填充流化床集成水煤气变换与二氧化碳矿化的模拟分析  

Simulation study on the integration of water-gas shift and CO_(2)-mineralization in a packed fluidized bed

作　　者：常麒 葛蔚[1,2] CHANG Qi;GE Wei(State Key Laboratory of Mesoscience and Engineering,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China;School of Chemical Engineering,University of Chinese Academy of Sciences,Beijing 101408,China)

机构地区：[1]中国科学院过程工程研究所介科学与工程全国重点实验室,北京100190 [2]中国科学院大学化学工程学院,北京101408

出　　处：《化工学报》2024年第11期4237-4253,共17页CIESC Journal

基　　金：国家自然科学基金项目(22293024)。

摘　　要：提出了在填充流化床中以矿物碳酸化(MC)原位封存水煤气变换反应(WGSR)制备H2副产CO_(2)的连续操作新工艺。除了借助WGSR的高温、高压、高湿环境强化MC,吸收剂粉末流化通过WGSR催化剂填充床的连续分离可应对产物层增厚导致的MC吸收速率快速衰减。基于晶粒尺度溶解扩散MC模型和WGSR表观动力学建立了该反应器的一维稳态活塞流模型,以此分析了750 MW整体气化联合循环(IGCC)装置中应用此新工艺的技术经济性。基于模拟获得的CO_(2)、MC吸收剂粉末转化率及给定能耗、碳税等计算CO_(2)减排费用表明:将MC吸收剂的碳酸化产物作为水泥辅助性凝胶材料(SCM)产生附加值是此技术商业化的前提;考虑CO_(2)、MC吸收剂粉末转化率与研磨能耗,宜采用10μm左右的MC吸收剂细粉末。A new continuous operation process was proposed for in-situ sequestrating the by-product CO_(2)of watergas shift reaction(WGSR)by mineral carbonation(MC)in a packed fluidized bed.In addition to utilizing the high temperature,pressure,and humidity environment of WGSR to intensify MC,the continuous separation of sorbent powders by their fluidization through WGSR catalyst packed bed can cope with the rapid decay of MC absorption rate caused by thickening of the product layer.Based on the grain-scale solution-diffusion MC model and the WGSR apparent kinetics,a one-dimensional steady-state plug flow model of the reactor was established to analyze the technical and economic feasibility of applying this new process in a 750 MW integrated gasification combined cycle(IGCC)unit.The CO_(2)mitigation cost is calculated based on the simulated conversion rates of CO_(2)and MC sorbent,with given energy consumption,carbon tax,etc.It shows that obtaining added value from the carbonation product of MC sorbent as supplementary cementitious materials(SCM)is a prerequisite for the commercialization of this technology.Considering the conversion rates of CO_(2)and MC sorbent powder and the grinding energy consumption,MC sorbent fine powders of about 10μm in diameter is preferred.

关 键 词：多相反应器 制氢 水煤气变换 二氧化碳捕集 矿化 填充流化床 活塞流模型 整体气化联合循环 

分 类 号：X511[环境科学与工程—环境工程] TQ116.2[化学工程—无机化工] TQ019