Journal
CHEMICAL ENGINEERING JOURNAL
Volume 311, Issue -, Pages 20-27Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2016.11.067
Keywords
Adsorption; Desulfurization; Cu(I) and Ce(IV) ions; Metal-organic framework; Synergistic effect
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Funding
- National Research Foundation of Korea (NRF) - Ministry of Science, ICT and future Planning [2015R1A2A1A15055291]
- Dongil Culture and Scholarship Foundation of Korea
- National Research Foundation of Korea [2015R1A2A1A15055291] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Copper and cerium oxides were synthesized via a new way within a highly porous metal-organic framework (MOF; here, MIL-101 or chromium-benzenedicarboxylate) in a consecutive manner under mild conditions for the first time. The crystal structure of MIL-101 remained intact after loading of the two metal oxides using this approach. The efficiencies of the new adsorbents in selective adsorptive removal of benzothiophene (BT) from a model liquid fuel were evaluated. Compared with that of virgin MOF, the maximum adsorption capacity (Q(0)) of the modified MIL-101 increased by 57% and 188%, based on the weight and unit surface area, respectively. The increased Q(0) could be explained by the synergistic effect of pi-complexation (between Cu(I) and BT) and direct bond formation (between Ce(IV) and S) on BT adsorption. Moreover, Cu-Ce/MIL-101, unlike Cu/MIL-101, selectively adsorbed BT even in the presence of an aromatic additive (toluene) because Ce(IV) could effectively bind to sulfur in BT (without interacting with the aromatic ring). The adsorbent was reused in up to four cycles without significant loss of BT adsorption capacity, and it was presumed that the presence of Ce species could stabilize the +1 oxidation state of Cu via a redox phenomenon throughout the synthesis regeneration processes. (C) 2016 Elsevier B.V. All rights reserved.
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