Manipulating chemistry through nanoparticle morphology

Litti, Lucio; Reguera, Javier; Abajo, F. Javier García de; Meneghetti, Moreno; Liz‐Marzán, Luis M.

doi:10.1039/c9nh00456d

Cited by 34 publications

(39 citation statements)

References 58 publications

(77 reference statements)

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“…[19][20][21] The suitability of plasmonic nanomaterials to tune enzyme activity arises from their tunable localized surface plasmon resonances (LSPR), in the UV-Vis and nearinfrared wavelength ranges. [22][23][24] Under incident light, conduction electrons in metal nanoparticles display coherent collective oscillations, thereby generating intense absorption and scattering at specific wavelengths, resulting in LSPR signals. 25,26 It is well-known that the LSPR response is largely dictated by the dimensions and morphology of the plasmonic nanoparticles, but it is also highly sensitive to the interaction between biomolecules and the nanoparticles' surface.…”

Section: Toc Graphicmentioning

confidence: 99%

“…The suitability of plasmonic nanomaterials to tune enzyme activity arises from their tunable localized surface plasmon resonances (LSPR), in the UV–vis and near-infrared wavelength ranges. − Under incident light, conduction electrons in metal nanoparticles display coherent collective oscillations, thereby generating intense absorption and scattering at specific wavelengths, resulting in LSPR signals. , It is well-known that the LSPR response is largely dictated by the dimensions and morphology of the plasmonic nanoparticles, but it is also highly sensitive to the interaction between biomolecules and the nanoparticles’ surface. , Therefore, LSPR excitation in resonance with light irradiation can be used as a potential tool to regulate protein functionality at the interface with the nanomaterial. For example, enzymes immobilized on the surface of nanoparticles can be readily triggered by light irradiation, to enhance their catalytic activity. ,,, When LSPR was harnessed, biocatalysis can be remotely regulated upon light irradiation to fine-tuning artificial reaction biocascades. ,,,− Hence, the use of light is a precise, sustainable, noninvasive, and remote method to foster innovative solutions in the biocatalysis field through merging enzymes and plasmonic nanoparticles (Figure ).…”

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Light-Driven Catalytic Regulation of Enzymes at the Interface with Plasmonic Nanomaterials

2020

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Regulation of enzymes is highly relevant toward orchestrating cell-free and stepwise biotransformations, thereby maximizing their overall performance. Plasmonic nanomaterials offer a great opportunity to tune the functionality of enzymes, through their remarkable optical properties. Localized surface plasmon resonances (LSPR) can be used to modify chemical transformations at the nanomaterial's surface, upon light irradiation.Incident light can promote energetic processes, which may be related to an increase of local temperature (photothermal effects), but also to effects triggered by generated hotspots or hot-electrons (photoelectronic effects). As a consequence, light irradiation of the protein-nanomaterial interface affects enzyme functionality. To harness these effects to finely and remotely regulate enzyme activity, the physicochemical features of the

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Light-Driven Catalytic Regulation of Enzymes at the Interface with Plasmonic Nanomaterials

2020

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“…As alternative SERS substrates, Au nanostars feature intrinsic hot spots located at the tips, thereby being advantageous with respect to spherical nanoparticles. 34 , 35 Moreover, their combination with iron oxide, forming a small and compact hybrid nanomaterial, ensures efficient magnetic manipulation enabled by its superparamagnetic properties. 36 − 38 The small dimensions as compared to the usually employed microbeads also allow a much faster diffusion and mixing with other reagents and analytes.…”

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confidence: 99%

3D Printed Microfluidic Device for Magnetic Trapping and SERS Quantitative Evaluation of Environmental and Biomedical Analytes

Litti

Trivini

Ferraro³

et al. 2021

ACS Appl. Mater. Interfaces

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Surface-enhanced Raman scattering (SERS) is an ideal technique for environmental and biomedical sensor devices due to not only the highly informative vibrational features but also to its ultrasensitive nature and possibilities toward quantitative assays. Moreover, in these areas, SERS is especially useful as water hinders most of the spectroscopic techniques such as those based on IR absorption. Despite its promising possibilities, most SERS substrates and technological frameworks for SERS detection are still restricted to research laboratories, mainly due to a lack of robust technologies and standardized protocols. We present herein the implementation of Janus magnetic/plasmonic Fe 3 O 4 /Au nanostars (JMNSs) as SERS colloidal substrates for the quantitative determination of several analytes. This multifunctional substrate enables the application of an external magnetic field for JMNSs retention at a specific position within a microfluidic channel, leading to additional amplification of the SERS signals. A microfluidic device was devised and 3D printed as a demonstration of cheap and fast production, with the potential for large-scale implementation. As low as 100 μL of sample was sufficient to obtain results in 30 min, and the chip could be reused for several cycles. To show the potential and versatility of the sensing system, JMNSs were exploited with the microfluidic device for the detection of several relevant analytes showing increasing analytical difficulty, including the comparative detection of p -mercaptobenzoic acid and crystal violet and the quantitative detection of the herbicide flumioxazin and the anticancer drug erlotinib in plasma, where calibration curves within diagnostic concentration intervals were obtained.

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“…Plasmonic nanomaterials, such as gold nanoparticles (Au NPs), display remarkable optical properties in the visible and near-infrared (NIR) spectral regions. [1][2][3] Such properties arise as a result of the excitation of localized surface plasmon resonances (LSPRs). It has been established that LSPR excitation in plasmonic NPs can accelerate a myriad of chemical transformations.…”

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confidence: 99%

Mechanistic Insights into the Light-Driven Catalysis of an Immobilized Lipase on Plasmonic Nanomaterials

et al. 2020

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The use of light as an external stimulus to control enzyme activity is an emerging strategy that enables accurate, remote and noninvasive biotransformations. In this context, immobilization of enzymes on plasmonic nanoparticles offers an opportunity to create light-responsive biocatalytic materials. Nevertheless, a fundamental and mechanistic understanding on the effects of localized surface plasmon resonance (LSPR) excitation over enzyme regulation remains elusive. We investigate herein the plasmonic effects on biocatalysis using Au nanospheres (AuNSp) and nanostars (AuNSt) as model plasmonic nanoparticles, lipase from Candida antarctica fraction B (CALB) as a proof of concept enzyme, and 808 nm as NIR light excitation. Our data show that LSPR excitation enables an enhancement of 58% in enzyme activity for CALB adsorbed on AuNSt, compared with the dark conditions. This work shows how photothermal heating over the LSPR excitation enhances CALB activity through favoring product release in the last step of the enzyme mechanism. We propose that the results reported herein shed important mechanistic and kinetic insights in the field of plasmonic biocatalysis and may inspire the rational development of plasmonic nanomaterial-enzyme hybrids with tailored activities under external light irradiation.

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Manipulating chemistry through nanoparticle morphology

Abstract: The complex anisotropy of Au-nanostars is used to manipulate the protonation chemistry of selected molecules, monitored through their SERS signals.

Cited by 34 publications

References 58 publications

Light-Driven Catalytic Regulation of Enzymes at the Interface with Plasmonic Nanomaterials

Light-Driven Catalytic Regulation of Enzymes at the Interface with Plasmonic Nanomaterials

3D Printed Microfluidic Device for Magnetic Trapping and SERS Quantitative Evaluation of Environmental and Biomedical Analytes

Mechanistic Insights into the Light-Driven Catalysis of an Immobilized Lipase on Plasmonic Nanomaterials

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