煤与城市污泥超临界水共气化的动力学研究

Kinetic Study on Supercritical Water Co-Gasification of Coal and Sewage Sludge

摘要

针对当前煤与城市污泥超临界水共气化过程中中间产物的转化关系和气态产物来源等反应机理解析不充分的问题，提出了一种双中间体集总反应动力学模型。基于液态中间产物中易分解（苯胺类等）与较稳定（多环芳烃类等）的两类主要有机成分，构建动力学模型，通过模型分析气化过程中中间产物随时间的转化关系，结合反应速率常数解析各种气态产物的来源和产量，进一步阐明煤与城市污泥超临界水共气化的转化机理。研究结果表明：模型预测结果与实验数据相对误差仅为7.13%，一致性较好；气态产物中，H₂、CO₂、CO主要通过中间产物的蒸汽重整反应生成，CH₄主要通过热解反应生成；共气化过程中，蒸汽重整反应和热解反应占据核心地位，当反应温度为620℃、煤与城市污泥混合物料质量分数为5%时，蒸汽重整反应的最大速率为0.15 mol/（L·min），最大热解反应速率为0.06 mol/（L·min）。该研究可为煤与城市污泥超临界水共气化技术的反应机理揭示与工艺优化提供理论参考。

Abstract

In view of the insufficient analysis of the reaction mechanism concerning the transformation relationships of intermediate products and the sources of gaseous products in the current supercritical water co-gasification process of coal and sewage sludge, a two-intermediate lumped kinetics model was proposed. This model was established based on two main organic components in the liquid intermediate products, namely the easily decomposable components (e.g., aniline) and the stable components (e.g., polycyclic aromatic hydrocarbons). Using the model, the transformation relationships of intermediate products over time during the gasification process were analyzed, and the sources and yields of various gaseous products were further examined in combination with the reaction rate constants. Consequently, the transformation mechanism of supercritical water co-gasification of coal and sewage sludge was further clarified. The research results show that the relative error between the model predictions and the experimental data is only 7.13%, indicating good consistency. Among the gaseous products, H₂, CO₂, and CO are mainly produced by steam reforming of intermediates, whereas CH₄ is dominantly formed through pyrolysis reactions. Steam reforming and pyrolysis dominate the entire co-gasification process. Under the conditions of 620℃ and a mixed solid mass fraction of 5%, the maximum reaction rate of steam reforming reaches 0.15 mol/(L·min), and the maximum pyrolysis reaction rate is 0.06 mol/(L·min). This study provides a theoretical basis for mechanism revelation and process parameter optimization of coal sewage sludge supercritical water co-gasification technology.

关键词

煤 / 城市污泥 / 超临界水 / 共气化 / 动力学模型

Key words

coal / sewage sludge / supercritical water / co-gasification / kinetic model

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基金资助

国家重点研发计划资助项目(2024YFF0505801)

陕西省自然科学基础研究计划资助项目(2024JC-YBMS-296)

咸阳市科技创新人才计划资助项目(L2024-CXNL-KJRCTD-KJRC-0017)