氧化锶催化酯交换生产生物柴油的分子动力学研究
1. 华中科技大学, 能源与动力工程学院, 湖北武汉 430074
2. 山东大学, 能源与动力工程学院, 山东济南 250061
| 摘 要： | 生物柴油是一种典型的可再生能源，其生产过程离不开酯交换反应催化剂。固体碱催化剂具有选择性高、不腐蚀设备、反应产物易分离回收等优点而得到广泛应用。深入研究固体碱催化剂的反应机理，理解催化反应的过程，对于指导生物柴油生产具有重要的意义。本研究基于密度泛函理论，采用分子动力学模拟的方法对甲醇、乙酸和甲酸乙酯等酯交换反应物在固体碱催化剂氧化锶表面上的吸附构型进行了研究，计算了不同端吸附体系的吸附能，确定了甲醇、乙酸和甲酸乙酯在氧化锶表面上的具有最低吸附能的位点；从扩散系数和径向分布函数等角度对酯交换反应的理想反应温度进行了探究。本研究在300-500 K的温度范围内确定了一个最优的反应温度可以获得甲醇与甲酸乙酯或乙酸与甲酸乙酯更高的反应速率，以及一个最优的温度可以让甲醇、乙酸和甲酸乙酯快速地吸附在氧化锶表面上，为后续甲醇、乙酸和甲酸乙酯在氧化锶上发生酯交换反应提供了理想的反应温度。 |
| 关 键 词： | 生物柴油; 酯交换; 催化剂; 分子模拟 |
| DOI： | 10.57237/j.jest.2023.04.003 |
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收稿日期: 2023-07-30
接受日期: 2023-09-05
在线出版日期: 2023-09-08
Molecular Dynamic Studies of the Transesterification Process Using Strontium Oxide as an Effective Catalyst for Biodiesel Production
1. School of Power and Energy Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
2. School of Power and Energy Engineering, Shandong University, Jinan 250061, China
| Abstract: | Biodiesel as a typical renewable energy relies on catalysts for transesterification reaction in the mass production process. Solid base catalysts are widely used for their advantages of high selectivity, no corrosion of equipment, and easy separation and recovery of reaction products. Studying the reaction scheme of solid base catalysts and understanding the reaction processes are fundamentally important for guiding the mass production of biodiesel. This work employed a molecular dynamic simulation method based on the density functional theory to systematically study the adsorption configurations of transesterification reactants including methanol, acetic acid, and ethyl formate on the surface of solid base catalyst strontium oxide. The adsorption energies of different end adsorption systems were calculated, and the sites with the lowest adsorption energies of methanol, acetic acid and ethyl formate on the surface of strontium oxide were determined. The ideal reaction temperature of transesterification reaction was investigated from the diffusion coefficient and radial distribution function. An optimized reaction temperature in the range of 300-500 K was determined that can yield the highest reaction rate between methanol and ethyl formate or acetic acid and ethyl formate. Meanwhile, an optimized reaction temperature was also determined for methanol, acetic acid and ethyl formate to adsorb on the surface of strontium oxide, which is favorable for the subsequent transesterification of methanol, acetic acid and ethyl formate on strontium oxide. |
| Keywords: | Biodiesel; Transesterification; Catalyst; Molecular Simulation |
参考文献
| [1] | 邹才能, 陈艳鹏, 熊波, et al. 碳中和目标下中国新能源使命 [J]. 中国科学院院刊, 2023, 38 (01): 48-58. |
| [2] | CHUAH L F, KLEMEŠ J J, YUSUP S, et al. A review of cleaner intensification technologies in biodiesel production [J]. Journal of Cleaner Production, 2017, 146: 181-93. |
| [3] | 韩宗江, 江国和, 吴刚. 生物柴油生产加工技术的研究进展 [J]. 应用化工: 1-8. |
| [4] | ABBASZAADEH A, GHOBADIAN B, OMIDKHAH M R, et al. Current biodiesel production technologies: A comparative review [J]. Energy Conversion and Management, 2012, 63: 138-48. |
| [5] | 陈晓淇, 朱晓, 齐建荟, et al. 焦炭-NO异相还原的密度泛函理论研究进展 [J]. 燃料化学学报, 2022, 50 (03): 257-67. |
| [6] | SONG J, NIU X, LING L, et al. A density functional theory study on the interaction mechanism between H2S and the α-Fe2O3(0001) surface [J]. Fuel Processing Technology, 2013, 115: 26-33. |
| [7] | 宁一麟. 固体催化剂的优化制备及催化餐饮废油合成生物柴油的性能研究 [D]; 山东大学, 2021. |
| [8] | 李颖. 钙钛矿型催化剂的调控制备及催化高酸值油合成生物柴油的性能研究 [D]; 山东大学, 2022. |
| [9] | DELLEY B. Hardness conserving semilocal pseudopotentials [J]. Physical Review B, 2002, 66 (15): 155125. |
| [10] | 刘思彤, 牛胜利, 韩奎华, et al. α-Fe2O3(001)及其掺杂表面吸附As2O3机制的密度泛函理论 [J]. 哈尔滨工业大学学报, 2022, 54 (07): 20-8. |
| [11] | LIU S, NIU S. An investigation on microscopic and mechanical properties of polyethylene/boron nitride graphene nanocomposites by DFT calculations [J]. Computational Materials Science, 2023, 228: 112324. |
| [12] | MAN I-C, SORIGA S G, PARVULESCU V. Effect of Ca and Sr in MgO(100) on the activation of methanol and methyl acetate [J]. Catalysis Today, 2018, 306: 207-14. |
| [13] | WANG L-Z, DUAN L-L. Isothermal crystallization of a single polyethylene chain induced by graphene: A molecular dynamics simulation [J]. Computational and Theoretical Chemistry, 2012, 1002: 59-63. |
| [14] | FEYZI M, NOROUZI L. Preparation and kinetic study of magnetic Ca/Fe3O4@SiO2 nanocatalysts for biodiesel production [J]. Renewable Energy, 2016, 94: 579-86. |
| [15] | 庞彪, 李家云. 分子动力学模拟研究Cu60Zr40非晶中的二十面体结构 [J]. 哈尔滨师范大学自然科学学报, 2012, 28 (05): 35-7. |
