分子-旋转-工程金属-有机框架与各种相互透的程度/模式,具有可调节的多孔性/稳定性对二元/三元C2H2/CO2/C2H4分离
Zhen-Hua Guo1, Li-Qiu Yang2, Quan-Guo Zhai2
1Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, Shaanxi Key Laboratory of Physico-Inorganic Chemistry, College of Chemistry and Materials Science, Northwest University, Xi'an, 710127, P.R. China.
Angewandte Chemie (International ed. in English)
|October 7, 2025
概括
这项研究使用分子旋转器设计了相互透的金属有机框架 (MOF),以增强乙烯分离. 开发的MOF显示出对乙烯/乙烯和乙烯/二氧化碳混合物的高孔隙性和选择性.
科学领域:
- 材料科学 材料科学 材料科学
- 化学工程是化学工程的重要组成部分.
- 纳米技术 纳米技术
背景情况:
- 乙烯/乙烯和乙烯/二氧化碳混合物的有效分离对于化学工业至关重要.
- 相互透的金属有机框架 (MOFs) 提供了气体分离的潜力,但通常会与透性-稳定性权衡作斗争.
研究的目的:
- 开发具有调节孔隙性和稳定性的新型相互透的MOF,以应对具有挑战性的气体分离.
- 为了研究基于分子转子的辅配体对MOF结构和气体分离性能的影响.
- 从乙烯/二氧化碳/乙烯混合物中获得高纯度乙烯.
主要方法:
- 使用基于分子转子的协同配体 (,,) 来创建具有不同相互透性的MOF的晶体工程策略.
- 气体吸附测量以确定多孔性和乙吸收.
- 气体混合物分离性能评估的突破性实验.
- 理论计算和现场红外光谱学以阐明分离机制.
主要成果:
- 合成了具有不同纠度的三个MOF (Ni-dcpp-bpb,Ni-dcpp-bpn,Ni-dcpp-bpan).这些MOF具有不同的纠度.
- Ni-dcpp-bpb和Ni-dcpp-bpn表现出增强的多孔性 (27.2%/32.1%) 和高的乙吸收.
- Ni-dcpp-bpan表现出独特的旋转驱动门效应,使得压力依赖状态切换.
- 从复杂的C2H2/CO2/C2H4混合物中,通过使用Ni-dcpp-bpb.使用Ni-dcpp-bpb.实现了乙烯 (>99.9%) 的单步净化,具有基准生产率 (396.9 L kg-1).
- 分离机制被确定为C─HO/N和C─Hπ相互作用.
结论:
- 一种分子转子工程方法有效调节MOF中的相互透,平衡透性和稳定性.
- 开发的MOF为基于乙的高性能气体净化提供了一个强大的平台.
- 这项工作为乙分离和乙烯净化提供了新的基准.
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