Stepwise assembly of heterometallic, heteroleptic “triblock Janus-type” metal–organic polyhedra

von, Baeckmann Cornelia; Ruiz-Relaño, Sara; Imaz, Inhar; Handke, Marcel; Juanhuix, Judith; Gándara, Felipe; Carné‐Sánchez, Arnau; Maspoch, Daniel

doi:10.1039/d2cc06815j

Cited by 7 publications

(7 citation statements)

References 34 publications

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“…1 ). The starting point was the Rh 2 (bdc) 4 cluster, which has four available carboxylic acid groups, 45 which were used to attach, via amide coupling, four alkyne-terminated NH 2 -PEG 6 -alkyne chains (Fig. S42–S45 † ).…”

Section: Resultsmentioning

confidence: 99%

Giant oligomeric porous cage-based molecules

Cortés-Martínez,

von Baeckmann,

Hernández-López

et al. 2024

Chem. Sci.

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Section: Resultsmentioning

confidence: 99%

Giant oligomeric porous cage-based molecules

Cortés-Martínez,

von Baeckmann,

Hernández-López

et al. 2024

Chem. Sci.

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“…To answer this question, we functionalized the sensing area of the BiMW with a discrete Rh(II)-based paddlewheel cluster with formula Rh 2 (bdc) 4 ( Figure S11 ). 28 This metal–organic complex replicates a metal–organic fragment present in the MOP structure and presents four available, un-coordinated COOH groups, which makes it an ideal model compound to assess the impact of structuring Rh(II) sites on the analytical response of BiMW sensors. The sensitivity of the Rh 2 (bdc) 4 -BiMW sensor toward BTA was significantly lower than that obtained for the MOP-BiMW sensor under otherwise identical conditions ( Figure S12 ).…”

Section: Resultsmentioning

confidence: 99%

Integration of Metal–Organic Polyhedra onto a Nanophotonic Sensor for Real-Time Detection of Nitrogenous Organic Pollutants in Water

Calvo-Lozano,

Hernández-López,

Gomez

et al. 2023

ACS Appl. Mater. Interfaces

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The grave health and environmental consequences of water pollution demand new tools, including new sensing technologies, for the immediate detection of contaminants in situ. Herein, we report the integration of metal−organic cages or polyhedra (MOCs/MOPs) within a nanophotonic sensor for the rapid, direct, and realtime detection of small (<500 Da) pollutant molecules in water. The sensor, a bimodal waveguide silicon interferometer incorporating Rh(II)-based MOPs as specific chemical receptors, does not require sample pretreatment and enables minimal expenditure of time and reagents. We validated our sensor for the detection of two common pollutants: the industrial corrosion inhibitor 1,2,3-benzotriazole (BTA) and the systemic insecticide imidacloprid (IMD). The sensor offers a fast time-to-result response (15 min), high sensitivity, and high accuracy. The limit of detection (LOD) in tap water for BTA is 0.068 μg/mL and for IMD, 0.107 μg/mL, both of which are below the corresponding toxicity thresholds defined by the European Chemicals Agency (ECHA). By combining innovative chemical molecular receptors such as MOPs with state-of-the-art photonic sensing technologies, our research opens the path to implement competitive sensor devices for in situ environmental monitoring.

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“…The quasi‐static nature of MOPs at ambient temperatures imparts a strong thermosetting character to MOP‐crosslinked networks, while higher temperatures (e.g., exceeding 120 °C) activate the dynamic behavior of MOPs, facilitating rapid ligand exchange and conferring facile processability akin to thermoplastics [12a] . The reversible dynamics of MOPs provides a desirable strategy for the precise synthesis of MSPs with tunable compositions [13] . Herein, 24‐arm star homo‐polymers (Scheme 1b) from six different types of polymers, respectively, are firstly prepared using MOPs as templates.…”

Section: Methodsmentioning

confidence: 99%

“…[12a] The reversible dynamics of MOPs provides a desirable strategy for the precise synthesis of MSPs with tunable compositions. [13] Herein, 24-arm star homo-polymers (Scheme 1b) from six different types of polymers, respectively, are firstly prepared using MOPs as templates. The homopolymers can be mixed in solutions and thermal-annealed for the synthesis of 24-arm MSPs, whose compositions can be facilely and precisely tuned via the recipe of the inputted star polymer mixtures.…”

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confidence: 99%

Modulating Ligand‐Exchange Dynamics on Metal‐Organic Polyhedra for Reversible Sorting and Hybridization of Miktoarm Star Polymers

Lai,

He,

Xue

et al. 2023

Angew Chem Int Ed

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The precise synthesis of miktoarm star polymers (MSPs) remains one of the great challenges in synthetic chemistry due to the difficulty in locating appropriate structural templates and polymer grafting/growing strategies with high selectivity and efficiency. Herein, ~ 2 nm metal‐organic polyhedra (MOPs), constructed from the coordination of isophthalic acid (IPA) and Cu2+, are applied as templates for the precise synthesis of 24‐arm MSPs for their unique logarithmic ligand exchange dynamics. Six different polymers are prepared with IPA as an end group and they further coordinated with Cu2+ to afford corresponding 24‐arm star homo‐polymers, respectively. MSPs can be obtained by mixing targeted homo‐arm star polymers in solutions upon thermal annealing. The compositions of MSPs can be facilely and precisely tuned via the recipe of the inputted star polymer mixtures. Interestingly, the obtained MSPs can be sorted into homo‐arm star polymers through a typical solvent extraction protocol. The hybridization and sorting process can be reversibly conducted via the cycle of thermal annealing and solvent treatment. The complex coordination framework not only opens new avenues for the facile and precise synthesis of MSPs and MOPs with hybrid functionalities, but also provides the capability to design sustainable polymer systems.

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Stepwise assembly of heterometallic, heteroleptic “triblock Janus-type” metal–organic polyhedra

Abstract: Increasing the chemical complexity of metal-organic cages (MOCs) or polyhedra (MOPs) demands control over the simultaneous organization of diverse organic linkers and metal ions into discrete caged structures. Herein, we...

Cited by 7 publications

References 34 publications

Giant oligomeric porous cage-based molecules

Giant oligomeric porous cage-based molecules

Integration of Metal–Organic Polyhedra onto a Nanophotonic Sensor for Real-Time Detection of Nitrogenous Organic Pollutants in Water

Modulating Ligand‐Exchange Dynamics on Metal‐Organic Polyhedra for Reversible Sorting and Hybridization of Miktoarm Star Polymers

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