Abstract:

The massive emission of CO₂ is one of the primary reasons behind global warming. CO₂ capture, utilization and storage (CCUS) technology stands as a pivotal means to reduce CO₂ emissions. However, the high capture costs in CCUS technology limit its widespread application. This study employed an Integrated Carbon Capture and Conversion (ICCC) technology, which coupled the capture process with the conversion process, thereby avoiding the substantial energy consumption required for the regeneration of CO₂ capture materials and reducing the cost of the CCUS capture process. The experiment utilized non-precious metals based on Fe and Co as catalytic components and Ca as the adsorption component. A series of Fe _x Co _y Ca₃Al dual-functional materials were prepared using a co-current co-precipitation method for application in the ICCC process for syngas production. The influence of the Fe/Co ratio on the performance of the dual-functional materials was investigated. The dual-functional materials were characterized using techniques such as TEM, XPS, H₂-TPR and CO₂-TPD. The relevant results indicated that the elements Fe, Co, Ca and Al in the dual-functional materials were uniformly distributed without aggregation. There was an interaction between Fe and Co elements, enhancing the integrated performance of the dual-functional materials. Under optimized conditions, the Fe_0.5Co_0.5Ca₃Al material exhibited a CO₂ capture capacity of 11.05mmol/g and a CO yield of 11.94mmol/(g∙h).

Key words: integrated carbon capture and conversion, reverse water gas shift reaction, synthesis gas, dual-function materials, greenhouse gas, catalyst

摘要：

二氧化碳（CO₂）的大量排放是导致全球变暖的主要原因之一，其中CO₂捕集、利用与封存（CO₂ capture, utilization and storage，CCUS）技术是减少碳排放的关键手段，然而传统CCUS技术中捕集成本较高，限制了CCUS技术的推广应用。本文采用CO₂捕集-转化一体化（integrated carbon capture and conversion，ICCC）技术方案，通过将碳捕集过程与碳转化过程相耦合，避免CO₂捕集材料再生所需的大量能耗，从而降低CCUS捕集过程成本。实验以Fe、Co基非贵金属作为催化组分，Ca为吸附组分，采用并流共沉淀的方法制备了Fe _x Co _y Ca₃Al系列双功能材料，应用于ICCC制备合成气过程，探究了Fe/Co对双功能材料性能的影响，通过透射电子显微镜、X射线光电子能谱、H₂-程序升温还原、CO₂-程序升温脱附等对双功能材料进行表征，相关结果表明双功能材料Fe、Co、Ca、Al等元素分布均匀，未出现团聚现象，Fe-Co元素之间存在相互作用，提升了双功能材料的一体化性能。在优化条件下，Fe_0.5Co_0.5Ca₃Al材料CO₂捕集容量为11.05mmol/g，CO产率达到11.94mmol/(g∙h)。

关键词: CO₂捕集-转化一体化, 逆水煤气变换, 合成气, 双功能材料, 温室气体, 催化剂