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Principles Of Fluorescence Spectroscopy

Confining molecules can fundamentally change their chemical and physical properties. Confinement effects are considered instrumental at various stages of the origins of life, and life continues to rely on layers of compartmentalization to maintain an out-of-equilibrium state and efficiently synthesize complex biomolecules under mild conditions. As interest in synthetic confined systems grows, we are realizing that the principles governing reactivity under confinement are the same in abiological systems as they are in nature. In this Review, we categorize the ways in which nanoconfinement effects impact chemical reactivity in synthetic systems. Under nanoconfinement, chemical properties can be modulated to increase reaction rates, enhance selectivity and stabilize reactive species. Confinement effects also lead to changes in physical properties. The fluorescence of light emitters, the colours of dyes and electronic communication between electroactive species can all be tuned under confinement. Within each of these categories, we elucidate design principles and strategies that are widely applicable across a range of confined systems, specifically highlighting examples of different nanocompartments that influence reactivity in similar ways.

Chemical reactivity under nanoconfinement

A simple, instrument-free, paper-based analytical device with dual-emission carbon dots (CDs) (blue CDs and red CDs) was developed for the semiquantitative, visual, and sensitive speciation analysis of lead ions in a real sample with a sensitive detection limit of 2.89 nM. When a paper strip was immersed into the sample solution, the blue fluorescence was quenched by Pb2+ in solution, while the red fluorescence served as a background reference without color change, and significant color evolutions from blue to red were observed under the ultraviolet lamp, resulting in a semiquantitative visual detection. Furthermore, a smartphone was used in the visual detection of lead ions by identifying the RGB value of the fluorescent probe solution and corresponding paper strip. The application of smartphones and fluorescent paper strips has greatly shortened the detection time and reduced the cost of detection, providing a new strategy for the on-site and semiquantitative detection of heavy-metal ions in water samples.

Semiquantitative Visual Detection of Lead Ions with a Smartphone via a Colorimetric Paper-Based Analytical Device

Kosmotropic cosolvents added to an aqueous solution promote the aggregation of hydrophobic solute particles, while chaotropic cosolvents act to destabilise such aggregates. We discuss the mechanism for these phenomena within an adapted version of the two-state Muller-Lee-Graziano model for water, which provides a complete description of the ternary water/cosolvent/solute system for small solute particles. This model contains the dominant effect of a kosmotropic substance, which is to enhance the formation of water structure. The consequent preferential exclusion both of cosolvent molecules from the solvation shell of hydrophobic particles and of these particles from the solution leads to a stabilisation of aggregates. By contrast, chaotropic substances disrupt the formation of water structure, are themselves preferentially excluded from the solution, and thereby contribute to solvation of hydrophobic particles. We use Monte Carlo simulations to demonstrate at the molecular level the preferential exclusion or binding of cosolvent molecules in the solvation shell of hydrophobic particles, and the consequent enhancement or suppression of aggregate formation. We illustrate the influence of structure-changing cosolvents on effective hydrophobic interactions by modelling qualitatively the kosmotropic effect of sodium chloride and the chaotropic effect of urea.

https://arxiv.org/pdf/cond-mat/0305204.pdf

Kosmotropes and chaotropes: modelling preferential exclusion, binding and aggregate stability

Open framework materials (OFM) constitute a large and growing class of nanoporous crystalline structures that is attracting considerable attention for electronic device applications. This review summarizes the most recent reports concerning electronic devices enabled by either of the two primary categories of OFM, metal-organic frameworks (MOFs) and covalent-organic frameworks (COFs). Devices in which the OFM plays an active role (as opposed to acting only as a selective sorbent or filter) are the principal focus, with examples cited that include field-effect transistors, capacitors, memristors, and a wide variety of sensing architectures. As a brief tutorial, we also provide a concise summary of various methods of depositing or growing OFM on surfaces, as these are of crucial importance to the deployment of electronic OFM. Finally, we offer our perspective concerning future research directions, particularly regarding what in our view are the biggest challenges remaining to be addressed. On the basis of the literature discussed here, we conclude that OFM constitute a unique class of electronic materials with characteristics and advantages that are distinct from either conventional inorganic semiconductors or organic conductors. This suggests a bright future for these materials in applications such as edge computing, resistive switching, and mechanically flexible sensing and electronics.

Electronic Devices Using Open Framework Materials.

There is great need for stand-alone luminescence-based chemosensors that exemplify selectivity, sensitivity, and applicability and that overcome the challenges that arise from complex, real-world media. Discussed herein are recent developments toward these goals in the field of supramolecular luminescent chemosensors, including macrocycles, polymers, and nanomaterials. Specific focus is placed on the development of new macrocycle hosts since 2010, coupled with considerations of the underlying principles of supramolecular chemistry as well as analytes of interest and common luminophores. State-of-the-art developments in the fields of polymer and nanomaterial sensors are also examined, and some remaining unsolved challenges in the area of chemosensors are discussed.

/pdf/supramolecular-luminescent-sensors-1rs45r4um4.pdf

Supramolecular Luminescent Sensors

High concentrations of certain nutrients, including phosphate, are known to lead to undesired algal growth and low dissolved oxygen levels, creating deadly conditions for organisms in marine ecosystems. The rapid and robust detection of these nutrients using a colorimetric, paper-based system that can be applied on-site is of high interest to individuals monitoring marine environments and others affected by marine ecosystem health. Several techniques for detecting phosphate have been reported previously, yet these techniques often suffer from high detection limits, reagent instability, and the need of the user to handle toxic reagents. In order to develop improved phosphate detection methods, the commonly used molybdenum blue reagents were incorporated into a paper-based, colorimetric detection system. This system benefited from improved stabilization of the molybdenum blue reagent as well as minimal user contact with toxic reagents. The colorimetric readout from the paper-based devices was analyzed and quantified using RGB analyses (via ImageJ), and resulted in the detection of phosphate at detection limits between 1.3 and 2.8 ppm in various aqueous media, including real seawater.

/pdf/a-paper-based-device-for-ultrasensitive-colorimetric-2p1n2mv6lc.pdf

A Paper-Based Device for Ultrasensitive, Colorimetric Phosphate Detection in Seawater

The ability to bind and detect analytes with high levels of selectivity, sensitivity and broad applicability for a variety of analytes is an essential goal, with applications in public health and e...

A polycationic pillar[5]arene for the binding and removal of organic toxicants from aqueous media

Poly(ethyleneimine) (PEI)-based CO2 sorbents are a promising material class for use in CO2 capture applications, particularly direct air capture (DAC), due to their high amine content and CO2 capacities. The sorbent lifetime is a key uncertainty in the deployment of these materials in such applications, as they oxidize under conditions relevant to candidate DAC process cycles. Here, we utilize thermogravimetric analysis/differential scanning calorimetry/FTIR spectroscopy to characterize the nature, rate, and quantity of volatile species formed from the oxidation of PEI when supported on mesoporous Al2O3. We show that NH3, CO2, and H2O are primary volatile species formed from PEI oxidation and that their production rate matches the overall oxidation rate as measured via heat flow from a differential scanning calorimeter. We show that the total quantity of NH3 evolved is consistent with terminal primary amines being cleaved from the polymer chain and that approximately one hydrogen atom per PEI repeat unit reacts to form H2O during the reaction. Finally, metadynamics and quantum chemical simulations performed on a simplified system are used to highlight the likely importance of radicals in the elementary reactions that comprise the oxidation reaction set. The findings here represent the first characterization of the volatile products from the oxidation of PEI in CO2 sorbents and lead to a greater understanding of the mechanisms behind the oxidative degradation of these materials. 

Volatile Products of the Autoxidation of Poly(ethylenimine) in CO2 Sorbents

Covalent functionalization of cellulose with β-cyclodextrin by succinic acid-promoted cross-linking leads to a dual-function material that efficiently promotes proximity-induced energy transfer from polycyclic aromatic hydrocarbons (PAHs) to squaraine fluorophores with high quantum yields, and removes PAHs from aqueous solution through non-covalent binding. This material, which possesses a high functionalization density (0.17 μg/mm2 of cyclodextrin on cellulose), promotes energy transfer efficiencies as high as 58 % (for an anthracene donor in combination with a squaraine fluorophore acceptor), and leads to the removal of up to 91 % of a PAH (pyrene) from aqueous solution by mixing of the solution with the functionalized material. Overall, the high performance of this material in both proximity-induced energy transfer and the removal of PAHs from water means that such a method has significant potential impact in a variety of real-world environmental remediation scenarios.

Joan M. Racicot

Papers

Supramolecular Luminescent Sensors

A Paper-Based Device for Ultrasensitive, Colorimetric Phosphate Detection in Seawater

A polycationic pillar[5]arene for the binding and removal of organic toxicants from aqueous media

Volatile Products of the Autoxidation of Poly(ethylenimine) in CO2 Sorbents

Efficient Detection and Removal of Polycyclic Aromatic Hydrocarbons Using Cyclodextrin‐Modified Cellulose