摘要
当前我国气候治理已进入“双碳”目标实施的攻坚期。CO_(2)捕集、利用与封存(CCUS)是电力、化工、钢铁等行业实现零碳乃至负碳排放的关键托底技术。其中,燃煤烟气具有排放量大、CO_(2)分压低的特征,基于有机胺的化学吸收法是目前最成熟有效的捕集手段,通过有机胺与CO_(2)发生可逆反应实现高效捕集,但CO_(2)解吸能耗过高限制了该技术的规模化应用。固体酸催化剂(SACs)通过加速质子转移和降低C—N键断裂能垒,可显著提升CO_(2)解吸速率并降低再生温度,兼具节能降本与提升效率的双重优势。系统综述了不同种类的SACs在胺溶液中的催化CO_(2)解吸最新研究进展,研究表明催化剂经表面修饰、磺酸化改性、催化剂表面亲水性与酸性位点密度调控等策略,可显著提升CO_(2)解吸效率,并全面分析了催化材料的物化性能、催化剂结构及表征方法。在此基础上,进一步揭示了SACs中路易斯酸与布朗斯特酸位点的协同机制,路易斯酸吸附氧原子引发C—N键异构断裂、布朗斯特酸提供质子促进氨基甲酸盐质子化,阐述了SACs催化CO_(2)解吸反应机理,而催化剂碱性活性位点构筑有效促进CO_(2)解吸效率,提升解吸性能。最后,根据不同催化剂的特点,对工业应用潜力进行了分析比较。未来研究需聚焦酸性位点稳定性提升、催化剂规模化制备及与新型吸收剂、如相变胺吸收剂的耦合设计,以推动CCUS技术低成本落地。
Global climate governance has now entered a critical stage for implementing the“Dual Carbon”strategy.Carbon Capture,Utilization and Storage(CCUS)is a key supporting technology for achieving carbon neutrality to net-negative emissions in industries such as power,chemical,and steel.Among these,coal-fired flue gas is characterized by large emission volumes and low CO_(2)partial pressure.Amine-based chemical absorption is currently the most mature and effective capture method,achieving efficient capture through reversible reactions between organic amines and CO_(2).However,excessively high energy consumption during CO_(2)desorption restricts the large-scale application of this technology.Solid acid catalysts(SACs)can significantly increase CO_(2)desorption rates and reduce regeneration temperatures by accelerating proton transfer and lowering the energy barrier for C-N bond cleavage,offering dual advantages of saving energy/reducing costs and enhancing efficiency.We systematically review the latest research advances in SACcatalyzed CO_(2)desorption from amine solutions across different catalyst types.Studies show that strategies including surface modification,sulfonation,and regulation of catalyst surface hydrophilicity and acid site density can significantly improve CO_(2)desorption efficiency.We comprehensively analyze the physicochemical properties,catalyst structures,and characterization methods of catalytic materials.Building on this,we further reveal the synergistic mechanism between Lewis acid and Brønsted acid sites in SACs:Lewis acid adsorbs oxygen atoms to induce isomeric cleavage of C-N bonds,while Brønsted acid provides protons to promote carbamate protonation.This elucidates the reaction mechanism of SAC-catalyzed CO_(2)desorption.Moreover,constructing alkaline active sites on catalysts effectively enhances CO_(2)desorption efficiency and improves desorption performance.Finally,we analyze and compare the industrial application potential based on characteristics of different catalysts.Future research needs to focus on enhancing acid site stability,scaling up catalyst preparation,and coupling design with novel absorbents(e.g.,phase-change amine absorbents)to promote low-cost implementation of CCUS technology.
作者
杨蒙
房昆
王珊珊
陆诗建
侯婷
杨菲
黄志刚
梅杰琼
YANG Meng;FANG Kun;WANG Shanshan;LU Shijian;HOU Ting;YANG Fei;HUANG Zhigang;MEI Jieqiong(Beijing Design Branch of China Petroleum Engineering&Construction Corporation,Beijing 100085,China;Jiansu Key Laboratory of Coal-Based Greenhouse Gas Control and Utilization,China University of Mining and Technology,Xuzhou 221008,China;Institute of Carbon Neutralization,China University of Mining and Technology,Xuzhou 221116,China)
出处
《洁净煤技术》
北大核心
2025年第8期51-64,共14页
Clean Coal Technology
基金
中国石油天然气股份有限公司科学研究与技术开发资助项目(2021ZZ01-07)
浙江省“尖兵”“领雁”研发攻关计划资助项目(2023C03156)
2023年度江苏省碳达峰碳中和科技创新专项资助项目(BE2023852)
中央高校基本科研业务费项目-科研基地建设专项资助项目(2023KYJD1004)。
关键词
化学吸收法
胺溶液
固体酸催化
表征方法
催化性能
chemical absorption method
amine solution
solid acid catalysis
characterization methods
catalytic performance
作者简介
杨蒙(1984-),男,山东临沂人,高级工程师,博士研究生。E-mail:yangmeng.cpe@cnpc.com.cn;通讯作者:陆诗建(1984-),男,河南濮阳人,研究员,博士。E-mail:lushijian@cumt.edu.cn。
