Publications by authors named "Jacob McKenzie"

2D materials can be isolated as monolayer sheets when interlayer interactions involve weak van der Waals forces. These atomically thin structures enable novel topological physics and open chemical questions of how to tune the structure and properties of the sheets while maintaining them as isolated monolayers. Here, this work investigates 2D electroactive sheets that exfoliate in solution into colloidal nanosheets, but aggregate upon oxidation, giving rise to tunable interlayer charge transfer absorption and photoluminescence.

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Article Synopsis
  • Anion sensing technology is essential for understanding biological systems and environmental interactions, yet traditional electrochemical methods are limited in distinguishing various anions in mixtures.
  • This study introduces a novel approach using nanocrystalline films of the metal-organic framework (MOF) Cr(1,2,3-triazolate) to differentiate anions based on their size, which influences the reversible oxidation process of the MOF.
  • The research demonstrates the effectiveness of this method by creating a highly sensitive and recyclable electrochemical sensor for ClO in water that can detect concentrations as low as 100 nM, showcasing the potential of MOFs for advanced anion sensing applications.
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Redox intercalation involves coupled ion-electron motion within host materials, finding extensive application in energy storage, electrocatalysis, sensing, and optoelectronics. Monodisperse MOF nanocrystals, compared to their bulk phases, exhibit accelerated mass transport kinetics that promote redox intercalation inside nanoconfined pores. However, nanosizing MOFs significantly increases their external surface-to-volume ratios, making the intercalation redox chemistry into MOF nanocrystals difficult to understand due to the challenge of differentiating redox sites at the exterior of MOF particles from the internal nanoconfined pores.

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Interactions between ions and itinerant charges govern electronic processes ranging from the redox chemistry of molecules to the conductivity of organic semiconductors, but remain an open frontier in the study of microporous materials. These interactions may strongly influence the electronic behavior of microporous materials that confine ions and charges to length scales comparable to proton-coupled electron transfer. Yet despite mounting evidence that both solvent and electrolyte influence charge transport through ion-charge interactions in metal-organic frameworks, fundamental microscopic insights are only just beginning to emerge.

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