With the increasingly prominent environmental problems and depletion of light petrochemical resources, the clean utilization of heavy oil has become the research focal area. The hydrodenitrogenation (HDN) experiments and kinetics of full‐range middle‐low temperature coal tar (MLCT) was studied on a fixed‐bed reactor with a Ni‐Mo/γ‐Al₂O₃ catalyst. Two kinds of three‐lumped kinetic models (K₁ and K_1.24) based on different reaction orders and high‐middle‐low reactivities were established and fitted by a simulated annealing algorithm for coal tar HDN reactions. The results presented good correspondence with experimental data following an average relative error of less than 0.3%. The effect of temperature, pressure, and liquid hourly space velocity (LHSV) on HDN of different reactivity nitrogen compounds (NCs) of MLCT was studied using the lumped kinetic models. Also, the difference between K₁ and K_1.24 models on the embodiment ability for HDN laws was also discussed from multiple perspectives. It has been observed that the HDN reactions of low and middle reactivity NCs are more influenced by LHSV; high temperature and pressure are more critical for the removal of low reactivity NCs, and low‐temperature or ‐pressure zone have larger effects on coal tar HDN reactions, especially at high LHSV; temperature has much more influence than pressure on the HDN effect, particularly towards the low reactivity NCs. The results of HDN laws for high reactivity NCs are concordant with K₁ and K_1.24 models. The K_1.24 model is a bit more reasonable to reveal the HDN law of middle to low reactivity NCs.

中文翻译：

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全范围中低温煤焦油加氢脱氮的集总动力学模拟

随着日益突出的环境问题和轻质石化资源的枯竭，重油的清洁利用已成为研究重点。加氢脱氮（HDN）实验和全范围中低温煤焦油（MLCT）的动力学研究在固定床反应器中与Ni-Mo系/γ-Al系₂ ö ₃催化剂。两种三集总动力学模型（K ₁和K _1.24）根据不同的反应顺序建立了高中低反应性，并通过模拟退火算法对煤焦油HDN反应进行了拟合。在平均相对误差小于0.3％的情况下，结果与实验数据具有良好的对应性。使用集总动力学模型研究了温度，压力和液时空速（LHSV）对MLCT不同反应性氮化合物（NCs）HDN的影响。另外，K ₁与K _1.24之差还从多个角度讨论了HDN法则的体现能力模型。已经观察到，低反应性和中反应性NCs的HDN反应受LHSV的影响更大。高温和高压对于去除低反应性NCs更为关键，而低温或高压区对煤焦油HDN反应的影响更大，尤其是在高LHSV的情况下；温度对压力的影响远大于压力对HDN的影响，特别是对低反应性NC的影响。高反应性NCs的HDN法则的结果与K ₁和K _1.24模型一致。K _1.24模型对于揭示中低反应性NC的HDN规律更为合理。