Detailed chemical kinetic modeling as an innovative approach for understanding complex reactions included in thermochemical conversions of carbon resources

研究了纤维素等碳源的热化学转化所包含的反应化学。用两段管式反应器评价了初生热裂解产物的二次气相反应动力学。实验还得到了一个详细的化学动力学模型的数值验证，该模型由500多个化学物种的8000多个基本阶跃反应组成。动力学模型在预测产品浓度分布方面的可接受能力使我们能够评估从纤维素的初级热解产物中通过炔烃和二烯生成苯和萘的反应路径。在低温下，C3炔和二烯是苯的主要前体，而在高温下，乙烯和乙烯乙炔的组合生成主要的苯。环戊二烯是一种重要的萘前驱体。乙炔与丙炔或烯丙基结合可生成环戊二烯。

The reaction chemistries included in the thermochemical conversion of carbon resources such as cellulose were studied. A two-stage tubular reactor was used for evaluating the reaction kinetics of secondary vapor phase reactions of the nascent pyrolysates. Experiments were also numerically validated by a detailed chemical kinetic model consisting of more than 8000 elementary step like reactions with over 500 chemical species. Acceptable capabilities of the kinetic model in predicting concentration profiles of the products enabled us to assess reaction pathways leading to benzene and naphthalene via the alkyne and diene from primary pyrolysates of cellulose. C3 alkyne and diene are primary precursors of benzene at low temperature, while combination of ethylene and vinylacetylene produces benzene dominantly at high temperature. Cyclopentadiene is a prominent precursor of naphthalene. Combination of acetylene with propyne or allyl radical leads to the formation of cyclopentadiene.