wastes, including oyster shell ash, rice husk ash, water-treatment-plant sludge, basic-oxygen-furnace slag, and electroplating sludge, as cement raw materials for the production of BRC, and to investigate the effects of heavy metals on the phase transformations of belite and the hydration characteristics of the resulting BRC pastes. In addition, the quantitative phase analysis method was established to determine the calcium silicates in the cement clinkers in order to study the appropriate compositions of raw mixes for the production of BRC and reveal the effects of heavy metals on the C2S phase transformations.

In the establishment of quantitative phase analysis for calcium silicates, it was found that the spray drying technique was useful to increase the precision and reproductivity of the quantitative results of alite and belite, and the quantitative phase analysis also had good performance with regard to accuracy. The inorganic wastes can entirely replace the cement raw materials for the clinker production. Based on the free calcium oxide content in clinkers, it was discovered that the suitable sintering temperature for the alite formation was 1400 °C, whereas that for the belite formation was 1250 °C. The clinkers containing the maximum amount of alite can be obtained from the raw mixes with lime saturation factor (LSF) at 1.00–1.05 and silica ratio (SR) at 3.0–4.0. On the other hand, the LSF value equal to 0.75 and the SR value equal to 4.0 were selected for the preparation of the BRC clinkers.

In terms of the stabilization of β-C2S by heavy metals, it was noticed that nickel, zinc, and chromium had positive effects (Cr3+ > Ni2+ > Zn2+), while copper had a negative effect. In the clinkers produced with the electroplating sludge, the C2S can also be stabilized in the β phase by the heavy metals, and the non-hydraulic γ-C2S almost disappeared when 5.0 wt.% or more electroplating sludge was used to replace the raw mixes. From the results of residual heavy metals and the microstructural examination with a transmission electron microscope (TEM), it was concluded that the stabilization of β-C2S in the clinkers made from the electroplating sludge was mainly attributed to nickel and chromium.

In the hydration characteristics of the BRC pastes, the cements pastes blended with BRC had comparable later strength to the commercial OPC pastes, although their early strength (within 28 days) decreased with increasing the BRC fraction. When the BRC fraction was up to 40 wt.%, the blended cement pastes could still satisfy the compressive-strength requirements of the CNS and ASTM standards for Type I cements. The hydration reaction of the blended cement containing 80 wt.% BRC was more active in the later period than the early period, a result which is related to the hydration of β-C2S. The interlaced and dense hydration products were present in the blended cement pastes at 90 and 180 days of curing time. By using the 29Si magic angle spinning/nuclear magnetic resonance (MAS/NMR) analysis, it was noticed that higher BRC fractions (40 wt.% and 80 wt.%) in the blended cements can increase the length of linear polysilicate anions in calcium silicate hydrates at the later curing ages. This can explain the growth in later compressive strength of the blended cement pastes, and these hydration characteristics of the BRC pastes will provide useful information for engineering design.

In terms of the leaching characteristics of the hardened BRC pastes, the variation in concentration of calcium ions was in line with the progress of the hydration reactions. Nickel, zinc, copper, and lead were not detected in any of the leachates, and only small amounts of chromium were present in the initial periods of the leaching test. Therefore, it is suggested that the heavy metals have good stability in the hardened cement pastes, and that concerns about the leaching of heavy metals from the products can be mostly alleviated.

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