Molecular-level understanding of highly selective heavy rare earth element uptake by organophosphorus modified MIL-101(Cr)

Keshavarz, Fatemeh; Kavun, Vitalii; Veen, Monique A. van der; Repo, Eveliina; Barbiellini, B.

doi:10.1016/j.cej.2022.135905

Cited by 15 publications

(3 citation statements)

References 75 publications

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“…Replacing HF with mineral acids that penetrate tissues less readily [16] is an alternative. MIL-101(Cr) syntheses using hydrochloric acid (HCl), [17,55,[57][58][59][60][61][62][63][64][65][66][67] nitric acid (HNO 3 ), [12,18,31,[68][69][70][71][72][73][74][75][76][77][78][79][80][81][82][83][84][85][86][87] and even sulfuric acid (H 2 SO 4 ) [12] as mineralizers have been reported. [11] Although HCl is a stronger acid than HNO 3 , H 2 SO 4 , and HF (Table 3), MIL-101(Cr) synthesized using HCl (denoted HCl-MIL-101(Cr)) in molar ratios such as 1 Cr:1 H 2 BDC:1 HCl:266 H 2 O remains highly crystalline.…”

Section: Mineral Acidsmentioning

confidence: 99%

Elucidating Improvements to MIL‐101(Cr)’s Porosity and Particle Size Distributions based on Innovations and Fine‐Tuning in Synthesis Procedures

Wee

Chinnappan

Ramakrishna

2023

Adv Materials Inter

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Among the existing metal–organic frameworks (MOFs), MIL‐101(Cr) is renowned for its stability in air and water. As a result, MIL‐101(Cr) has numerous potential applications ranging from adsorptive cooling to catalysis. The industrial‐scale production of MIL‐101(Cr) is necessary before realizing these applications. Yet, there remain two main bottlenecks in preparing MIL‐101(Cr) in bulk: the toxicity of hydrofluoric acid (HF) used in conventional MIL‐101(Cr) synthesis and the challenge of ensuring that the as‐prepared MIL‐101(Cr) is highly porous with specific Brunauer–Emmett–Teller surface area (SBET) above 4000 m2 g−1. On the laboratory scale, MIL‐101(Cr) often presents SBET 2300–3500 m2 g−1. The synthesis and purification procedures often influence the yield, particle size, porosity, and other properties of MIL‐101(Cr). This critical review examines trends in MIL‐101(Cr) preparation procedures and the MOF's resulting properties to elucidate areas for improvement toward its real‐world applications. The purification processes for conventional HF‐based MIL‐101(Cr) whereby porosities vary despite the same synthesis approach are first investigated. Next, the reported additives for substituting HF and their influence on the resulting MIL‐101(Cr)’s porosity and particle size are discussed. The selection of additives may be application‐specific: exemplified in the examination of MIL‐101(Cr)’s preparation, its corresponding water sorption capacity, and desiccant‐related applications.

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Section: Mineral Acidsmentioning

confidence: 99%

Elucidating Improvements to MIL‐101(Cr)’s Porosity and Particle Size Distributions based on Innovations and Fine‐Tuning in Synthesis Procedures

Wee

Chinnappan

Ramakrishna

2023

Adv Materials Inter

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“…Metal–organic frameworks (MOFs) have attracted considerable attention as potential adsorbents for heavy metal removal due to their high surface area, tunable pore size, and diverse functionality. − In recent years, numerous MOFs have been synthesized and investigated for heavy metal removal, such as UIO-66, MIL-101, − BUT-52, and ZIF-8 . The UIO-66 is a well-known example of a Zr-based MOF with excellent water and thermal stability composed of cationic Zr 6 O 4 (OH) 4 nodes and 1,4-benzenedicarboxylate (BDC) organic linkers. − Such features make the UIO-66 series of MOF materials have the potential to serve as excellent adsorbents for metal ions.…”

Section: Introductionmentioning

confidence: 99%

Enhanced Breathing Effect of Nanoporous UIO-66-DABA Metal–Organic Frameworks with Coordination Defects for High Selectivity and Rapid Adsorption of Hg(II)

Zhao,

Yang,

Zhang

et al. 2023

ACS Appl. Nano Mater.

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Herein, the diamino-functionalized UIO-66-DABA is constructed by introducing coordination defects of 3,5-diaminobenzoic acid (DABA) as the metal–organic framework (MOF) linkers, which are systematically characterized by scanning electron microscopy, 1H nuclear magnetic resonance, and Brunauer–Emmett–Teller analysis. The powder X-ray diffraction and thermogravimetric analysis results show that it exhibits excellent thermal stability and acid stability. Importantly, the adsorption experiments show that UIO-66-DABA has high selectivity and excellent adsorption performance (713 mg/g) for Hg2+. The adsorption data, including isotherms and kinetics, are well-matched with both Langmuir and pseudo-second-order models. Thermodynamic analysis reveals that the adsorption process is spontaneous, disordered, and exothermic. It is observed that the adsorption of a low concentrations of Hg2+ (20 μg/L) can reach drinking standards within 8 h. The recyclable usage of UIO-66-DABA for the removal of Hg2+ makes it potentially useful for industrial applications. Furthermore, the density functional theory results and molecule dynamics simulations further explore the interactions and conformational relationships between Hg2+ and MOFs (UIO-66, UIO-66-(NH2)2, and UIO-66-DABA). Among these, the lone electron pair on the amino nitrogen plays the key role in the selective adsorption for Hg2+. Additionally, the DABA ligand’s large vibrational amplitudes induce an increased breathing effect within the MOF structure, thereby facilitating the rapid entry of Hg2+ into the pores. As such, our work provides a novel strategy that can regulate the adsorption selectivity and adsorption efficiency of heavy metal ions by MOFs via introducing coordination defects.

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“…Because the oxidation potential of Au(III) is much higher than that of Cu, Ni, Fe, Zn, and other metal ions, the reduction-capable groups can be introduced into the MOF structure for efficient adsorption of Au(III). At present, there are many chromium-based MOF materials used for adsorption separation in aqueous solution because of their excellent water stability. − The excellent acid stability of Cr-MOFs is mainly due to the high charge/radius ratio of Cr 3+ and its d 3 configuration, which maximizes the ligand field stability . In this work, a novel Cr-based MOF with 1,2,4-triazole and 4-aminobenzoic acid as ligands was synthesized via a one-step process for Au adsorption.…”

Section: Introductionmentioning

confidence: 99%

Cr-Based MOF for Efficient Adsorption of Au at Low Concentrations

Tang

2022

Langmuir

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The efficient enrichment and selection of Au are crucial for gold recovery. The adsorption technology is considered to have potential due to the advantages of operation simplicity and green processability. Nevertheless, the poor Au selectivity at low concentrations in complex solutions limits the further application of the adsorption technology. In this work, a novel Cr-based MOF adsorbent was successfully synthesized using 1,2,4-triazole and 4-aminobenzoic acid as ligands. Benefitting from the surface positive charge and extensive chelation and reduction sites, the novel Cr-based MOF exhibited a total adsorption capacity of up to 357 mg/g and excellent adsorption selectivity toward Au(III) in the complex metal mixed solutions, such as simulated sewage ash waste liquid and actual e-waste leachate. Furthermore, the adsorption kinetics, isotherms, and thermodynamics were discussed in depth for investigating the adsorption mechanisms of the MOF. The PXRD and XPS analyses reveal that the adsorption process involves complexation, redox, and electrostatic interactions. We believe that this study of novel Cr-based MOF adsorbents for efficient Au adsorption is meaningful for further application in the gold recovery technology from e-waste.

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Molecular-level understanding of highly selective heavy rare earth element uptake by organophosphorus modified MIL-101(Cr)

Cited by 15 publications

References 75 publications

Elucidating Improvements to MIL‐101(Cr)’s Porosity and Particle Size Distributions based on Innovations and Fine‐Tuning in Synthesis Procedures

Elucidating Improvements to MIL‐101(Cr)’s Porosity and Particle Size Distributions based on Innovations and Fine‐Tuning in Synthesis Procedures

Enhanced Breathing Effect of Nanoporous UIO-66-DABA Metal–Organic Frameworks with Coordination Defects for High Selectivity and Rapid Adsorption of Hg(II)

Cr-Based MOF for Efficient Adsorption of Au at Low Concentrations

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