Effective and selective adsorption of organoarsenic acids from water over a Zr-based metal-organic framework

Lin, Zhiping; Zheng, He‐Qi; Zeng, Yongnian; Wang, Yulin; Chen, Jin; Cao, Gaoping; Gu, Jia‐Fang; Chen, Banglin

doi:10.1016/j.cej.2019.122196

Cited by 94 publications

(34 citation statements)

References 45 publications

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“…Preparation of Zr-BTC-H Catalysts. Zr-BTC (also known as MOF-808) based on Zr 6 (μ 3 -O 4 )(μ 3 -OH) 4 (HCO 2 ) 6 nodes and 1,3,5-benzenetricarboxylic acid (H 3 BTC) bridging ligands (denoted Zr-BTC) was synthesized following a reported method with a few modi cations (See in Methods, Supplementary Figure 1) [40][41][42] . The formate capping groups on Zr-BTC were removed by hydrochloric acid treatment, followed by activation with HBpin to afford the Zr-H active sites.…”

Section: Full Textmentioning

confidence: 99%

A noble-metal-free metal-organic framework for alkane borylation

Zeng

Cao

et al. 2022

Preprint

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Catalytic borylation of unactivated C(sp3)‒H bond is of great interest but quite challenging. Reported catalysts mostly contain noble metals such as iridium and ruthenium. Here, we report an earth-abundant zirconium-based metal-organic framework (MOF) catalyst with zirconium hydride (Zr‒H) active sites for methane borylation. Isotope exchange experiment and spectroscopic evidence confirm methane activation by Zr‒H active sites to generate Zr‒CH3 and H2, possibly via σ-bond metathesis. Theoretical calculations suggest another σ-bond metathesis step for C‒B bond formation. The MOF catalyst selectively borylates end methyl group in alkanes and other compounds. For example, the MOF catalyst mono-borylated the end methyl group of n-pentane in 87% yield with > 98% selectivity. The selectivity of primary C‒H bond over secondary C‒H bond is attributed to the steric effect around the Zr‒H site in the MOF, as Zr‒H sites on supports with less stringent steric control have poorer selectivity. This work provides new insights into developing catalysts for alkane functionalization.

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Section: Full Textmentioning

confidence: 99%

A noble-metal-free metal-organic framework for alkane borylation

Zeng

Cao

et al. 2022

Preprint

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“…Therefore, the feature of enthalpically governed adsorption reactions can be exploited to regenerate the material by thermal treatment and/or supporting other recovery treatments. In contrast, ferric hydroxide and zirconium-based metal-organic framework are adsorbents with entropically and enthalpic-entropically governed adsorption reactions, respectively [69,70].…”

Section: Adsorption Free Energiesmentioning

confidence: 99%

Removal of Water-Soluble Inorganic Arsenicals with Phosphorene Oxide Nanoadsorbents: A First-Principles Study

Cortés‐Arriagada

Wrighton-Araneda²

2021

Preprint

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A complete picture of the phosphorene oxide (PhosO) sorption properties for the simultaneous removal of inorganic As(III) and As(V) pollutants from water has been developed using first-principles calculations. Calculated adsorption energies, competitive adsorption with co-existing species, energy decomposition analyses (ALMO-EDA), implicitly/explicitly solvated geometries, and adsorption free energies provide deep insights into the adsorption mechanism as well as the origin of the strong selectivity sorption ability. The PhosO nanoadsorbents establish inner-sphere surface complexes with arsenicals even under competition with water molecules. These proposed structures also show a strong affinity with the highly mobile As(III), where energy saving is achieved by avoiding the pre oxidation process to convert As(III) into As(V) as requested in related materials. Results show that electrostatic driving forces govern the adsorption of neutral arsenicals, while the interplay between electrostatic and polarization phenomena drives the uptake of anionic arsenicals. By computing the adsorption strength as a function of the oxidation degree, the optimum adsorption efficiency is reached with a 25% in the content of oxidizing groups. In this oxidation degree, the strong repulsive surface charge at high pH turns the PhosO nanoadsorbents convenient to recycle via simple treatment with alkaline eluents. Finally, the adsorption ability remains thermodynamically allowed in a wide range of ambient temperatures (enthalpically governed reaction). Conceptually understanding the sorption properties of phosphorene-oxide-based materials towards arsenic pollutants provides a useful framework for future water treatment technologies.<br>

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“…In this regards, Zr-based metal organic frameworks (Zr-MOFs) are one of the best MOFs because of their excellent thermal, mechanical, and chemical stability [ 24 , 25 ]. Since they contain a structure which has water-tolerant across a wide range of pHs, they can be used in many applications which need to be performed in both acidic and basic media [ 26 ]. MOF-808 is a type of Zr-MOF that is assembled from Zr 6 (µ 3 -O)4(µ 3 -OH) 4 nodes connected to both six 1,3,5-benzenetricarboxylate (BTC 3− ) linkers and charge-balancing formate ligands.…”

Section: Introductionmentioning

confidence: 99%

Synthesis, characterization and application of a zirconium-based MOF-808 functionalized with isonicotinic acid for fast and efficient solid phase extraction of uranium(VI) from wastewater prior to its spectrophotometric determination

et al. 2022

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Background A zirconium-based metal-organic framework (Zr-MOF), named MOF-808, was synthesized and fully characterized by solvo-thermal method and functionalized by isonicotinic acid and employed as an efficient adsorbent for selective extraction and preconcentration of uranyl ions from water and waste water samples in a batch solid phase extraction. Results Parameters affecting extraction such as volume and pH of the sample solution, the amount of sorbent, type and volume of eluting solvent, and adsorption and desorption times were investigated and optimized. Under the optimized conditions, high extraction efficiency was observed with a limit of detection of 0.9 µg L− 1 for uranyl ions and relative standard deviations were found to be better than 2.1% in the range of 0.07–1000 µg L− 1. Conclusions These results indicated that the above procedure is fast, inexpensive, effective, reliable, applicable and organic solvent-free and showed the highly performance and stability of the Zr-MOF in SPE based analytical techniques.

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Effective and selective adsorption of organoarsenic acids from water over a Zr-based metal-organic framework

Cited by 94 publications

References 45 publications

A noble-metal-free metal-organic framework for alkane borylation

A noble-metal-free metal-organic framework for alkane borylation

Removal of Water-Soluble Inorganic Arsenicals with Phosphorene Oxide Nanoadsorbents: A First-Principles Study

Synthesis, characterization and application of a zirconium-based MOF-808 functionalized with isonicotinic acid for fast and efficient solid phase extraction of uranium(VI) from wastewater prior to its spectrophotometric determination

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