Despite extensive advances in the field of molecular recognition, the real-time monitoring of small molecule binding to nanoparticles (NP) remains a challenge. To this end, we report on a versatile approach, based on quartz crystal microbalance with dissipation monitoring, for the stepwise in situ quantification of gold nanoparticle (AuNPs) immobilisation and subsequent uptake and release of binding partners. AuNPs stabilised by thiol-bound ligand shells of prescribed chemical composition were densely immobilised onto gold surfaces via dithiol linkers. The boronate ester formation between salicylic acid derivatives in solution and boronic acids in the AuNP ligand shell was then studied in real time, revealing a drastic effect of both ligand architecture and Lewis base concentration on the interaction strength. The binding kinetics were analysed with frequency response modelling for a thorough comparison of binding parameters including relaxation time as well as association rate constant. The results directly mirror those from previously reported in-depth studies using nuclear magnetic resonance spectroscopy. By achieving quantitative characterisation of selective binding of analytes with molecular weight below 300 Da, this new method enables rapid, low cost, rational screening of AuNP candidates for molecular recognition. † Electronic supplementary information (ESI) available: Experimental details on synthetic procedures, sample preparation and characterisation techniques; further results on QCM-D characterisation. See
In spite of widespread interest in the unique size-dependent properties and consequent applications of gold nanoparticles (AuNPs), synthetic protocols that reliably allow for independent tuning of surface chemistry and core size, the two critical determinants of AuNP properties, remain limited. Often, core size is inherently affected by the ligand structure in an unpredictable fashion. Functionalized ligands are commonly introduced using postsynthesis exchange procedures, which can be inefficient and operationally delicate. Here, we report a one-step protocol for preparing monolayer-stabilized AuNPs that is compatible with a wide range of ligand functional groups and also allows for the systematic control of core size. In a single-phase reaction using the mild reducing agent tert-butylamine borane, AuNPs that are compatible with solvents spanning a wide range of polarities from toluene to water can be produced without damaging reactive chemical functionalities within the small-molecule surface-stabilizing ligands. We demonstrate that the rate of reduction, which is easily controlled by adjusting the period over which the reducing agent is added, is a simple parameter that can be used irrespective of the ligand structure to adjust the core size of AuNPs without broadening the size distribution. Core sizes in the range of 2–10 nm can thus be generated. The upper size limit appears to be determined by the nature of each specific ligand/solvent pairing. This protocol produces high quality, functionally sophisticated nanoparticles in a single step. By combining the ability to vary size-related nanoparticle properties with the option to incorporate reactive functional groups at the nanoparticle–solvent interface, it is possible to generate chemically reactive colloidal building blocks from which more complex nanoparticle-based devices and materials may subsequently be constructed.
The annual global fish production reached a record 178 million tonnes in 2020, which continues to increase. Today, 49% of the total fish is harvested from aquaculture, which is forecasted to reach 60% of the total fish produced by 2030. Considering that the wastes of fishing industries represent up to 75% of the whole organisms, the fish industry is generating a large amount of waste which is being neglected in most parts of the world. This negligence can be traced to the ridicule of the value of this resource as well as the many difficulties related to its valorisation. In addition, the massive expansion of the aquaculture industry is generating significant environmental consequences, including chemical and biological pollution, disease outbreaks that increase the fish mortality rate, unsustainable feeds, competition for coastal space, and an increase in the macroalgal blooms due to anthropogenic stressors, leading to a negative socio-economic and environmental impact. The establishment of integrated multi-trophic aquaculture (IMTA) has received increasing attention due to the environmental benefits of using waste products and transforming them into valuable products. There is a need to integrate and implement new technologies able to valorise the waste generated from the fish and aquaculture industry making the aquaculture sector and the fish industry more sustainable through the development of a circular economy scheme. This review wants to provide an overview of several approaches to valorise marine waste (e.g., dead fish, algae waste from marine and aquaculture, fish waste), by their transformation into biofuels (biomethane, biohydrogen, biodiesel, green diesel, bioethanol, or biomethanol) and recovering biomolecules such as proteins (collagen, fish hydrolysate protein), polysaccharides (chitosan, chitin, carrageenan, ulvan, alginate, fucoidan, and laminarin) and biosurfactants.
Switchable selectivity within a series of boronate esters for dynamic covalent exchange in nonaqueous solvents The reversible condensation-hydrolysis reactions of boronic acids have proven to be a highly useful class of thermodynamically controlled dynamic covalent process, enabling the construction of sugar sensors, stimuli-responsive materials, and complex covalent architectures. Yet, the common diol or diphenol coupling partners tend to produce relatively unstable condensation products, exhibit oxidative sensitivity, or offer limited options for expanding structural diversity. To address these drawbacks, we explore a series of coupling partners including non-diol salicylate and salicylamide derivatives, in combination with two boronic acids. In nonaqueous solvents, the condensation-hydrolysis equilibria are sensitive to the nature and concentration of Lewis bases, with equilibrium constants that can be tuned across at least five orders of magnitude. Furthermore, differential responses to base concentration can be exploited to create a switchable dynamic covalent system in which a boronic acid can be cycled between expressing each of two condensation products with high fidelity, in response to a simple chemical stimulus.
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