本研究探討以廢棄油脂（FOG, Fats, Oils, and Grease）為原料生產生質柴油及高附加價值化學品之製程設計、最佳化與永續性分析。研究建立五種替代製程方案，並利用 Aspen Plus 模擬與經驗證的動力學模型，評估以均相與非均相觸媒進行的兩步酯化與酯交換反應。結果顯示，方案三雖需較高的再沸器與冷凝器熱負荷，但可簡化生質柴油與觸媒的分離程序；而方案五則能降低再沸器熱負荷達 22.3%，同時回收甘油與 K₂HPO₄作為副產品，並生成 205 kmol/h 的再利用水，達到無廢水排放的目標。透過反應曲面法（RSM）求得最佳操作條件，在 CSTR-1 與 CSTR-2 中分別達到 94% 的 OLAC 轉化率與 99.8% 的 TRIOL 轉化率。結合甘油蒸氣重組（GSR）與尿素合成後，建立了多聯產途徑，顯著提升了能源與碳效益。在最佳 GSR 操作條件下（H₂O/GLY = 6.01、775 °C、1.64 atm），可達到 99.95% 的甘油轉化率與 70.4% 的冷氣體效率。在能量整合部分，方案二利用夾點法（pinch analysis）進行熱整合，減少熱、冷公用能需求 45.7–71.8%；而方案三結合聯合循環發電系統後，可實現 89–93% 的二氧化碳減量。3E（能源、火用、經濟）分析結果證實，大型且經熱整合的製程最具競爭力。熱整合使公用能效率提升 40–65%，整體火用效率達 86.4%，其中 GSR 單元的火用破壞最大（約佔 30%）。在經濟分析方面，原料成本為主要營運支出來源（約 4.15–4.23 億美元/噸）。小型廠（≤100 kton/y）因具高單位生產成本（BBP = 1306–2004 USD/ton）、低投資報酬率（ARR ≤ 96%）、長回收期（PBP = 17–34 年）而缺乏競爭力；相對地，大型廠（≥500 kton/y）可達高投資報酬率（ARR = 186–320%）、低生產成本（BBP = 638–749 USD/ton），且回收期僅 3–5 年，顯示其在經濟與永續性上的顯著優勢。

This study investigates the process design, optimization, and sustainability of biodiesel and value-added chemical production from waste fats, oils, and grease (FOG) through five alternative process schemes. Aspen Plus simulations with validated kinetic models were employed to evaluate two-step esterification and transesterification using homogeneous and heterogeneous catalysts. Among the designs, Scheme-3 required higher reboiler and condenser duties but enabled simpler biodiesel–catalyst separation, while Scheme-5 reduced reboiler duty by 22.3%, recovered glycerol and K₂HPO₄ as byproducts, and generated 205 kmol/h of recycled water without wastewater discharge. Optimal operating conditions determined by response surface methodology achieved 94% conversion of OLAC and 99.8% conversion of TRIOL in CSTR-1 and CSTR-2, respectively. Integration with glycerol steam reforming (GSR) and urea synthesis established polygeneration pathways with enhanced energy and carbon performance. At optimized GSR conditions (H₂O/GLY = 6.01, 775 °C, 1.64 atm), 99.95% glycerol conversion and 70.4% cold gas efficiency were achieved. Scheme-2, incorporating pinch-based heat integration, reduced hot and cold utility requirements by 45.7–71.8%, while Scheme-3, coupled with combined cycle power generation, achieved the highest CO₂ reduction (89–93%). The 3E (Energy, Exergy, and Economic) analysis confirmed that large-scale, heat-integrated processes are the most competitive. Heat integration improved utility efficiency by 40–65%, overall exergy efficiency reached 86.4%, and the GSR unit contributed the largest exergy destruction (~30%). Economically, feedstock dominated total operating cost (~415–423 million USD/ton). Small plants (≤100 kton/y) were uncompetitive, with high BBPs (1306–2004 USD/ton), low ARR (≤96%), and long PBPs (17–34 years). In contrast, large-scale facilities (≥500 kton/y) achieved high ARR (186–320%), low BBPs (638–749 USD/ton) compared to conventional diesel price with short PBPs of 3–5 years.

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