摘要
煤矿主导的能源结构与密集采矿作业不可避免地导致有害颗粒物(PM)和温室气体(CO_(2))的同根同源排放,对气候环境及矿工生命安全构成严重威胁。传统多孔吸附剂因操作简便、吸附热低且易于再生等优势,在协同捕获有害颗粒物与气体领域备受关注。然而,吸附能力与传质阻力间的固有“权衡”效应,以及粉末加工成型后的低气体渗透性,严重制约其工业应用范围与前景。研究采用“自下而上”策略,将芴基功能砌块与1,3,5-三乙炔苯结构砌块通过交叉偶联反应实现碳-碳共价键高效结合,一锅法制备具有均匀孔结构、柔性可加工与环境耐受性的整体式块状共轭微孔聚合物吸附剂(D-CMPs)。具有刚性芳香π共轭骨架的D-CMPs在长时间高湿条件下表现出优异的结构和功能稳定性,对PM_(0.3)的捕获效率超过99.79%,对PM_(2.5)的捕获效率超过99.98%。在此基础上,由D-CMPs开放的三维分层多孔结构引起的“滑移效应”显著增强了气流分散,提高了气体吞吐量(最小渗透阻力仅17 Pa)。得益于连续均匀的分级孔隙性质和芴基功能位点的充分暴露,D-CMPs表现出良好的CO_(2)吸附与封存性能。在压力为1.0×10^(5) Pa、温度为273.15 K下,CO_(2)的吸附容量高达2.59 mmol/g。在低碳和清洁能源技术广泛采用之前,具有优异结构稳定性、孔隙可调性、环境耐受性和高吸附能力的多孔固体材料将成为矿井作业环境净化的优异候选对象。
The coal-mine-dominated energy structure and intensive mining operations inevitably result in co-source emissions of harmful particulate matter(PM)and greenhouse gases(CO_(2)),posing severe threats to the climatic environment and the safety of miners'lives.Traditional porous adsorbents have attracted significant attention in the field of synergistic capture of harmful particulates and gases,owing to their advantages such as facile operation,low adsorption heat,and easy regenerability.However,the inherent“trade-off”effect between adsorption capacity and mass transfer resistance,coupled with the low gas permeability of powdered adsorbents after processing and shaping,severely restricts their industrial application scope and prospects.In this study,a“bottom-up”strategy was employed to achieve efficient carbon-carbon covalent bonding between fluorene-based functional building blocks and 1,3,5-triethynylbenzene structural units via cross-coupling reactions,enabling the one-pot synthesis of monolithic conjugated microporous polymer adsorbents(D-CMPs)with uniform pore structures,flexible processability,and environmental tolerance.D-CMPs,featuring rigid aromatic π-conjugated backbones,exhibit excellent structural and functional stability under prolonged high-humidity conditions,with capture efficiencies exceeding 99.79% for PM_(0.3) and 99.98% for PM_(2.5).Furthermore,the“slip effect”induced by the open 3D hierarchical porous structure of D-CMPs significantly enhances gas flow dispersion and improves gas throughput(with a minimum permeation resistance of only 17 Pa).Bene-fiting from their continuous and uniform hierarchical porosity and the full exposure of fluorene-based functional sites,D-CMPs demonstrate favorable CO_(2) adsorption and sequestration performance.At a pressure of 1.0×10^(5) Pa and a temperature of 273.15 K,the CO_(2) adsorption capacity reaches as high as 2.59 mmol/g.Prior to the widespread adoption of low-carbon and clean ener-gy technologies,porous solid materials with excellent structural stability,tunable porosity,environmental tolerance,and high ad-sorption capacity will emerge as promising candidates for the purification of mine operation environments.
作者
李明利
汪少振
李湘
张一帆
尹媛
刘今
王存民
张明明
徐欢
LI Mingli;WANG Shaozhen;LI Xiang;ZHANG Yifan;YIN Yuan;LIU Jin;WANG Cunmin;ZHANG Mingming;XU Huan(Shendong Coal Group,CHN Group,Yulin 719315,China;School of Safety Engineering,China University of Mining and Technology,Xuzhou 221116,China;School of Materials Science and Physics,China University of Mining and Technology,Xuzhou 221116,China;Beijing Innowind Aerospace Equipment Co.,Ltd.,Beijing 100854,China;China Academy of Safety Science&Technology,Beijing 100012,China)
出处
《金属矿山》
北大核心
2025年第8期218-226,共9页
Metal Mine
基金
“十四五”国家重点研发计划项目(编号:2023YFC3011704)
中央高校基本科研业务费专项(编号:2024-10958,2024-10967)
中国矿业大学研究生创新计划项目(编号:2024WLJCRCZL195,2024WLKXJ143,2024WLKXJ140)
国家能源集团井工煤矿粉尘与职业病防治研究(六)煤矿粉尘防护装备研发项目(编号:E210100285)。
关键词
矿井环境净化
整体吸附剂
分级多孔结构
耐高温高湿
协同捕获
mine environment purification
monolithic adsorbent
hierarchical porous structure
high temperature and humidity resistance
cooperative capture
