通过等离子体–冰相互作用优化及利用 N2 + CO2 与 NH3 + CO2 气体混合物的机制洞察实现尿素合成的绿色路径
Green pathway of Urea Synthesis through Plasma-Ice Interaction Optimization and Mechanistic Insights with N2 + CO2 and NH3 + CO2 Gas Mixtures
AI总结：
该研究优化等离子体–冰相互作用参数，比较 N2 + CO2 与 NH3 + CO2 体系，证实 NH3 + CO2 可显著提高尿素生成浓度，为绿色尿素合成提供新路径。
摘要：
本研究探索了一条利用等离子体–冰相互作用并采用 N2 + CO2 和 NH3 + CO2 气体混合物进行尿素合成的绿色路径。研究采用电学和光发射光谱对等离子体进行表征，结果表明尿素形成涉及由高能物种驱动的复杂反应，这些反应产生活性氮和碳中间体，后者进一步反应形成尿素。对经等离子体处理的冰进行的物理化学分析显示，其 pH 值和电导率（EC）升高，氧化还原电位（ORP）降低。为促进尿素形成，研究对等离子体工艺参数（气体压力、施加电压和处理时间）进行了优化。在这些参数中，等离子体处理时间的影响最为显著。将处理时间从 20 分钟增加到 60 分钟，对物理化学性质产生了显著影响：对于 N2 + CO2 等离子体，pH 值升高 21.05%，EC 升高 184.7%，ORP 降低 27.48%；对于 NH3 + CO2 等离子体，pH 值升高 27.37%，EC 升高 239.05%，ORP 降低 72.67%。研究表明，NH3 + CO2 等离子体产生的尿素浓度（7.7 mg L-1）显著高于 N2 + CO2 等离子体（0.55 mg L-1）。这归因于氨的直接可获得性和反应活性，其简化了反应路径并增强了中间体形成。这些发现凸显了等离子体–冰相互作用作为一种节能且环境友好的尿素合成方法的潜力，并为传统工艺提供了一种可持续替代方案。
英文摘要：
This study explores a green pathway for urea synthesis using plasma-ice interaction with gas mixtures of N2 + CO2 and NH3 + CO2. Electrical and optical emission spectroscopy were employed to characterize the plasmas, revealing that urea formation involves complex reactions driven by high-energy species, producing reactive nitrogen and carbon intermediates that further react to form urea. Physicochemical analyses of plasma-treated ice showed increased pH, electrical conductivity (EC), and reduced oxidation-reduction potential (ORP). Optimization of plasma process parameters (gas pressure, applied voltage, and treatment time) was performed to enhance urea formation. Among these parameters, plasma treatment time had the most substantial influence. Increasing treatment time from 20 to 60 minutes significantly impacted physicochemical properties: for N2 + CO2 plasma, pH increased by 21.05%, EC by 184.7%, and ORP decreased by 27.48%; for NH3 + CO2 plasma, pH increased by 27.37%, EC by 239.05%, and ORP decreased by 72.67%, respectively. The study shows that NH3 + CO2 plasma produces a significantly higher concentration of urea (7.7 mg L-1) compared to N2 + CO2 plasma (0.55 mg L-1). This is attributed to the direct availability and reactivity of ammonia, which simplifies reaction pathways and enhances intermediate formation. These findings highlight the potential of plasma-ice interaction as an energy-efficient and environmentally friendly method for urea synthesis, offering a sustainable alternative to conventional processes.
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