Abstract
A two-dimensional lanthanum(III) porous coordination polymer was prepared, characterized and applied as an efficient adsorbent for the removal of uranium from aqueous solution. Lanthanum(III) was the metal center of MOFs, and the deprotonated anions of pyridine-2,6-dicarboxylic acid (H2PDA), PDA2− was the organic ligand, this MOF was name as La-PDA, which was synthesized by hydrothermal reaction method. Scanning electron microscope (SEM), Fourier transform infrared (FTIR), powder X-ray diffraction (PXRD) and thermal gravimetric (TG) analysis were used for characterization, and the results indicated that the La-PDA composites were successfully prepared. Compared with traditional adsorbents of uranium, La-PDA showed excellent adsorption properties. The adsorption capacity was 247.6 mg g−1 at 298 K and pH 4.0. The adsorption equilibrium achieved within 120 min, and the adsorption process was exothermic and spontaneous. The absorption mechanism of La-PDA was also explored, from the XPS spectra, the pyridine-like nitrogen atoms (C=N–C) and carboxyl oxygen atoms (–COO–) contributed to the adsorption of uranium. The results suggested that PDA2− was a potential ligand of uranium adsorption, La-PDA composites were effective adsorbents for the removal of uranium from aqueous solution.
Funding source: National Key Research and Development Program
Award Identifier / Grant number: 2016YFC1402507
Funding source: National Natural Science Foundation of China
Award Identifier / Grant number: 51578307
Award Identifier / Grant number: IRT-13026
Funding statement: The research was supported by the National Key Research and Development Program (2016YFC1402507), the National Natural Science Foundation of China (51578307), and the Program for Changjiang Scholars and Innovative Research Team in University (IRT-13026).
List of abbreviations
- AO
amidoxime
- b
the Langmuir constant (L mg−1)
- c0
the initial concentration of uranium (mg L−1)
- ce
the equilibrium concentration of uranium (mg L−1)
- ct
the concentration of uranium at time t (mg L−1)
- EDS
energy dispersive spectrometer
- FTIR
Fourier transform infrared
- ΔG0
the Gibbs free energy changes (kJ mol−1)
- ΔH0
the standard enthalpy changes (kJ mol−1)
- HKUST-1
Cu-BTC (BTC=pyridine-2,6-dicarboxylate)
- H2BDC
benzene-1,4-dicarboxylic acid
- H3BTC
benzene-1,3,5-tricarboxylic acid
- H2PDA
pyridine-2,6-dicarboxylic acid
- Kd
the distribution coefficient (mL g−1)
- Kf
Freundlich constant [(mg g−1) (L mg−1)1/n]
- k1
the pseudo-first-order rate constant (min−1)
- k2
the pseudo-second-order rate constant (g mg−1 min−1)
- La-PDA
{[La4(PDA)10(H2O)8]·2H2O}n (PDA=pyridine-2,6-dicarboxylate)
- MIL-101(Cr)
Cr-BDC (BDC=benzene-1,4-dicarboxylate)
- MIL-53
M(OH)(O2C-C6H4-CO2) (M=Al, Cr)
- MOFs
metal–organic frameworks
- MOF-76
Tb-BTC (BTC=pyridine-2,6-dicarboxylate)
- m
the weight of the adsorbents (mg)
- n
Freundlich exponent (dimensionless)
- PTFE
polytetrafluoroethylene
- PXRD
powder X-ray diffraction
- qe
the equilibrium adsorption capacity (mg g−1)
- qt
the adsorption capacity at time t (mg g−1)
- qm
the capacity of Langmuir adsorption (mg g−1)
- R
the ideal gas constant (8.314 J mol−1 K−1)
- r2
the corresponding correlation
- SEM
scanning electron microscope
- ΔS0
the standard entropy changes (J mol−1 K−1)
- T
the thermodynamic temperature (K)
- TG
thermal gravimetric analysis
- UiO-66
Zr-BDC (BDC=benzene-1,4-dicarboxylate)
- UiO-68
Zr-TPDC (TPDC=terphenyl-4,4′-dicarboxylate)
- V
the volume of the solution (mL)
- XPS
X-ray photoelectron spectroscopy
- Zn-MOF-74
Zn-DOBDC (DOBDC=2,5-dioxidobenzene-1,4-dicarboxylate)
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