Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 10, Issue 28, Pages 23918-23927Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b07130
Keywords
rare earth elements; metal-organic frameworks; organic functionalization; adsorption equilibrium; adsorption kinetics; structural stability
Funding
- Basic Science Research Program through National Research Foundation of Korea (NRF)
- Ministry of Education [NRF-2015R1A4A1042434]
- National Strategic Project Carbon Upcycling project of the National Research Foundation of Korea (NRF)
- Ministry of Science and ICT (MSIT)
- Ministry of Environment (ME)
- Ministry of Trade, Industry, and Energy (MOTIE) [NRF-2017M3D8A2086050]
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Efficient rare earth elements (REEs) separation and recovery are crucial to meet the ever-increasing demand for REEs extensively used in various high technology devices. Herein, we synthesized a highly stable chromium-based metal organic framework (MOF) structure, Cr-MIL-101, and its derivatives with different organic functional groups (MIL-101-NH2, MIL-101-ED (ED: ethylenediamine), MIL-101-DETA (DETA: diethylenetriamine), and MIL-101-PMIDA (PMIDA: N-(phosphonomethyl)iminodiacetic acid)) and explored their effectiveness in the separation and recovery of La3+, Ce3+, Nd3+, Sm3+, and Gd3+ in aqueous solutions. The prepared materials were characterized using various analytical instrumentation. These MOFs showed increasing REE adsorption capacities in the sequence MIL-101 < MIL-101-NH2 < MIL-101-ED < MIL-101-DETA < MIL-101-PMIDA. MIL-101-PMIDA showed superior REE adsorption capacities compared to other MOFs, with Gd3+ being the element most efficiently adsorbed by the material. The adsorption of Gd3+ onto MIL-101-PMIDA was examined in detail as a function of the solution pH, initial REE concentration, and contact time. The obtained adsorption equilibrium data were well represented by the Langmuir model, and the kinetics were treated with a pseudo-second-order model. A plausible mechanism for the adsorption of Gd3+ on MIL-101-PMIDA was proposed by considering the surface complexation and electrostatic interaction between the functional groups and Gc(3+) ions under different pH conditions. Finally, recycling tests were carried out and demonstrated the higher structural stability of MIL-101-PMIDA during the five adsorption-regeneration runs.
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