A nanofluidic device for parallel single nanoparticle catalysis in solution

Levin, Sune; Fritzsche, Joachim; Nilsson, Sara; Runemark, August; Dhokale, Bhausaheb; Ström, Henrik; Sundén, Henrik; Langhammer, Christoph; Westerlund, Fredrik

doi:10.1038/s41467-019-12458-1

Cited by 33 publications

(28 citation statements)

References 37 publications

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“…Most gold nanozyme studies reported in the literature are based on AuNPs synthesized using bottom-up approaches due to their low-cost and facile syntheses. However, gold nanostructures exhibiting catalytic properties have also been fabricated through top-down approaches [90][91][92]. Cao et al [90] found that these properties could be improved by fabrication of nanostructured arrays on Au thin film.…”

Section: Catalytic Properties Of Gold Nanoparticlesmentioning

confidence: 99%

“…Electron beam lithography has also been used to fabricate a nanofluidic device consisting of 11 sets of 5 nanochannels, each decorated with a set of single-Au nanoparticles with identical size. These NPs were grown through Au evaporation and used for the reduction of fluorescein as a model reaction [91]. Also arrays of electrically driven plasmonic nanorods have been used for catalytic purposes, as the numerous resulting tunnel junctions favour the generation of hot electrons, facilitating strongly confined chemical reactions.…”

Section: Catalytic Properties Of Gold Nanoparticlesmentioning

confidence: 99%

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Gold Nanozymes: From Concept to Biomedical Applications

et al. 2020

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In recent years, gold nanoparticles have demonstrated excellent enzyme-mimicking activities which resemble those of peroxidase, oxidase, catalase, superoxide dismutase or reductase. This, merged with their ease of synthesis, tunability, biocompatibility and low cost, makes them excellent candidates when compared with biological enzymes for applications in biomedicine or biochemical analyses. Herein, over 200 research papers have been systematically reviewed to present the recent progress on the fundamentals of gold nanozymes and their potential applications. The review reveals that the morphology and surface chemistry of the nanoparticles play an important role in their catalytic properties, as well as external parameters such as pH or temperature. Yet, real applications often require specific biorecognition elements to be immobilized onto the nanozymes, leading to unexpected positive or negative effects on their activity. Thus, rational design of efficient nanozymes remains a challenge of paramount importance. Different implementation paths have already been explored, including the application of peroxidase-like nanozymes for the development of clinical diagnostics or the regulation of oxidative stress within cells via their catalase and superoxide dismutase activities. The review also indicates that it is essential to understand how external parameters may boost or inhibit each of these activities, as more than one of them could coexist. Likewise, further toxicity studies are required to ensure the applicability of gold nanozymes in vivo. Current challenges and future prospects of gold nanozymes are discussed in this review, whose significance can be anticipated in a diverse range of fields beyond biomedicine, such as food safety, environmental analyses or the chemical industry.

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Section: Catalytic Properties Of Gold Nanoparticlesmentioning

confidence: 99%

Section: Catalytic Properties Of Gold Nanoparticlesmentioning

confidence: 99%

Gold Nanozymes: From Concept to Biomedical Applications

et al. 2020

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“…This ensures that the obtained single particle results can provide the anticipated guidance for improving the performance of real catalysts, which naturally are composed of a large ensemble. To this end, the demonstrated use of nanofluidic structures in single particle catalysis in the gas phase also constitutes the first application of the nanofluidics paradigm to a gaseous fluid in general and therefore goes substantially beyond its recently introduced liquid-phase counterpart (18).…”

Section: Introductionmentioning

confidence: 99%

Operando detection of single nanoparticle activity dynamics inside a model pore catalyst material

et al. 2020

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Nanoconfinement in porous catalysts may induce reactant concentration gradients inside the pores due to local conversion. This leads to inefficient active material use since parts of the catalyst may be trapped in an inactive state. Experimentally, these effects remain unstudied due to material complexity and required high spatial resolution. Here, we have nanofabricated quasi–two-dimensional mimics of porous catalysts, which combine the traits of nanofluidics with single particle plasmonics and online mass spectrometry readout. Enabled by single particle resolution at operando conditions during CO oxidation over a Cu model catalyst, we directly visualize reactant concentration gradient formation due to conversion on single Cu nanoparticles inside the “model pore” and how it dynamically controls oxidation state—and, thus, activity—of particles downstream. Our results provide a general framework for single particle catalysis in the gas phase and highlight the importance of single particle approaches for the understanding of complex catalyst materials.

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“…In response, we introduce highly multiplexed operando single particle plasmonic nanoimaging in combination with our recently developed nanofluidic reactor platform 24,25 that enables online mass spectrometry from extremely small amounts of catalyst material. As the key advance, we demonstrate how this concept is able to combine single particle resolution in catalyst state dynamics imaging from a quasi-2D array of 1000 nominally identical Cu nanoparticles that constitute the whole catalyst bed, with online quadrupole mass spectrometry (QMS) from the same particles.…”

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confidence: 99%

Copper catalysis at operando conditions—bridging the gap between single nanoparticle probing and catalyst-bed-averaging

et al. 2020

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In catalysis, nanoparticles enable chemical transformations and their structural and chemical fingerprints control activity. To develop understanding of such fingerprints, methods studying catalysts at realistic conditions have proven instrumental. Normally, these methods either probe the catalyst bed with low spatial resolution, thereby averaging out single particle characteristics, or probe an extremely small fraction only, thereby effectively ignoring most of the catalyst. Here, we bridge the gap between these two extremes by introducing highly multiplexed single particle plasmonic nanoimaging of model catalyst beds comprising 1000 nanoparticles, which are integrated in a nanoreactor platform that enables online mass spectroscopy activity measurements. Using the example of CO oxidation over Cu, we reveal how highly local spatial variations in catalyst state dynamics are responsible for contradicting information about catalyst active phase found in the literature, and identify that both surface and bulk oxidation state of a Cu nanoparticle catalyst dynamically mediate its activity.

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A nanofluidic device for parallel single nanoparticle catalysis in solution

Cited by 33 publications

References 37 publications

Gold Nanozymes: From Concept to Biomedical Applications

Gold Nanozymes: From Concept to Biomedical Applications

Operando detection of single nanoparticle activity dynamics inside a model pore catalyst material

Copper catalysis at operando conditions—bridging the gap between single nanoparticle probing and catalyst-bed-averaging

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