航空生物燃料高效制备实验研究与机理分析
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摘要
目前，包括中国在内的世界各国航空公司都在积极寻求解决方案来应对航空燃料价格急剧波动和航空碳减排的双重压力。开发第二代可再生航空生物替代燃料是航空业减排和降低燃油成本的重要出路。
本文简要分析了航空燃料制备的典型技术（主要包括常规炼制工艺、非传统原料炼制工艺、费托合成技术、氢化处理技术、生物合成烃技术、裂解工艺、转酯化技术以及其它发酵工艺），并对各种工艺进行了对比。同时，本文以生物柴油和脂肪酸为原料，采用柯尔贝电解联合催化裂化工艺制得可再生航空生物燃料，该产品具有优良的稳定性、低温流动性以及安全性能，完全可以作为现有航空燃料的替代产品或调合组分，而且不需要对现有的燃料设施进行改造。
柯尔贝电解工艺主要是去除原料中的氧。研究结果表明：铂电极具有较好的稳定性能，较高的电解温度和电压有利于该反应的进行，优化的电解温度为45±5°C；乙醇溶剂适用于酸性电解体系，而甲醇更适于弱酸性或者中性电解体系；当采用甲醇作溶剂时，电解电压不能低于7.5V。标准三电极体系电化学测试（循环伏安测试、线性伏安扫描、塔菲尔曲线测试）结果表明：柯尔贝电解是完全不可逆的合成过程，且电解过程中的电子转移数是1。
NKC-7、NKC-11、HY、NKC-12催化剂用于催化裂化/异构化实验来制备碳链个数在5~15的宽切割组分航空燃料。通过催化剂的表征及失活特性分析表明NKC-7具有较好的催化裂化稳定性。优化的催化裂化反应条件为：反应温度485°C，物料流量0.600mL/min，催化剂用量15g （质量空速为2.2h-1）。该反应条件下航空燃料组分的产率在90%以上。本文还建立了集总反应动力学模型并利用龙格库塔方程和非线性最小二乘法对催化裂化工艺进行了动力学参数的估算。
本文建立了成本分析模型对航空生物燃料的生产进行技术经济性评估，该模型以废弃油脂为原料，生产规模为年产1万吨航空燃料。分析结果表明：采用该工艺技术生产航空燃料的总投资额为2410万元，生产成本为7780万元每年，其中原料价格所占比重接近88%。
本文以能源微藻等能源作物为原料，对可再生航空生物燃料进行全生命周期评价。结果表明：虽然以微藻为原料生产并使用1MJ的生物燃料所产生的二氧化碳当量值最低，但是仍达到0.285kg eq-CO_2/MJ生物燃料。开发废弃油脂资源作为我国发展可再生生物燃料的主要原料将会带来极大的环保效益和社会效益。
The world is changing and so is the aviation industry. Now with decliningpetroleum resources, shocking surge in the price of fuel, combined with the increasein political and environmental concerns, it is imperative for aviation industries todevelop clean and energy-efficient technologies of producing sustainable alternativebiofuels. In present study, an innovative but simple and effective method wasdeveloped for the production of aviation biofuels by Kolbe electrosynthesis coupledwith catalytic cracking reaction from fatty acid methyl esters (biodiesel) or saturatedfatty acids. The aviation biofuels produced showed good properties even at extremelycritical conditions.
For the preparation of long carbon chain hydrocarbons by Kolbe reactions fromsaturated fatty acids. Several reaction conditions (such as potential, solvent, supportelectrolyte, reaction time, and electrode materials) were evaluated to optimize theKolbe electrosynthesis. The optimum conditions for Kolbe reaction were: thepotential higher than7.5V and20wt.%of KOH used as the support electrolyte withtemperature of45±5oC, while the methanol as solvent. Besides, the mechanism wasalso proposed according to the electrochemical tests (cyc1ic voltammetry tests, linearsweep voltammetry tests, and tafel tests). The results show that it is a very promisingchoice for the preparation of aviation jet fuel by Kolbe processes, which are energyefficient as the reactions are conducted mostly at ambient pressure and temperature.
In order to get higher conversion ratio and higher jet fuel yield in the catalyticcracking reaction,15g NKC-7catalyst was used while the feedstock flow rate was0.600mL/min under485oC after1h when the catalyst has stable react activation. Also,a detailed lumping procedure for obtaining a kinetic model of catalytic crackingreaction is developed. The kinetic constants were estimated by nonlinear least squaresfitting method.
In order to estimate the cost of producing aviation biofuel, technical andeconomic analysis on a conceptual design of an aviation biofuel production plant(with a capacity of10,000tonnes per year) was made. The estimated total capital costand annual operating cost were approximately RMB24.10million and RMB77.8million, respectively. The present results demonstrated that the industrial scale plant would be promisingly competitive in the market using waste cooking oils and animalfats as raw material.
A life cycle assessment was carried out to quantify and compare theenvironmental impacts by producing and utilizing of biofuels derived from the bestfeedstock options available in the short and medium term (palm oil, jatropha oil, andmicroalgae oil) referring to China conditions. According to the well-to-pump (WTP)and pump-to-wheels (PTW) results, the total amount of CO_2emitted for both casescenarios is different, arranging from0.285kg eq-CO_2/MJ biofuel to0.730kgeq-CO_2/MJ biofuel based on the production of1MJ biofuel. The new generationrenewable materials (especially microalgae) and waste cooking oil appear to be themost likely feedstock for aviation biofuels in medium and long term of China.Considering the extensive application of microalgae and waste cooking oil forbiofuels production, new market will be opened up and there will be real andpotentially very promising impacts on ecosystems and on society.
本文简要分析了航空燃料制备的典型技术（主要包括常规炼制工艺、非传统原料炼制工艺、费托合成技术、氢化处理技术、生物合成烃技术、裂解工艺、转酯化技术以及其它发酵工艺），并对各种工艺进行了对比。同时，本文以生物柴油和脂肪酸为原料，采用柯尔贝电解联合催化裂化工艺制得可再生航空生物燃料，该产品具有优良的稳定性、低温流动性以及安全性能，完全可以作为现有航空燃料的替代产品或调合组分，而且不需要对现有的燃料设施进行改造。
柯尔贝电解工艺主要是去除原料中的氧。研究结果表明：铂电极具有较好的稳定性能，较高的电解温度和电压有利于该反应的进行，优化的电解温度为45±5°C；乙醇溶剂适用于酸性电解体系，而甲醇更适于弱酸性或者中性电解体系；当采用甲醇作溶剂时，电解电压不能低于7.5V。标准三电极体系电化学测试（循环伏安测试、线性伏安扫描、塔菲尔曲线测试）结果表明：柯尔贝电解是完全不可逆的合成过程，且电解过程中的电子转移数是1。
NKC-7、NKC-11、HY、NKC-12催化剂用于催化裂化/异构化实验来制备碳链个数在5~15的宽切割组分航空燃料。通过催化剂的表征及失活特性分析表明NKC-7具有较好的催化裂化稳定性。优化的催化裂化反应条件为：反应温度485°C，物料流量0.600mL/min，催化剂用量15g （质量空速为2.2h-1）。该反应条件下航空燃料组分的产率在90%以上。本文还建立了集总反应动力学模型并利用龙格库塔方程和非线性最小二乘法对催化裂化工艺进行了动力学参数的估算。
本文建立了成本分析模型对航空生物燃料的生产进行技术经济性评估，该模型以废弃油脂为原料，生产规模为年产1万吨航空燃料。分析结果表明：采用该工艺技术生产航空燃料的总投资额为2410万元，生产成本为7780万元每年，其中原料价格所占比重接近88%。
本文以能源微藻等能源作物为原料，对可再生航空生物燃料进行全生命周期评价。结果表明：虽然以微藻为原料生产并使用1MJ的生物燃料所产生的二氧化碳当量值最低，但是仍达到0.285kg eq-CO_2/MJ生物燃料。开发废弃油脂资源作为我国发展可再生生物燃料的主要原料将会带来极大的环保效益和社会效益。
The world is changing and so is the aviation industry. Now with decliningpetroleum resources, shocking surge in the price of fuel, combined with the increasein political and environmental concerns, it is imperative for aviation industries todevelop clean and energy-efficient technologies of producing sustainable alternativebiofuels. In present study, an innovative but simple and effective method wasdeveloped for the production of aviation biofuels by Kolbe electrosynthesis coupledwith catalytic cracking reaction from fatty acid methyl esters (biodiesel) or saturatedfatty acids. The aviation biofuels produced showed good properties even at extremelycritical conditions.
For the preparation of long carbon chain hydrocarbons by Kolbe reactions fromsaturated fatty acids. Several reaction conditions (such as potential, solvent, supportelectrolyte, reaction time, and electrode materials) were evaluated to optimize theKolbe electrosynthesis. The optimum conditions for Kolbe reaction were: thepotential higher than7.5V and20wt.%of KOH used as the support electrolyte withtemperature of45±5oC, while the methanol as solvent. Besides, the mechanism wasalso proposed according to the electrochemical tests (cyc1ic voltammetry tests, linearsweep voltammetry tests, and tafel tests). The results show that it is a very promisingchoice for the preparation of aviation jet fuel by Kolbe processes, which are energyefficient as the reactions are conducted mostly at ambient pressure and temperature.
In order to get higher conversion ratio and higher jet fuel yield in the catalyticcracking reaction,15g NKC-7catalyst was used while the feedstock flow rate was0.600mL/min under485oC after1h when the catalyst has stable react activation. Also,a detailed lumping procedure for obtaining a kinetic model of catalytic crackingreaction is developed. The kinetic constants were estimated by nonlinear least squaresfitting method.
In order to estimate the cost of producing aviation biofuel, technical andeconomic analysis on a conceptual design of an aviation biofuel production plant(with a capacity of10,000tonnes per year) was made. The estimated total capital costand annual operating cost were approximately RMB24.10million and RMB77.8million, respectively. The present results demonstrated that the industrial scale plant would be promisingly competitive in the market using waste cooking oils and animalfats as raw material.
A life cycle assessment was carried out to quantify and compare theenvironmental impacts by producing and utilizing of biofuels derived from the bestfeedstock options available in the short and medium term (palm oil, jatropha oil, andmicroalgae oil) referring to China conditions. According to the well-to-pump (WTP)and pump-to-wheels (PTW) results, the total amount of CO_2emitted for both casescenarios is different, arranging from0.285kg eq-CO_2/MJ biofuel to0.730kgeq-CO_2/MJ biofuel based on the production of1MJ biofuel. The new generationrenewable materials (especially microalgae) and waste cooking oil appear to be themost likely feedstock for aviation biofuels in medium and long term of China.Considering the extensive application of microalgae and waste cooking oil forbiofuels production, new market will be opened up and there will be real andpotentially very promising impacts on ecosystems and on society.
引文
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