4.7 Article

Exceptionally amino-quantitated 3D MOF@CNT-sponge hybrid for efficient and selective recovery of Au(III) and Pd(II)

期刊

CHEMICAL ENGINEERING JOURNAL
卷 431, 期 -, 页码 -

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ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.133367

关键词

Hybrid MOF; CNT sponge; Amino groups; Precious metals; Selectivity and recovery

资金

  1. National Natural Science Foundation of China [41977329]
  2. Natural Science Foundation of Guangdong Province [2021B1515020041]
  3. Special Funds for the Cultivation of Guangdong College Students' Scientific and Technological Innovation [pdjh2019c471]

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Designing materials for selective recovery of precious metals is critical in response to the economic and environmental concerns caused by electronic waste outbreaks. In this study, high-performance hybrid materials (MCNTs) based on hexaaminobenzene metal-organic framework (HAB-MOF) and carbon nano-tube (CNT) sponge were introduced for selective recovery of Au(III) and Pd(II). The synthesized 30-MCNT demonstrated the highest adsorption capacity for Au(III) and Pd(II) among all reported MOFs, making it a benchmark material in the MOF family. The material showed high selectivity and excellent recovery and recycling properties, making it a potential candidate for industrial applications in precious metal recovery.
Designing materials for selective recovery of precious metals is a critical challenge in response to recent outbreaks of electronic wastes owing to economic and environmental concerns. We introduced high-performance hybrid materials (MCNTs) comprising of six-amino groups based on hexaaminobenzene metal-organic framework (HAB-MOF) and carbon nano-tube (CNT) sponge for selective recovery of Au(III) and Pd(II). Among all MOFs ever reported in the literature, the particular synthesized 30-MCNT (30 mg HAB-MOF on CNT sponge) exhibited the highest adsorption capacity (q(e)) of 1832 mg/g (45 C, pH 3.0) for Au(III) and 1651 mg/g (45 C, pH 1.0) for Pd(II), which can be regarded as a benchmark in the MOF family. The highly selective nature of 30-MCNT was examined in the presence of ten different metal ions and the results showed that the Au(III)/Pd(II) adsorption efficiency was decreased by only 5-10%. Moreover, the Au(III) and Pd(II) recovery was maintained ~ 100% from the initial solution with metal concentration of 200 mg/L. The superior performance was mainly attributed to the role of abundant amino groups in the hybrid framework, developing several types of interactions with Au(III) and Pd(II) ions such as hydrogen bonding, electrostatic interactions, acid-base affinity and 7C-7C inner sphere complexation. Furthermore, the remarkably high surface area and robust chemical and mechanical stability of CNT-sponge provided an exceptional support for impregnation of HAB-MOF to avail greater active sites and easier handpicked recycle. Density functional theory (DFT) simulation and X-ray photoelectron spectroscopy (XPS) studies were employed to explore the interaction mechanisms during the adsorption processes. Owing to facile and environment-friendly synthesis, excellent recovery and recycling, the material can be possibly considered for industrial application in precious metal recovery.

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