Design of Ultra‑Stable Solid Amine Adsorbents and Mechanisms of Hydroxyl Group‑Dependent Deactivation for Reversible CO_(2)Capture from Flue Gas  

作　　者：Meng Zhao Liang Huang Yanshan Gao Ziling Wang Shuyu Liang Xuancan Zhu Qiang Wang Hong He Dermot O’Hare 

机构地区：[1]College of Environmental Science and Engineering,Beijing Forestry University,Beijing 100083,People’s Republic of China [2]State Key Laboratory of Efficient Production of Forest Resources,Beijing Forestry University,Beijing 100083,People’s Republic of China [3]Research Center of Solar Power and Refrigeration,Institute of Refrigeration and Cryogenics,Shanghai Jiao Tong University,Shanghai 200240,People’s Republic of China [4]State Key Joint Laboratory of Environment Simulation and Pollution Control,Research Centre for Eco-Environmental Sciences,Chinese Academy of Sciences,Beijing 100085,People’s Republic of China [5]Chemistry Research Laboratory,Department of Chemistry,University of Oxford,Mansfield Road,Oxford OX13TA,UK

出　　处：《Nano-Micro Letters》2025年第7期355-373,共19页纳微快报(英文版)

基　　金：supported by the Fundamental Research Funds for the National Natural Science Foundation of China 52225003,22208021,22109004;the National Key R&D Program of China 2022YFB4101702.

摘　　要：Although supported solid amine adsorbents have attracted great attention for CO_(2) capture,critical chemical deactivation problems including oxidative degradation and urea formation have severely restricted their practical applications for flue gas CO_(2) capture.In this work,we reveal that the nature of surface hydroxyl groups(metal hydroxyl Al–OH and nonmetal hydroxyl Si–OH)plays a key role in the deactivation mechanisms.The polyethyleneimine(PEI)supported on Al–OH-containing substrates suffers from severe oxidative degradation during the CO_(2) capture step due to the breakage of amine-support hydrogen bonding networks,but exhibits an excellent anti-urea formation feature by preventing dehydration of carbamate products under a pure CO_(2) regeneration atmosphere.In contrast,PEI supported on Si–OHcontaining substrates exhibits excellent anti-oxidative stability under simulated flue gas conditions by forming a robust hydrogen bonding protective network with Si–OH,but suffers from obvious urea formation during the pure CO_(2) regeneration step.We also reveal that the urea formation problem for PEI-SBA-15 can be avoided by the incorporation of an OH-containing PEG additive.Based on the intrinsic understanding of degradation mechanisms,we successfully synthesized an adsorbent 40PEI-20PEG-SBA-15 that demonstrates outstanding stability and retention of a high CO_(2) capacity of 2.45 mmol g^(−1) over 1000 adsorption–desorption cycles,together with negligible capacity loss during aging in simulated flue gas(10%CO_(2)+5%O_(2)+3%H_(2)O)for one month at 60–70℃.We believe this work makes great contribution to the advancement in the field of ultra-stable solid amine-based CO_(2) capture materials.

关 键 词：CO_(2)capture Solid amine adsorbent Long-term stability Oxidative degradation Urea formation 

分 类 号：X701.2[环境科学与工程—环境工程]