| 1. |
- Fritzsche, Joachim, 1977, et al.
(författare)
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Single Particle Nanoplasmonic Sensing in Individual Nanofluidic Channels
- 2016
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Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 16:12, s. 7857-7864
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Tidskriftsartikel (refereegranskat)abstract
- Nanoplasmonics allows label-free optical sensing and spectroscopy at the single nanoparticle level by exploiting plasmonic excitations in metal nanoparticles. Nanofluidics offers exclusive possibilities for applying and controlling fluid flow and mass transport at the nanoscale and toward nanosized objects. Here, we combine these two concepts in a single device, by integrating single particle nanoplasmonic sensing with nanofluidics using advanced nanofabrication. The developed devices enable on-chip referenced parallel single particle nanoplasmonic sensing inside multiple individual nanofluidic channels with dimensions down to the 100 nm range. Beyond detailed discussion of the nanofabrication, general device characterization, and parallelized single particle plasmonic readout concepts, we demonstrate device function on two examples: (i) in situ measurements of local buffer concentrations inside a nanofluidic channel; (ii) real time binding kinetics of alkanethiol molecules to a single plasmonic nanonatenna sensor in a single nanochannel. Our concept thus provides a powerful solution for controlling mass transport to and from individual (plasmonic) nanoparticles, which in a long-term perspective offers unique opportunities for label-free detection of analyte molecules at low concentrations and for fundamental studies of fluids in extreme confinement.
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| 2. |
- Albinsson, David, 1990, et al.
(författare)
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Operando detection of single nanoparticle activity dynamics inside a model pore catalyst material
- 2020
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Ingår i: Science advances. - : American Association for the Advancement of Science (AAAS). - 2375-2548. ; 6:25
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Tidskriftsartikel (refereegranskat)abstract
- 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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| 3. |
- Albinsson, David, 1990, et al.
(författare)
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Shedding light on CO oxidation surface chemistry on single Pt catalyst nanoparticles inside a nanofluidic model pore
- 2021
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Ingår i: ACS Catalysis. - : American Chemical Society (ACS). - 2155-5435. ; 11:4, s. 2021-2033
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Tidskriftsartikel (refereegranskat)abstract
- Investigating a catalyst under relevant application conditions is experimentally challenging and parameters like reaction conditions in terms of temperature, pressure, and reactant mixing ratios, as well as catalyst design, may significantly impact the obtained experimental results. For Pt catalysts widely used for the oxidation of carbon monoxide, there is keen debate on the oxidation state of the surface at high temperatures and at/above atmospheric pressure, as well as on the most active surface state under these conditions. Here, we employ a nanoreactor in combination with single-particle plasmonic nanospectroscopy to investigate individual Pt catalyst nanoparticles localized inside a nanofluidic model pore during carbon monoxide oxidation at 2 bar in the 450-550 K temperature range. As a main finding, we demonstrate that our single-particle measurements effectively resolve a kinetic phase transition during the reaction and that each individual particle has a unique response. Based on spatially resolved measurements, we furthermore observe how reactant concentration gradients formed due to conversion inside the model pore give rise to position-dependent kinetic phase transitions of the individual particles. Finally, employing extensive electrodynamics simulations, we unravel the surface chemistry of the individual Pt nanoparticles as a function of reactant composition and find strongly temperature-dependent Pt-oxide formation and oxygen spillover to the SiO2 support as the main processes. These results therefore support the existence of a Pt surface oxide in the regime of high catalyst activity and demonstrate the possibility to use plasmonic nanospectroscopy in combination with nanofluidics as a tool for in situ studies of individual catalyst particles.
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| 4. |
- Albinsson, David, 1990, et al.
(författare)
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Single Particle Nanoplasmonic Sensing in Individual Nanofluidic Channels
- 2017
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Ingår i: The 8th International Conference on Surface Plasmon Photonics (SPP8).
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Konferensbidrag (refereegranskat)abstract
- By combining the precise mass transport control of nanofluidics with the single particle sensing abilities of nanoplasmonics we demonstrate real time single particle parallel readout of multiple nanofluidic channels from the same chip using plasmonic nanospectroscopy.The exceptional label-free sensitivity of individual plasmonic nanoparticles combined with dark-field scattering spectroscopy has proven to be a powerful tool in catalysis[1], materials science[2], and gas sensing[3], as well as to detect single molecular binding events[4]. However, despite the proven sensitivity of single particle plasmonic nanosensors, the detection of ultralow concentrations of specific analyte molecules is limited by the fact that they usually are free to diffuse away from the sensing surface, which gives rise to unpractical detection times on the order of days.As a first step to alleviate this limitation, we present an integrated nanoplasmonic-nanofluidic platform comprised of nanochannels integrated with a single plasmonic nanoantenna sensor, schematically presented in Fig 1. The dimensions of the nanofluidic system are chosen such that the entire volume of analyte solution is forced to pass the plasmonic sensor within the decay length of the near field, in order to significantly enhance the probability of direct interaction of the sensor surface with analyte in the channel. The developed devices enable on-chip referenced parallel single particle nanoplasmonic sensing inside multiple individual nanofluidic channels with dimensions down to the 100 nm range. Beyond detailed discussion of the nanofabrication, general device characterization, and parallelized single particle plasmonic readout concepts, we present the device function on two examples: (i) in situ measurements of local buffer concentrations inside a nanofluidic channel; (ii) real time binding kinetics of alkanethiol molecules to a single plasmonic nanoantenna sensor in a single nanochannel.
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| 5. |
- Alekseeva, Svetlana, 1987, et al.
(författare)
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Grain-growth mediated hydrogen sorption kinetics and compensation effect in single Pd nanoparticles
- 2021
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723 .- 2041-1723. ; 12:1
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Tidskriftsartikel (refereegranskat)abstract
- Grains constitute the building blocks of polycrystalline materials and their boundaries determine bulk physical properties like electrical conductivity, diffusivity and ductility. However, the structure and evolution of grains in nanostructured materials and the role of grain boundaries in reaction or phase transformation kinetics are poorly understood, despite likely importance in catalysis, batteries and hydrogen energy technology applications. Here we report an investigation of the kinetics of (de)hydriding phase transformations in individual Pd nanoparticles. We find dramatic evolution of single particle grain morphology upon cyclic exposure to hydrogen, which we identify as the reason for the observed rapidly slowing sorption kinetics, and as the origin of the observed kinetic compensation effect. These results shed light on the impact of grain growth on kinetic processes occurring inside nanoparticles, and provide mechanistic insight in the observed kinetic compensation effect. Grains are the building blocks of crystalline solids. Here the authors show how hydrogen-sorption induced grain-growth in Pd nanoparticles slows down the hydrogen sorption kinetics and constitutes the physical origin of corresponding kinetic compensation.
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| 6. |
- Altenburger, Björn, 1990, et al.
(författare)
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Label-Free Imaging of Catalytic H 2 O 2 Decomposition on Single Colloidal Pt Nanoparticles Using Nanofluidic Scattering Microscopy
- 2023
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Ingår i: ACS Nano. - 1936-086X .- 1936-0851. ; 17:21, s. 21030-21043
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Tidskriftsartikel (refereegranskat)abstract
- Single-particle catalysis aims at determining factors that dictate the nanoparticle activity and selectivity. Existing methods often use fluorescent model reactions at low reactant concentrations, operate at low pressures, or rely on plasmonic enhancement effects. Hence, methods to measure single-nanoparticle activity under technically relevant conditions and without fluorescence or other enhancement mechanisms are still lacking. Here, we introduce nanofluidic scattering microscopy of catalytic reactions on single colloidal nanoparticles trapped inside nanofluidic channels to fill this gap. By detecting minuscule refractive index changes in a liquid flushed trough a nanochannel, we demonstrate that local H2O2 concentration changes in water can be accurately measured. Applying this principle, we analyze the H2O2 concentration profiles adjacent to single colloidal Pt nanoparticles during catalytic H2O2 decomposition into O2 and H2O and derive the particles’ individual turnover frequencies from the growth rate of the O2 gas bubbles formed in their respective nanochannel during reaction.
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| 7. |
- Andersson, Carl, 1996, et al.
(författare)
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A Microshutter for the Nanofabrication of Plasmonic Metal Alloys with Single Nanoparticle Composition Control
- 2023
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Ingår i: ACS Nano. - 1936-086X .- 1936-0851. ; 17:16, s. 15978-15988
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Tidskriftsartikel (refereegranskat)abstract
- Alloying offers an increasingly important handle in nanomaterials design in addition to the already widely explored size and geometry of nanostructures of interest. As the key trait, the mixing of elements at the atomic level enables nanomaterials with physical or chemical properties that cannot be obtained by a single element alone, and subtle compositional variations can significantly impact these properties. Alongside the great potential of alloying, the experimental scrutiny of its impact on nanomaterial function is a challenge because the parameter space that encompasses nanostructure size, geometry, chemical composition, and structural atomic-level differences among individuals is vast and requires unrealistically large sample sets if statistically relevant and systematic data are to be obtained. To address this challenge, we have developed a microshutter device for spatially highly resolved physical vapor deposition in the lithography-based fabrication of nanostructured surfaces. As we demonstrate, it enables establishing compositional gradients across a surface with single nanostructure resolution in terms of alloy composition, which subsequently can be probed in a single experiment. As a showcase, we have nanofabricated arrays of AuAg, AuPd, and AgPd alloy nanoparticles with compositions systematically controlled at the level of single particle rows, as verified by energy dispersive X-ray and single particle plasmonic nanospectroscopy measurements, which we also compared to finite-difference time-domain simulations. Finally, motivated by their application in state-of-the-art plasmonic hydrogen sensors, we investigated PdAu alloy gradient arrays for their hydrogen sorption properties. We found distinctly composition-dependent kinetics and hysteresis and revealed a composition-dependent contribution of a single nanoparticle response to the ensemble average, which highlights the importance of alloy composition screening in single experiments with single nanoparticle resolution, as offered by the microshutter nanofabrication approach.
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| 8. |
- Levin, Sune, 1991, et al.
(författare)
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A nanofluidic device for parallel single nanoparticle catalysis in solution
- 2019
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723 .- 2041-1723. ; 10:1
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Tidskriftsartikel (refereegranskat)abstract
- Studying single catalyst nanoparticles, during reaction, eliminates averaging effects that are an inherent limitation of ensemble experiments. It enables establishing structure-function correlations beyond averaged properties by including particle-specific descriptors such as defects, chemical heterogeneity and microstructure. Driven by these prospects, several single particle catalysis concepts have been implemented. However, they all have limitations such as low throughput, or that they require very low reactant concentrations and/or reaction rates. In response, we present a nanofluidic device for highly parallelized single nanoparticle catalysis in solution, based on fluorescence microscopy. Our device enables parallel scrutiny of tens of single nanoparticles, each isolated inside its own nanofluidic channel, and at tunable reaction conditions, ranging from the fully mass transport limited regime to the surface reaction limited regime. In a wider perspective, our concept provides a versatile platform for highly parallelized single particle catalysis in solution and constitutes a promising application area for nanofluidics.
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| 9. |
- Levin, Sune, 1991, et al.
(författare)
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Nanofluidic Trapping of Faceted Colloidal Nanocrystals for Parallel Single-Particle Catalysis
- 2022
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Ingår i: Acs Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 16:9
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Tidskriftsartikel (refereegranskat)abstract
- Catalyst activity can depend distinctly on nano -particle size and shape. Therefore, understanding the structure sensitivity of catalytic reactions is of fundamental and technical importance. Experiments with single-particle resolution, where ensemble-averaging is eliminated, are required to study it. Here, we implement the selective trapping of individual spherical, cubic, and octahedral colloidal Au nanocrystals in 100 parallel nanofluidic channels to determine their activity for fluorescein reduction by sodium borohydride using fluorescence microscopy. As the main result, we identify distinct structure sensitivity of the rate-limiting borohydride oxidation step originating from different edge site abundance on the three particle types, as confirmed by first -principles calculations. This advertises nanofluidic reactors for the study of structure-function correlations in catalysis and identifies nanoparticle shape as a key factor in borohydride-mediated catalytic reactions.
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| 10. |
- Nilsson, Sara, 1990, et al.
(författare)
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Competing oxidation mechanisms in Cu nanoparticles and their plasmonic signatures
- 2022
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Ingår i: Nanoscale. - : Royal Society of Chemistry (RSC). - 2040-3372 .- 2040-3364. ; 14:23, s. 8332-8341
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Tidskriftsartikel (refereegranskat)abstract
- Chemical reactions involving nanoparticles often follow complex processes. In this respect, real-time probing of single nanoparticles under reactive conditions is crucial for uncovering the mechanisms driving the reaction pathway. Here, we have captured in situ the oxidation of single Cu nanoparticles to unravel a sequential competitive activation of different mechanisms at temperatures 50-200 degrees C. Using environmental scanning transmission electron microscopy, we monitor the evolution of oxide formation with sub-nanometre spatial resolution, and show how the prevalence of oxide island nucleation, Cabrera-Mott, Valensi-Carter and Kirkendall mechanisms under different conditions determines the morphology of the particles. Moreover, using in situ electron energy-loss spectroscopy, we probe the localised surface plasmons of individual particles during oxidation, and with the aid of finite-difference time-domain electrodynamic simulations investigate the signature of each mechanism in their plasmonic response. Our results shed light on the rich and intricate processes involved in the oxidation of nanoparticles, and provide in-depth insight into how these processes govern their morphology and optical response, beneficial for applications in catalysis, sensing, nanomedicine and plasmonics.
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