<p>Recovery of rare earth elements (REEs) from industrial runoff is a sustainable approach for resource recycling and environmental treatment. We report the one-pot fabrication of HKUST-1-graphene oxide (HKUST-1-GO) composite for the recovery of La(III), an indispensable component in hydrogen storage materials and fuel cells, from aqueous solutions. The as-fabricated HKUST-1-GO was intensively characterized using X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, Brunauer-Emmett-Teller (BET), Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. HKUST-1-GO was then used as an adsorbent to recover La(III), and the recovery efficacy was evaluated via batch adsorption and optimized through the use of response surface methodology (RSM). In addition, the adsorption mechanism was meticulously explored through both theoretical and experimental investigations. The derived results are summarized as follows: (1) HKUST-1-GO has a prominent BET specific surface area of 1522.8029 m<sup>2</sup> g<sup>−1</sup>; (2) a recovery percentage of 95.54% for La(III) was achieved in 80 min, and the maximum Langmuir adsorption capacity reached 1090.24 mg g<sup>−1</sup>; (3) through applying RSM, the optimum La(III) recovery efficacy was found to be 97.133% through applying HKUST-1-GO at a dosage of 407.760 mg L<sup>−1</sup>, at pH 6.0, and with a contact time of 87.235 min; (4) statistical physics calculations determined that the adsorption process is exothermic and spontaneous, accompanied by an increase in entropy. Through isotherm and kinetic fittings, the adsorption was classified as favorable chemisorption controlled by surface reaction. Moreover, adsorbent speciation analysis and multifarious spectroscopic exploration showed the involvement of O–H, C=O, and C–O in La(III) uptake via electron donation to form La–O bonds, and electrostatic attraction was found to be involved in adsorption. Through this study, the recovery efficacy and mechanism of HKUST-1-GO toward La(III) were determined, and the results can be used as a constructive reference for tailoring MOF-based materials in the recycling of REEs, which holds importance for both energy and the environment.</p>

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Optimization of lanthanum (III) recovery by HKUST-1-graphene oxide composite using response surface methodology and adsorption mechanism

  • Chaoke Bulin,
  • Chenna Li,
  • Ting Guo,
  • Jinxiao Bao,
  • Qingchun Wang,
  • Jinling Song,
  • Guoxiang Xin

摘要

Recovery of rare earth elements (REEs) from industrial runoff is a sustainable approach for resource recycling and environmental treatment. We report the one-pot fabrication of HKUST-1-graphene oxide (HKUST-1-GO) composite for the recovery of La(III), an indispensable component in hydrogen storage materials and fuel cells, from aqueous solutions. The as-fabricated HKUST-1-GO was intensively characterized using X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, Brunauer-Emmett-Teller (BET), Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. HKUST-1-GO was then used as an adsorbent to recover La(III), and the recovery efficacy was evaluated via batch adsorption and optimized through the use of response surface methodology (RSM). In addition, the adsorption mechanism was meticulously explored through both theoretical and experimental investigations. The derived results are summarized as follows: (1) HKUST-1-GO has a prominent BET specific surface area of 1522.8029 m2 g−1; (2) a recovery percentage of 95.54% for La(III) was achieved in 80 min, and the maximum Langmuir adsorption capacity reached 1090.24 mg g−1; (3) through applying RSM, the optimum La(III) recovery efficacy was found to be 97.133% through applying HKUST-1-GO at a dosage of 407.760 mg L−1, at pH 6.0, and with a contact time of 87.235 min; (4) statistical physics calculations determined that the adsorption process is exothermic and spontaneous, accompanied by an increase in entropy. Through isotherm and kinetic fittings, the adsorption was classified as favorable chemisorption controlled by surface reaction. Moreover, adsorbent speciation analysis and multifarious spectroscopic exploration showed the involvement of O–H, C=O, and C–O in La(III) uptake via electron donation to form La–O bonds, and electrostatic attraction was found to be involved in adsorption. Through this study, the recovery efficacy and mechanism of HKUST-1-GO toward La(III) were determined, and the results can be used as a constructive reference for tailoring MOF-based materials in the recycling of REEs, which holds importance for both energy and the environment.