Abstract: In the context of "carbon peak and carbon neutrality", carbon capture, utilization and storage (CCUS) technology is becoming increasingly important. The study of CO2 separation has attracted high-profile as it is the key link in the CCUS process. Among various separation methods, the membrane separation technology stands out with its advantages of low energy and continuous operation. This work reviews the current research status of various CO2 separation membranes for membrane-based carbon capture both domestically and overseas. It emphatically introduces the research progress regarding the CO2 gas permeation and separation performance, as well as the optimized preparation methods, of mixed matrix membrane. The CO2 permeance of most mixed matrix membranes ranges from 0 to 1000 Barrer, and the CO2/N2 separation coefficient is between 20 and 120. In addition, it is proposed that the preparation method of mixed matrix membrane can be optimized by using modified crystalline porous fillers or directly adopting amorphous porous fillers, thereby improving the compatibility between polymer substrates and porous fillers. Meanwhile, from the perspective of the actual needs of subsequent industrial applications, this review analyzes the advantages and disadvantages of various CO2 separation membrane modules, and proposes that the spiral-wound membrane module is the most suitable for the field of membrane-based carbon capture. Mixed matrix membrane exhibit excellent mechanical and thermal stability, outstanding resistance to plasticization, and excellent CO2 permeation and separation performance. Therefore, they have the greatest potential to be fabricated into spiral-wound membrane modules and applied in the field of membrane-based carbon capture in the future. Additionally, it can be concluded that with the current performance of mixed matrix membrane and suitable capture process conditions (e.g., the addition of purge gas), the CO2 capture cost can be controlled within 23 USD/t CO2. From this perspective, the application of mixed matrix membranes in membrane-based carbon capture technology is considered feasible. This work aims to provide guidance for the widespread application of CO2 membrane separation in CCUS technology as soon as possible.

Key words: CO2 capture, CCUS technology, membrane, membrane module, mixed matrix, permeation, industrial applications

摘要： 在“双碳”战略背景下，碳捕集、利用与封存(Carbon Capture, Utilization and Storage, CCUS)技术的重要性日益凸显。作为CCUS技术中的关键环节，CO2分离已成为当前的研究热点。在众多分离法中，膜分离技术凭借低能耗、可连续操作的优势脱颖而出。本工作全面综述了国内外各类CO2分离膜在膜法碳捕集领域的研究现状，重点介绍了混合基质膜的CO2气体渗透分离性能及制备方法的优化。目前，绝大多数混合基质膜的CO2渗透速率介于0~1000 Barrer之间，CO2/N2的分离系数在20~120范围内。研究表明，通过使用修饰改性的晶态多孔填料或直接使用非晶态多孔填料，可有效提升聚合物基底与多孔填料的兼容性，是优化混合基质膜制备方法的可行途径。从后续工业应用的实际需求出发，本工作剖析了不同CO2分离膜组件的优势与不足，明确螺旋卷式是当前最适用于膜法碳捕集领域的组件形式。混合基质膜具备优异的机械与热稳定性、杰出的抗塑化能力及卓越的CO2渗透分离性能，因此在利用螺旋卷式膜组件实现膜法碳捕集应用中展现最大潜力。此外，在添加吹扫气等合适的捕集工艺条件下，基于当前混合基质膜的性能，CO2捕集成本可控制在23 USD/t CO2以内。充分证明了混合基质膜在膜法碳捕集技术中应用的可行性，本工作旨在为CO2膜分离在CCUS技术中的广泛应用提供有力指导。

关键词: 二氧化碳捕集, CCUS技术, 膜, 膜组件, 混合基质, 渗透, 工业应用