高级检索

    基于含钙矿石的CO2捕集与原位制备高品质合成气研究

    Research on CO2 capture and in-situ production of high-quality syngas with calcium-based ores

    • 摘要: 集成碳捕集与利用逆水煤气变换工艺(ICCU-RWGS)有效结合CO2捕集与加氢转化过程,是降低工业碳排放、推动碳中和目标实现的关键技术路径之一。该工艺以钙基CO2吸附材料为核心,可直接将捕集的CO2原位加氢转化为合成气,其品质通常以H2与COx(CO、CO2)的物质的量比(M值)衡量。研究旨在通过该工艺高效制备M值为2.00 ~ 2.05的合成气,从而为下游费托合成、甲醇合成等工段提供高适配性的原料气。对温度、压力及钙氢物质的量比(n(CaCO3):n(H2))等关键操作参数进行热力学平衡分析与计算。结果表明,最佳操作条件为700 ℃、0.1 MPa及钙氢物质的量比为1∶2,此外,H2O的存在会对加氢转化性能产生不利影响。在此基础上,通过固定床小试实验研究进行含钙天然矿石的筛选,结果表明,在反应温度为700 ℃、压力为0.1 MPa以及钙氢物质的量比为1∶2的条件下,白云石表现出更优的ICCU-RWGS反应性能,且该操作条件与热力学预测结果一致。在最优条件下,进一步探究其循环性能,结果表明,20个循环内的M值未发生显著衰减,且循环后的白云石未出现明显的烧结现象,展现出良好的循环稳定性和结构稳定性。总体而言,研究在ICCU-RWGS工艺的基础上,通过系统调控操作参数提高产物中COx的物质的量比例,制备高品质合成气以满足下游化学品与燃料合成原料需求。

       

      Abstract: The Integrated Carbon Capture and Utilization-Reverse Water Gas Shift (ICCU-RWGS) process effectively integrates CO2 capture with hydrogenation conversion, making it one of the key technological pathways for reducing industrial carbon emissions and advancing the goal of carbon neutrality. At the core of this process is a calcium-based CO2 sorbent materials, which enable the in-situ conversion of captured CO2 into syngas through hydrogenation. The syngas quality is typically evaluated using the molar ratio of H2 to COxM value). The study aims to efficiently produce syngas with an M value of 2.00 - 2.05 through the proposed process, thereby providing a highly compatible feed gas for downstream processes such as Fischer-Tropsch process and methanol synthesis. Thermodynamic equilibrium analysis and calculations were performed for key operational parameters including temperature, pressure, and calcium-to-hydrogen molar ratio (n(CaCO3):n(H2)). Results indicated that the optimal operating conditions were 700 ℃, 0.1 MPa, and a calcium-to-hydrogen molar ratio of 1:2. Additionally, the presence of H2O was found to have an adverse impact on the hydrogenation conversion performance. Based on these findings, the screening of calcium-based natural ores was carried out through fixed-bed experimental research. The results demonstrated that dolomite exhibited superior ICCU-RWGS reactivity under reaction conditions of 700 ℃, 0.1 MPa, and a calcium-to-hydrogen molar ratio of 1:2, which aligned well with the thermodynamic predictions. Under these optimal conditions, the cyclic performance of dolomite was further evaluated. The results showed that the M value remained relatively stable over 20 cycles without significant decay, and no evident sintering was observed in the post-reaction dolomite, indicating excellent cyclic stability and structural durability. Overall, based on the ICCU-RWGS process, the study aims to enhance the molar proportion of COx in the product gas through systematic optimization of operational parameters, thereby producing high-quality syngas that meets the feedstock requirements for downstream chemical and fuel synthesis.

       

    /

    返回文章
    返回