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Overcoming the Trade-Off between C2H2 Sorption and Separation Performance by Regulating Metal-Alkyne Chemical Interaction in Metal-Organic Frameworks |
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| Authors: | Yan-Xi Tan Jing Lin Prof Qiao-Hong Li Liqiong Li Rahul Anil Borse Prof Weigang Lu Prof Yaobing Wang Prof Daqiang Yuan |
| Institution: | 1. State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002 Fujian, P. R. China
Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, 350108 Fujian, P. R. China University of Chinese Academy of Sciences, Beijing, 100049 P. R. China These authors contributed equally to this work.;2. State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002 Fujian, P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, 350108 Fujian, P. R. China These authors contributed equally to this work.;3. State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002 Fujian, P. R. China University of Chinese Academy of Sciences, Beijing, 100049 P. R. China;4. College of Chemistry and Materials Science, Jinan University, Guangzhou, 510632 Guangdong, P. R. China;5. State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002 Fujian, P. R. China |
| Abstract: | Designing porous materials for C2H2 purification and safe storage is essential research for industrial utilization. We emphatically regulate the metal-alkyne interaction of PdII and PtII on C2H2 sorption and C2H2/CO2 separation in two isostructural NbO metal–organic frameworks (MOFs), Pd/Cu-PDA and Pt/Cu-PDA . The experimental investigations and systematic theoretical calculations reveal that PdII in Pd/Cu-PDA undergoes spontaneous chemical reaction with C2H2, leading to irreversible structural collapse and loss of C2H2/CO2 sorption and separation. Contrarily, PtII in Pt/Cu-PDA shows strong di-σ bond interaction with C2H2 to form specific π-complexation, contributing to high C2H2 capture (28.7 cm3 g?1 at 0.01 bar and 153 cm3 g?1 at 1 bar). The reusable Pt/Cu-PDA efficiently separates C2H2 from C2H2/CO2 mixtures with satisfying selectivity and C2H2 capacity (37 min g?1). This research provides valuable insight into designing high-performance MOFs for gas sorption and separation. |
| Keywords: | Acetylene Capture Breakthrough Experiment Metal-Alkyne Chemistry Metal-Organic Framework Sorption and Separation |