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

研究了碳源如纤维素的热化学转化过程中的反应化学。采用两级管式反应器对新生热解产物的二次气相反应动力学进行了研究。实验还进行了数值验证，由一个详细的化学动力学模型组成的8000多个基本步骤，如反应与500多个化学物种。可接受的能力的动力学模型在预测产品的浓度分布，使我们能够评估反应途径，导致苯和萘通过从纤维素的初级热解物的炔烃和二烯。在低温下，C3炔和二烯是苯的主要前体，而在高温下，乙烯和乙烯基乙炔的结合主要产生苯。环戊二烯是萘的主要前体。乙炔与丙炔或烯丙基自由基结合形成环戊二烯。

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.