TY - JOUR
T1 - Preparation of granulated UIO-66/graphene oxide using polyacrylamide/polyvinyl alcohol for selective fluoride removal
T2 - Mechanism studies via in situ surface-enhanced raman spectroscopy analysis and continuous-flow column operation
AU - Yoon, So Yeon
AU - Choong, Choe Earn
AU - Nam, Seong Nam
AU - Park, Chang Min
AU - Yoon, Yeomin
AU - Choi, Eun Ha
AU - Jang, Min
N1 - Publisher Copyright:
© 2024 Elsevier B.V.
PY - 2024/6/15
Y1 - 2024/6/15
N2 - The UIO-66 type of metal–organic frameworks (MOFs) showed excellent performance in water purification, however, the recovery difficulty for powdered UIO-66 remains challenging for the practical applications. Herein, we prepared granular adsorbents (gGO-U-N) derived from a UIO-66/GO composite and granulated them using polyacrylamide (PAM) and polyvinyl alcohol (PVA) polymers to improve F- removal capacity. The gGO-U-N resulted in C24O16Zr3 lattice contraction, improving the Coulomb interactions in Zr4+ for better F- interaction. Consequently, gGO-U-50 with 50 % (w/w) of UIO-66 mass ratio showed a higher F- adsorption capacity (102 mg g−1) than powdered UIO-66 (67 mg g−1), exhibiting high synergistic factor (fsyn = 2.1) for F- adsorption. Additionally, gGO-U-50 exhibited stable adsorption capability over a wide pH range and higher F- adsorption selectivity than gGO. Based on time-lapse Fourier transform infrared attenuated total reflection, X-ray photoelectron spectroscopy, and in situ Raman spectroscopic analysis, the Zr-O-C bond on gGO-U-50 was found to serve as the dominant F- sorption site, while the carbon–oxygen and amine groups contributed a minor portion for F- removal. Notably, the gGO-U-50 exhibited the F- water treatment cost of 1621.6 mg-F $-1, which is approximately 3 times cost-effective than the UIO-66 (632.07 mg-F $-1). Fixed-bed column experiments demonstrated that gGO-U-50 exhibited a higher F- adsorption capability (6.34 mg g−1) than other reported granular adsorbents, revealing that gGO-U-50 has the potential for F- remediation.
AB - The UIO-66 type of metal–organic frameworks (MOFs) showed excellent performance in water purification, however, the recovery difficulty for powdered UIO-66 remains challenging for the practical applications. Herein, we prepared granular adsorbents (gGO-U-N) derived from a UIO-66/GO composite and granulated them using polyacrylamide (PAM) and polyvinyl alcohol (PVA) polymers to improve F- removal capacity. The gGO-U-N resulted in C24O16Zr3 lattice contraction, improving the Coulomb interactions in Zr4+ for better F- interaction. Consequently, gGO-U-50 with 50 % (w/w) of UIO-66 mass ratio showed a higher F- adsorption capacity (102 mg g−1) than powdered UIO-66 (67 mg g−1), exhibiting high synergistic factor (fsyn = 2.1) for F- adsorption. Additionally, gGO-U-50 exhibited stable adsorption capability over a wide pH range and higher F- adsorption selectivity than gGO. Based on time-lapse Fourier transform infrared attenuated total reflection, X-ray photoelectron spectroscopy, and in situ Raman spectroscopic analysis, the Zr-O-C bond on gGO-U-50 was found to serve as the dominant F- sorption site, while the carbon–oxygen and amine groups contributed a minor portion for F- removal. Notably, the gGO-U-50 exhibited the F- water treatment cost of 1621.6 mg-F $-1, which is approximately 3 times cost-effective than the UIO-66 (632.07 mg-F $-1). Fixed-bed column experiments demonstrated that gGO-U-50 exhibited a higher F- adsorption capability (6.34 mg g−1) than other reported granular adsorbents, revealing that gGO-U-50 has the potential for F- remediation.
KW - Adsorption
KW - Fluoride removal
KW - Granulation
KW - Graphene oxide
KW - Metal-organic framework
KW - UIO-66
UR - http://www.scopus.com/inward/record.url?scp=85191614067&partnerID=8YFLogxK
U2 - 10.1016/j.cej.2024.151217
DO - 10.1016/j.cej.2024.151217
M3 - Article
AN - SCOPUS:85191614067
SN - 1385-8947
VL - 490
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 151217
ER -