Autor: |
Wang SM; School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an 710049, China., Shivanna M; Department of Chemical Sciences, Bernal Institute, University of Limerick, Limerick V94 T9PX, Republic of Ireland., Zheng ST; School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an 710049, China., Pham T; Department of Chemistry, University of South Florida, 4202 East Fowler Avenue, Tampa, Florida 33620, United States., Forrest KA; Department of Chemistry, University of South Florida, 4202 East Fowler Avenue, Tampa, Florida 33620, United States., Yang QY; School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an 710049, China., Guan Q; Key Laboratory of Oil and Gas Fine Chemicals of Ministry of Education, College of Chemical Engineering, Xinjiang University, Urumqi 830017, China., Space B; Department of Chemistry, University of South Florida, 4202 East Fowler Avenue, Tampa, Florida 33620, United States., Kitagawa S; Institute for Integrated Cell-Material Sciences, Kyoto University Institute for Advanced Study, Kyoto University, Yoshida Ushinomiya-cho, Sakyo-ku, Kyoto 606-8501, Japan., Zaworotko MJ; Department of Chemical Sciences, Bernal Institute, University of Limerick, Limerick V94 T9PX, Republic of Ireland. |
Abstrakt: |
Separating ethane (C 2 H 6 ) from ethylene (C 2 H 4 ) is an essential and energy-intensive process in the chemical industry. Here, we report two flexible diamondoid coordination networks, X-dia-1-Ni and X-dia-1-Ni 0.89 Co 0.11 , that exhibit gate-opening between narrow-pore (NP) and large-pore (LP) phases for C 2 H 6 , but not for C 2 H 4 . X-dia-1-Ni 0.89 Co 0.11 thereby exhibited a type F-IV isotherm at 273 K with no C 2 H 6 uptake and a high uptake (111 cm 3 g -1 , 1 atm) for the NP and LP phases, respectively. Conversely, the LP phase exhibited a low uptake of C 2 H 4 (12.2 cm 3 g -1 ). This C 2 H 6 /C 2 H 4 uptake ratio of 9.1 for X-dia-1-Ni 0.89 Co 0.11 far surpassed those of previously reported physisorbents, many of which are C 2 H 4 -selective. In situ variable-pressure X-ray diffraction and modeling studies provided insight into the abrupt C 2 H 6 -induced structural NP to LP transformation. The promise of pure gas isotherms and, more generally, flexible coordination networks for gas separations was validated by dynamic breakthrough studies, which afforded high-purity (99.9%) C 2 H 4 in one step. |