TY - JOUR
T1 - Concurrent Manipulation of Out-of-Plane and Regional In-Plane Orientations of NH2-UiO-66 Membranes with Significantly Reduced Anisotropic Grain Boundary and Superior H2/CO2 Separation Performance
AU - Sun, Yanwei
AU - Song, Chunshan
AU - Guo, Xinwen
AU - Liu, Yi
N1 - Funding Information:
The authors are grateful to the National Natural Science Foundation of China (21176231), the Liaoning Revitalization Talents Program (XLYC1807084), the Thousand Youth Talents Program, the Pennsylvania State University, and the Technology Innovation Team of Dalian University of Technology (DUT2017TB01) for the financial support.
Publisher Copyright:
Copyright © 2019 American Chemical Society.
PY - 2020/1/29
Y1 - 2020/1/29
N2 - Preferred orientation has proven to exert a significant impact on the gas separation performance of metal-organic framework membranes. Nevertheless, realizing three-dimensional orientation control remains a challenging issue. In this study, well-intergrown NH2-UiO-66 membranes with both (111) out-of-plane and regional in-plane orientations were prepared by combining oriented deposition of seeds and solvothermal epitaxial growth. Dynamic air-liquid interface-assisted self-assembly method was employed to organize uniform octahedral-shaped NH2-UiO-66 seeds into closely packed monolayers with (111) out-of-plane and regional in-plane orientations, whereas the use of ZrS2 as the zirconium precursor during the solvothermal epitaxial growth was found indispensible for sealing the intercrystalline gaps while preserving the preferred orientation inherited from seed layers. In addition, compared with solvothermal heating, employing microwave heating led to poor intergrowth between neighboring NH2-UiO-66 crystals because of a lower dielectric loss factor of the reaction medium. Gas permeation results indicated that the prepared NH2-UiO-66 membranes exhibited H2/CO2 selectivity up to 5.5 times higher than their counterparts with random and/or mere out-of-plane orientations as well as H2 permeability 14.5 times higher than NH2-MIL-125(Ti) membranes with mere out-of-plane orientation under similar operating conditions.
AB - Preferred orientation has proven to exert a significant impact on the gas separation performance of metal-organic framework membranes. Nevertheless, realizing three-dimensional orientation control remains a challenging issue. In this study, well-intergrown NH2-UiO-66 membranes with both (111) out-of-plane and regional in-plane orientations were prepared by combining oriented deposition of seeds and solvothermal epitaxial growth. Dynamic air-liquid interface-assisted self-assembly method was employed to organize uniform octahedral-shaped NH2-UiO-66 seeds into closely packed monolayers with (111) out-of-plane and regional in-plane orientations, whereas the use of ZrS2 as the zirconium precursor during the solvothermal epitaxial growth was found indispensible for sealing the intercrystalline gaps while preserving the preferred orientation inherited from seed layers. In addition, compared with solvothermal heating, employing microwave heating led to poor intergrowth between neighboring NH2-UiO-66 crystals because of a lower dielectric loss factor of the reaction medium. Gas permeation results indicated that the prepared NH2-UiO-66 membranes exhibited H2/CO2 selectivity up to 5.5 times higher than their counterparts with random and/or mere out-of-plane orientations as well as H2 permeability 14.5 times higher than NH2-MIL-125(Ti) membranes with mere out-of-plane orientation under similar operating conditions.
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U2 - 10.1021/acsami.9b18804
DO - 10.1021/acsami.9b18804
M3 - Article
C2 - 31873001
AN - SCOPUS:85078693540
SN - 1944-8244
VL - 12
SP - 4494
EP - 4500
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 4
ER -