title: In-situ observation for growth of hierarchical metal-organic frameworks and their self-sequestering mechanism for gas storage.
abstract: Although structures with the single functional constructions and micropores were demonstrated to capture many different molecules such as carbon dioxide, methane, and hydrogen with high capacities at low temperatures, their feeble interactions still limit practical applications at room temperature. Herein, we report in-situ growth observation of hierarchical pores in pomegranate metal-organic frameworks (pmg-MOFs) and their self-sequestering storage mechanism, not observed for pristine MOFs. Direct observation of hierarchical pores inside the pmg-MOF was evident by in-situ growth X-ray measurements while self-sequestering storage mechanism was revealed by in-situ gas sorption X-ray analysis and molecular dynamics simulations. The results show that meso/macropores are created at the early stage of crystal growth and then enclosed by micropore crystalline shells, where hierarchical pores are networking under self-sequestering mechanism to give enhanced gas storage. This pmg-MOF gives higher CO2 (39%) and CH4 (14%) storage capacity than pristine MOF at room temperature, in addition to fast kinetics with robust capacity retention during gas sorption cycles, thus giving the clue to control dynamic behaviors of gas adsorption.
authors.affiliation: Department of Materials Science &Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 305-701, Republic of Korea.
authors.forename: Jung
authors.initials: J
authors.lastname: Hyo Park
authors.affiliation: Department of Materials Science &Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 305-701, Republic of Korea.
authors.forename: Kyung Min
authors.initials: KM
authors.lastname: Choi
authors.affiliation: Department of Materials Science &Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 305-701, Republic of Korea.
authors.forename: Hyung Joon
authors.initials: HJ
authors.lastname: Jeon
authors.affiliation: Department of Materials Science &Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 305-701, Republic of Korea.
authors.forename: Yoon
authors.initials: Y
authors.lastname: Jung Choi
authors.affiliation: 1] Department of Materials Science &Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 305-701, Republic of Korea [2] Graduate School of EEWS, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 305-701, Republic of Korea.
authors.forename: Jeung Ku
authors.initials: JK
authors.lastname: Kang