摘要
生物质能是一种可以收集、储存、运输和最接近常规化石燃料的可再生能源，从原料构成到理化特性均与煤炭等化石能源相似，其不仅是绿色的洁净能源，而且是可再生能源中唯一可以培育和转化为液体燃料的碳资源，在6种可再生能源中占有重要的地位。木质纤维素生物质是目前地球上最丰富、最廉价的生物质资源，我国每年可作能源利用的农林剩余物等木质纤维素生物质达7亿吨以上，折合标煤3.5亿吨左右。木质纤维素生物质转化为液体燃料，进而可作为柴油机替代燃料，其对于增强我国石油安全、缓解能源和资源压力、减轻生态环境污染、发展社会经济等具有现实意义。乙酰丙酸乙酯可由木质纤维素转化获得，在国外已有作为车用燃料的研究，但国内对其在柴油机上燃烧动力及排放性能的研究几乎为空白。因此，结合我国生物质资源状况，以玉米秸秆基乙酰丙酸乙酯为对象，分析其与柴油的混合燃料柴油机特性，找出适合我国柴油机使用的合理配比混合燃料，有利于生物质基乙酰丙酸乙酯的推广利用和我国生物质资源的合理化、规模化利用。
本文研究了生物质中典型的玉米秸秆制取乙酰丙酸并进行酯化工艺方法和反应条件。分析了乙酰丙酸乙酯-柴油混合燃料的动力性性能，借助内燃机试验台架，进行了混合燃料的动力性、经济性及排放性试验，找到了适合我国柴油体系和柴油机系统的燃料混合范围。以乙酰丙酸乙酯为中心，结合乙酰丙酸乙酯和生物柴油的各自理化特性特点，开展了乙酰丙酸乙酯、生物柴油与柴油的多种燃料配方的理化特性研究，优选了满足国家标准的燃料配方，并对配方进行了柴油机动力性能验证。对玉米秸秆为原料的生物质基乙酰丙酸乙酯进行了生命周期能耗、环境排放和经济性分析，针对相关环节提出了一定的建议。结果表明：
(1)玉米秸秆纤维素和半纤维含量都较高，灰分含量较小，在水解制取乙酰丙酸平台化合物方面具有较大的优势。玉米秸秆制取糠醛后的残渣可用于制取乙酰丙酸，其较好的反应温度、硫酸浓度、固液质量比、反应时间等条件下，乙酰丙酸产率的可达70%。极性较强的吸附剂对乙酰丙酸水解液的分离效果较好，在合适的乙酰丙酸浓度、流量、填充柱的高径比、洗脱盐酸浓度情况下，乙酰丙酸收率为82.2%。酯化反应时，选用固体酸催化剂，找到了乙酰丙酸与乙醇酯化反应V酸:V醇、反应时间、反应温度、M催化剂:M酸等优化条件。
(2)合适比例的乙酰丙酸乙酯-柴油混合燃料可在水平单缸四冲程压燃式柴油发动机中正常工作；燃用这混合燃料与柴油的外特性的动力性变化趋势相同，转矩和功率较燃用纯柴油略小；混合燃料的燃油消耗率较柴油略大，能量消耗率却低于纯柴油；混燃燃料的NO_x、CO_2等排放在柴油机输出功率较大时较柴油排放浓度要高；CO和烟度排放在输出功率较大时，随乙酰丙酸乙酯含量的增加较为明显地降低。混合燃料柴油机利用过程中的油耗率受混合燃料的密度影响较大；NO_x、CO和CO_2等排放受混合燃料含氧量影响较大；HC排放和尾气烟度受混合燃料的运动粘度影响较大；混合燃料的含氧量是影响燃烧排放主要参数；尾气烟度受燃料特性变化影响最为明显。
(3)以乙酰丙酸乙酯为中心，开展乙酰丙酸乙酯、生物柴油和柴油不同配比混合燃料的理化特性研究，具体包括互溶性、低温流动性、雾化及蒸发性、氧化安定性、防腐性、洁净性、发火性、热值等方面，研究配制了13种B5系列混合燃料配方，经试验分析，有10种配方的满足GB/T25199-2010生物柴油调合燃料(B5)的指标要求。理化特性试验表明，乙酰丙酸乙酯和生物柴油的配合有一定的协同、相互促进作用，以柴油为主体，同时合理比例添加乙酰丙酸乙酯和生物柴油能够使燃料配方具有与柴油十分接近的理化特性等，较好地满足替代柴油的理化特性。对筛选的4种混燃燃料进行了柴油机试验验证，结果表明，燃料配方在柴油机中燃烧的动力性基本不变，经济性略有提高，HC、CO、烟度等污染物排放比燃烧柴油有明显降低，实现了节能减排。
(4)建立了玉米秸秆为原料制乙酰丙酸乙酯的生命周期能源消耗、排放和经济评价模型，考察了生物质的生长、收集、预处理、水解酯化、燃料运输分配及柴油机利用，详细讨论各个单元过程，定义了车用燃料生物质基乙酰丙酸乙酯生命周期的系统边界，进行了生物质转化乙酰丙酸乙酯的相关数据收集，整理和评价。生物质基乙酰丙酸乙酯生命周期中，乙酰丙酸乙酯的生产过程中水解和酯化过程的能耗最多，占到了总能耗的66%以上；玉米秸秆收集和预处理过程的能耗相当，分别占总能耗的16.0%和15.5%，提高水解和酯化效率是生物质转换为乙酰丙酸乙酯的主要节能途径和发展方向，减少玉米秸秆预处理和收集的能耗也是较为重要的节能途径。相比传统柴油，生物质基乙酰丙酸乙酯的环境污染物排放中NOx、PM10、SO2和温室气体均远低于传统柴油。随着乙酰丙酸乙酯价格和糠醛价格的升高，项目净现值增加；随着玉米秸秆价格、初投资费、乙醇费用、劳动力成本的增加，项目净现值减少。其中，对净现值影响最大的是乙酰丙酸乙酯价格。
Bioenergy is a kind of renewable energy which can be collected, stored, transported and isthe most similar to conventional fossil fuel. It is not only green clean energy, but also the onlykind of carbon resources of renewable energy that can be cultivated and converted into liquidfuels, and it thus plays an important role in the six kinds of renewable energy sources.Lignocellulosic biomass is the most abundant and cheapest biomass resources on the earth. Inchina, there is more than700million tons lignocellulosic biomass can be used as energy, suchas agricultural and forestry residues. Lignocellulosic biomass can be converted into liquid fuelsand then used as internal combustion engine alternative fuels, which is an importantdevelopment direction and has a practical significance for enhancing the oil security, alleviatingthe pressure of energy and resources, reducing environmental pollution, and developing thesocial economy. Ethyl leculinate (EL) can be gotten from lignocellulosic biomass, and EL hasbeen studied as a vehicle fuel abroad. But its power and emissions performance of diesel engineresearch has not been done domestic. Therefore, on the base of biomass resources in China, it isvery important to take corn stalk based EL as study object by analyzing performance of dieselengine with blended fuels of EL and diesel, so as to find the appropriate proportion of EL-dieselblended fuels. All of that is conducive to the promotion of biomass based EL, along withrational and large-scale utilization of biomass resource in China.
In the paper, process and reaction conditions of transforming biomass such as corn stalk tolevulinic acid and EL were study. Dynamic performance of EL-diesel blended fuels wasanalyzed. The combustion, economy and emission characteristics of EL-diesel blended fuelswere investigated using engine bench tests. The range of EL-diesel blended fuels to suit fordiesel and diesel engine system of China was found. For taking EL as the key fuel, physical andchemical properties of different fuel formulas were studied according to EL, biodiesel and dieselproperties. The fuel formulas were optimized and selected in line with China National Standardsand Codes, and dynamic performance of the fuel formulas were verified on a diesel engine. Lifecycle energy consumption, environmental emission and economy of corn stalk based EL were analyzed, and several improvement to related units were given. The results shown that:
(1)Corn stalk has a large advantage in producing potentially interesting derivatives oflevulinic acid by hydrolysis according to high content of cellulose and hemicellulose, lowcontent ash. Residue of corn stalk after producing furfural can be used to make levulinic acid,levulinic acid yield can be reached70%at the optimum condition of reaction temperature,concentration of sulfuric acid, ratio of liquid to solid, reaction time. Resin of polarizedadsorption has the better separation effect on levulinic acid, the levulinic acid yield was82.2%at the suitable condition of levulinic acid concentration, flow rate, ratio of height to diameter ofpacked column, concentration of hydrochloric acid. Solid acid catalyst was selected inesterification, the better condition of Vlevulinic acid:Vethanol, reaction time, reaction temperature, andMcatalyst:Msulfuric acidwere found, respectively.
(2)An appropriate proportion of EL-diesel blended fuels can be normally used in ahorizontal single cylinder four stroke diesel engine, without any modification to the engine.EL-diesel blended fuels and diesel have the same trend in the dynamic changes of the externalcharacteristics. Torque and power of EL-diesel blended fuels were slightly lower than diesel.Brake specific fuel consumptions (BSFC) of EL-diesel blended fuels were slightly higher thandiesel, but energy consumptions were lower. Emissions of NOxand CO_2were higher than dieselwhen the output power became larger. Emissions of CO and smoke opacity were reduced withincreasing percentage of EL when the output power became larger. BSFC was influenced mostby the density of the blended fuels. NOx, CO, and CO_2emissions were influenced most by theoxygen content. The KV was the most influential parameter for HC emissions and the opacity ofthe blended fuels. The oxygen content was the foremost influential parameter. The influence ofthe blended fuels parameters on smoke opacity was the greatest.
(3)For taking EL as the key fuel, physical and chemical properties including solubility,cold flow properties, atomization and evaporation, oxidation stability, anti-corrosion properties,cleanness, ignition properties, heat value of different fuel formulas of EL-biodiesel-diesel werestudied.13kinds of fuel formulas were gotten and10of them were in line with China NationalStandards and Codes: GB/T25199-2010biodiesel fuel blend(B5).The test of physical andchemical properties shown that the fuel formulas with EL and biodiesel have collaboration,mutual promotion. Physical and chemical properties of diesel with an appropriate proportion ofEL and biodiesel were similar to pure diesel and can be suit for diesel engine. Experimentalverification was taken in diesel engine with4selected fuel formulas, the results shown thatdynamic performance of the fuel formulas was almost the same as diesel, fuel economy wasbetter than diesel, emission of HC, CO and smoke opacity was significantly lower than diesel.Energy saving and emission reduction were realized.
(4)The model of life cycle energy consumption, environmental emission and economy ofcorn stalk based ethyl leculinate was built. The unit processes of corn stalk growth, collection,transportation, pretreatment, hydrolysis and esterification, EL fuel transportation, andcombustion in engine were investigated. The system boundary of life cycle was defined. Theinterrelated data was collected, arranged and assessment. In the life cycle of biomass based EL,the most energy consumption was in process of corn stalk hydrolysis and esterification,accounting for more than66%of total consumption. The similar energy consumption was incorn stalk collection and pretreatment, accounting for16.0%and15.5%of the total,respectively. It is the major energy-saving way and development direction to improve efficiencyof corn stalk hydrolysis and esterification. It is also important to reducing energy consumptionin corn stalk collection and pretreatment. Compared to conventional diesel, NOx, PM10, SO2andgreenhouse gas of biomass based EL was much lower. NPV increased with an increase in ELand furfural price; NPV decreased with an increase in corn stalk price, capital cost, ethanol costand labour cost. The influence of the EL price on the change in NPV was the most significant.
引文
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