In Situ Studies of the Adsorption Kinetics of 4-Nitrobenzenediazonium Salt on Gold

Jayasundara, Dilushan R.; Cullen, Ronan J.; Soldi, Laura; Colavita, Paula E.

doi:10.1021/la202862p

Cited by 19 publications

(28 citation statements)

References 69 publications

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“…This requires a systematic study that monitors adsorption and desorption behavior in situ and in real time. Quartz crystal microbalance (QCM) is one such method that measures change in mass in real time and in situ due to the adsorption and desorption of molecules from its surface in the form of a resonance frequency shift . This is given by the Sauerbrey equation. where f 0 is the resonance frequency of the uncoated QCM in air, A is the effective surface area of the electrodes, ρ and μ are the density and shear modulus of quartz, respectively …”

Section: Introductionmentioning

confidence: 99%

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Mechanistic Insights into Interactions at Urea–Hydroxyapatite Nanoparticle Interface

et al. 2021

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Development of controlled release biomolecules by surface modification of hydroxyapatite nanoparticles has recently gained popularity in the areas of bionanotechnology and nanomedicine. However, optimization of these biomolecules for applications such as drug delivery, nutrient delivery requires a systematic understanding of binding mechanisms and interfacial kinetics at the molecular level between the nanomatrix and the active compound. In this research, urea is used as a model molecule to investigate its interactions with two morphologically different thin films of hydroxyapatite nanoparticles. These thin films were fabricated on quartz crystal piezoelectric sensors to selectively expose Ca 2+ and PO 4 3− sites of hydroxyapatite. Respective urea adsorption and desorption on both of these sites were monitored in situ and in real time in the phosphate buffer solution that mimics body fluids. The measured kinetic parameters, which corroborate structural predisposition for controlled release, show desorption rates that are one-tenth of the adsorption rates on both surfaces. Furthermore, the rate of desorption from the PO 4 3− site is one-half the rate of desorption from the Ca 2+ site. The Hill kinetic model was found to satisfactorily fit data, which explains cooperative binding between the hydroxyapatite nanoparticle thin film and urea. Fourier transform infrared spectra and X-ray photoemission spectra of the urea adsorbed on the above surfaces confirm the cooperative binding. It also elucidates the different binding mechanisms between urea and hydroxyapatite that contribute to the changes in the interfacial kinetics. These findings provide valuable information for structurally optimizing hydroxyapatite nanoparticle surfaces to control interfacial kinetics for applications in bionanotechnology and nanomedicine.

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Section: Introductionmentioning

confidence: 99%

“…Quartz crystal microbalance (QCM) is one such method that measures change in mass in real time and in situ due to the adsorption and desorption of molecules from its surface in the form of a resonance frequency shift. 28 This is given by the Sauerbrey equation.…”

Section: ■ Introductionmentioning

confidence: 99%

Mechanistic Insights into Interactions at Urea–Hydroxyapatite Nanoparticle Interface

et al. 2021

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“…40 This cationinduced reaction is generally referred as a spontaneous grafting and may lead to the formation of monolayer at the surface of the substrate. 39,41 In the radical process, plasmon-induced electron transfers from the gold structures to the diazonium cation yield the formation of aryl radicals that in turn react with the surface to form an aryl molecular layer. Other radicals react with the first layer to form a thin polymer film which thickness varies with the irradiation conditions and local field enhancements.…”

Section: Resultsmentioning

confidence: 99%

Three-color plasmon-mediated reduction of diazonium salts over metasurfaces

et al. 2021

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“…The total change in resonant frequency Δ f for a crystal immersed in a liquid medium can result from multiple contributions so that

[ 63 , 64 , 65 ], where

is the frequency shift resulting from a mass increase at the crystal surface,

is the shift arising from viscous damping,

results from surface stress, and

is due to non-shear coupling.

and

are typically time-independent and therefore should not be responsible for the change observed over the 5 day incubations.…”

Section: Resultsmentioning

confidence: 99%

Controlling the Carbon-Bio Interface via Glycan Functional Adlayers for Applications in Microbial Fuel Cell Bioanodes

et al. 2021

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Surface modification of electrodes with glycans was investigated as a strategy for modulating the development of electrocatalytic biofilms for microbial fuel cell applications. Covalent attachment of phenyl-mannoside and phenyl-lactoside adlayers on graphite rod electrodes was achieved via electrochemically assisted grafting of aryldiazonium cations from solution. To test the effects of the specific bio-functionalities, modified and unmodified graphite rods were used as anodes in two-chamber microbial fuel cell devices. Devices were set up with wastewater as inoculum and acetate as nutrient and their performance, in terms of output potential (open circuit and 1 kΩ load) and peak power output, was monitored over two months. The presence of glycans was found to lead to significant differences in startup times and peak power outputs. Lactosides were found to inhibit the development of biofilms when compared to bare graphite. Mannosides were found, instead, to promote exoelectrogenic biofilm adhesion and anode colonization, a finding that is supported by quartz crystal microbalance experiments in inoculum media. These differences were observed despite both adlayers possessing thickness in the nm range and similar hydrophilic character. This suggests that specific glycan-mediated bioaffinity interactions can be leveraged to direct the development of biotic electrocatalysts in bioelectrochemical systems and microbial fuel cell devices.

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In Situ Studies of the Adsorption Kinetics of 4-Nitrobenzenediazonium Salt on Gold

Cited by 19 publications

References 69 publications

Mechanistic Insights into Interactions at Urea–Hydroxyapatite Nanoparticle Interface

Mechanistic Insights into Interactions at Urea–Hydroxyapatite Nanoparticle Interface

Three-color plasmon-mediated reduction of diazonium salts over metasurfaces

Controlling the Carbon-Bio Interface via Glycan Functional Adlayers for Applications in Microbial Fuel Cell Bioanodes

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