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2. Pathways to electrochemical solar-hydrogen technologies

Author

Ardo, S, Fernandez Rivas, D, Modestino, MA, Schulze Greiving, V, Abdi, FF, Alarcon Llado, E, Artero, V, Ayers, K, Battaglia, C, Becker, JP, Bederak, D, Berger, A, Buda, F, Chinello, E, Dam, B, Di Palma, V, Edvinsson, T, Fujii, K, Gardeniers, H, Geerlings, H, Hashemi, SM, Haussener, S, Houle, F, Huskens, J, James, BD, Konrad, K, Kudo, A, Kunturu, PP, Lohse, D, Mei, B, Miller, EL, Moore, GF, Muller, J, Orchard, KL, Rosser, TE, Saadi, FH, Schüttauf, JW, Seger, B, Sheehan, SW, Smith, WA, Spurgeon, J, Tang, MH, Van De Krol, R, Vesborg, PCK, and Westerik, P

Subjects
Bioengineering, MD Multidisciplinary, Energy
Abstract

Solar-powered electrochemical production of hydrogen through water electrolysis is an active and important research endeavor. However, technologies and roadmaps for implementation of this process do not exist. In this perspective paper, we describe potential pathways for solar-hydrogen technologies into the marketplace in the form of photoelectrochemical or photovoltaic-driven electrolysis devices and systems. We detail technical approaches for device and system architectures, economic drivers, societal perceptions, political impacts, technological challenges, and research opportunities. Implementation scenarios are broken down into short-term and long-term markets, and a specific technology roadmap is defined. In the short term, the only plausible economical option will be photovoltaic-driven electrolysis systems for niche applications. In the long term, electrochemical solar-hydrogen technologies could be deployed more broadly in energy markets but will require advances in the technology, significant cost reductions, and/or policy changes. Ultimately, a transition to a society that significantly relies on solar-hydrogen technologies will benefit from continued creativity and influence from the scientific community.

Published
2018

14. Positioning and finding quantum dots in silicon nanostructures

Author

Schulz, Andreas Stefan, Grishina, Diana, Harteveld, Cornelis A.M., Pacureanu, Alexandra Teodora, Lagendijk, Aart, Huskens, J., Vancso, Julius, Cloetens, Peter, Vos, Willem L., Complex Photonic Systems, MESA+ Institute, Molecular Nanofabrication, and Materials Science and Technology of Polymers

Subjects
Condensed Matter::Soft Condensed Matter, polymerbrushes, xrayfluorescencetomography, photoniccrystals, quantumdots
Abstract

Control over the interaction between light and matter will have far-ranging consequences in chemistry, material science, physics, and biology. An important tool for the advanced control of light is offered by 3D photonic crystals with a photonic band gap, a range of frequencies for which light is forbidden to exist. We have developed methods to precisely control the location of lead sulfide quantum dots on silicon surfaces by attaching the dots to functionalized polymer brushes. Encouraged by successes on planar silicon wafers, we introduced quantum dots with polymer brushes in the nanopores of 2D and even 3D photonic band gap crystals. By synchrotron X-ray fluorescence tomography, we obtain detailed information on the positioning of the brushes and the dots. Notably, the quantum dot signal correlates very strongly with the brush signal, validating our approach. In optical experiments we find evidence for considerable emission inhibition in the 3D photonic band gap.

Published
2020

17. Surface with poly-cationic polymers and functionalized using coupling chemistry, biosensor comprising the same and use thereof in bio-sensing

Author

Huskens, J., Ricciardi, R., Movilli, Jacopo, Di Iorio, Daniele, Marti Morant, Almudena, and Molecular Nanofabrication

Abstract

The invention relates to a surface functionalized with a poly-L-lysine polymer provided with oligo-ethylene glycol moieties, which are in turn partly modified with a functional moiety. In addition, the invention relates to said functionalized surface, wherein the surface is provided with exposed receptor molecules for binding to an analyte in e.g. a complex biological sample. More specifically, the invention relates to a functionalized surface for use in e.g. a biosensor for sensing (bio)molecules in e.g. a biological fluid or a solution comprising a biomarker, wherein the functionalized surface comprises poly-L-lysine polymer adhered thereto, said poly-L-lysine in part modified with oligo-ethylene glycol moieties which carry functional groups capable of specifically binding to the biomarker, i.e. receptor molecules for binding to an analyte. In addition, the invention relates to a method for providing such a functionalized surface and to the use of the functionalized surface as a binding partner for the biomarker. More specifically, the functionalized surface is for example suitable for binding cDNA from a complex mixture such as a biological sample.

Published
2018

18. Characterization of lanthanide(III) DOTP complexes: thermodynamics, protonation, and coordination to alkali metal ions

Author

Sherry, A.D., Ren, J., Huskens, J., Brucher, E., Toth, E., Geraldes, C.F.C.G., Castro, M.M.C.A., and Cacheris, W.P.

Subjects
Rare earth metals -- Research, Complex compounds -- Research, Thermodynamics -- Measurement, Nuclear magnetic resonance spectroscopy -- Usage, Potentiometry -- Usage, Hydrogen-ion concentration -- Measurement, Chemistry
Abstract

Spectrophotometric, potentiometric, osmometric, and NMR studies characterize the solution properties of lanthanide(III) DOTP complexes. Spectrophotometry suggests that the thermodynamic stability constants of the complexes range from 27.6 to 29.6 from La(super III) to Lu(super III). These results are supported by 1H NMR and potentiometric titrations. Four protonation steps are indicated between pH 10 and 2 for these complexes. The 31P shifts shown by NMR studies are pH-dependent. NMR and osmometric studies on alkali cation binding to TmDOTP5- predicts the number of unassociated species in solution.

Published
1996

21. Cucurbit[n]uril assemblies for biomolecular applications

Author

Cavatorta, E., Brunsveld, L., Huskens, J., Jonkheijm, P., Prins, L.J., Haag, R., Ravoo, B.J., Chemical Biology, and Molecular Nanofabrication

Subjects
chemistry.chemical_classification, Molecular recognition, chemistry, Biomolecule, Supramolecular chemistry, Self-assembly, macromolecular substances, Combinatorial chemistry, Amino acid
Abstract

Cucurbit[n]urils (CB[n]s) provide a class of macrocycles that are able to form stable host–guest complexes with various guests. A wide range of potential guests has stimulated an increasing number of fundamental molecular recognition studies that led to various biomolecular applications. The systems are intrinsically dynamic and can rearrange, while some of the interactions are reversible upon stimuli. We have discussed the origins of the molecular recognition properties of the CB[n] family and methods to gain control over the binding affinity to CB[n]. We have described the amino acid based recognition of CB[n] and subsequently review the literature on how these properties can be successfully employed to dynamically probe the properties and function of peptides, proteins and cells, which is important for bioanalytical and biomedical applications.

Published
2018

25. Orthogonal supramolecular protein assembly on patterned bifunctional surfaces

Author

Wasserberg, D., Cabanas-Danés, J., Subramaniam, V., Huskens, J., Jonkheijm, P., Wasserberg, D., Cabanas-Danés, J., Subramaniam, V., Huskens, J., and Jonkheijm, P.

Abstract

We report successful and selective dual protein assembly on patterned bifunctional βCD-Ni(ii)NTA surfaces, using red fluorescent protein variants with hexahistidine-tags and teal fluorescent protein variants conjugated with a peptide containing three adamantyl groups. We show that dual protein patterns can only be assembled, when opposing supramolecular interactions have been optimized and nonspecific interactions have been sufficiently suppressed.

Published
2018
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29. Enhanced surface plasmon polariton propagation length using a buried metal grating.

Author

Jose, J., Segerink, F. B., Korterik, J. P., Gomez-Casado, A., Huskens, J., Herek, J. L., and Offerhaus, H. L.

Subjects
POLARITONS, PLASMONS (Physics), SUBSTRATES (Materials science), DETECTORS, QUANTUM theory
Abstract

We report an enhancement in the propagation length of surface plasmon polaritons (SPPs) on a metallic grating when the grating is buried in the substrate. A template-stripping technique has been used to fabricate the buried grating. Near-field measurements on the buried and an exposed grating show that the full width at half maximum of the surface plasmon resonances are reduced to 57% for the prism-coupled SPPs and 77% for the grating-coupled SPPs. The reduction in the full width at half maximum is attributed to a decrease in the in-plane directional scattering of the SPPs on the buried grating. The propagation lengths of the SPPs measured beyond the gratings are close to the theoretical SPP propagation length on an ideal gold surface. The buried grating with a significant reduction in the full width at half maximum of the surface plasmon resonances is theoretically shown to improve the figure of merit of grating-incorporated SPR sensors. [ABSTRACT FROM AUTHOR]

Published
2011
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33. Behaviour of the extractant Me-TODGA upon gamma irradiation: quantification of degradation compounds and individual influences on complexation and extraction

Author

Hubscher-Bruder, V., primary, Mogilireddy, V., additional, Michel, S., additional, Leoncini, A., additional, Huskens, J., additional, Verboom, W., additional, Galán, H., additional, Núñez, A., additional, Cobos, J., additional, Modolo, G., additional, Wilden, A., additional, Schmidt, H., additional, Charbonnel, M.-C., additional, Guilbaud, P., additional, and Boubals, N., additional

Published
2017
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34. Modulating the nucleated self-assembly of Tri-beta3-peptides using Cucurbit[n]urils

Author

Satav, T., Korevaar, P.A., de Greef, T.F.A., Huskens, J., Jonkheijm, P., Satav, T., Korevaar, P.A., de Greef, T.F.A., Huskens, J., and Jonkheijm, P.

Abstract

The modulation of the hierarchical nucleated self-assembly of tri-β3-peptides has been studied. β3-Tyrosine provided a handle to control the assembly process through host-guest interactions with CB[7] and CB[8]. By varying the cavity size from CB[7] to CB[8] distinct phases of assembling tri-β3-peptides were arrested. Given the limited size of the CB[7] cavity, only one aromatic β3-tyrosine can be simultaneously hosted and hence CB[7] was primarily acting as an inhibitor of self-assembly. In strong contrast, the larger CB[8] can form a ternary complex with two aromatic amino acids and hence CB[8] was acting primarily as cross-linker of multiple fibers and hence promoting the formation of larger aggregates. General insights on modulating supramolecular assembly can lead to new ways to introduce functionality in supramolecular polymers.

Published
2016

40. Optical amplification of Eu3+ emission via energy transfer at molecular printboards for the efficiency enhancement of the solar cell

Author

Shu Han Hsu, Yilmaz, D., Reinhoudt, D. N., Velders, A. H., Huskens, J., and Molecular Nanofabrication

Subjects
macromolecular substances
Abstract

The main challenge in nanotechnology resides in the precise spatial (self-) organization of nanoscale components onto surfaces. The molecular printboards, monolayers of β-cyclodextrin (β-CD), can be employed to bind suitable guest molecules onto a surface with molecular accuracy based on the host-guest interactions. Several lanthanides and their organic complexes are known to exhibit photoluminescent properties. Based on this host-guest interaction, the first example of the controllable SAMs of Eu3+ complexes is prepared on the molecular printboards and is successful to demonstrate the stoichiometry of the efficient energy transfer pair with a close proximity proved by local image spectra and surface emission life-time. To further maximize the optical amplification, self-assembled organic/ nanoparticles multilayers based on multivalent supramolecular host-guest interactions between dendritic guest molecules and host-modified TiO2 particles can result in a strong absorption and efficient sensitization thin film. The stable positioning nanostructure is used as antireflecting layer for enhancing the solar cell UV conversion studied with the photo to current conversion efficiency.

Published
2009

46. Oriented Protein Immobilization using Covalent and Noncovalent Chemistry on a Thiol-Reactive Self-Reporting Surface

Author

Wasserberg, D., Nicosia, C., Tromp, E.E., Subramaniam, V., Huskens, J., Jonkheijm, P., Wasserberg, D., Nicosia, C., Tromp, E.E., Subramaniam, V., Huskens, J., and Jonkheijm, P.

Abstract

Item does not contain fulltext, We report the fabrication of a patterned protein array using three orthogonal methods of immobilization that are detected exploiting a fluorogenic surface. Upon reaction of thiols, the fluorogenic tether reports the bond formation by an instantaneous rise in (blue) fluorescence intensity providing a means to visualize the immobilization even of nonfluorescent biomolecules. First, the covalent, oriented immobilization of a visible fluorescent protein (TFP) modified to display a single cysteine residue was detected. Colocalization of the fluorescence of the immobilized TFP and the fluorogenic group provided a direct tool to distinguish covalent bond formation from physisorption of proteins. Subsequent orthogonal immobilization of thiol-functionalized biomolecules could be conveniently detected by fluorescence microscopy using the fluorogenic surface. A thiol-modified nitrilotriacetate ligand was immobilized for binding of hexahistidine-tagged red-fluorescing TagRFP, while an appropriately modified biotin was immobilized for binding of Cy5-labeled streptavidin.

Published
2013

47. Immobilization of ferrocene-modified SNAP-fusion proteins

Author

Wasserberg, D., Uhlenheuer, D.A., Neirynck, P., Cabanas-Danés, J., Schenkel, J.H., Ravoo, B.J., An, Q., Huskens, J., Milroy, L.G., Brunsveld, L., Jonkheijm, P., Wasserberg, D., Uhlenheuer, D.A., Neirynck, P., Cabanas-Danés, J., Schenkel, J.H., Ravoo, B.J., An, Q., Huskens, J., Milroy, L.G., Brunsveld, L., and Jonkheijm, P.

Abstract

The supramolecular assembly of proteins on surfaces has been investigated via the site-selective incorporation of a supramolecular moiety on proteins. To this end, fluorescent proteins have been site-selectively labeled with ferrocenes, as supramolecular guest moieties, via SNAP-tag technology. The assembly of guest-functionalized SNAP-fusion proteins on cyclodextrin- and cucurbit[7]uril-coated surfaces yielded stable monolayers. The binding of all ferrocene fusion proteins is specific as determined by surface plasmon resonance. Micropatterns of the fusion proteins, on patterned cyclodextrin and cucurbituril surfaces, have been visualized using fluorescence microscopy. The SNAP-fusion proteins were also immobilized on cyclodextrin vesicles. The supramolecular SNAP-tag labeling of proteins, thus, allows for the assembly of modified proteins via supramolecular host-guest interaction on different surfaces in a controlled manner. These findings extend the toolbox of fabricating supramolecular protein patterns on surfaces taking advantage of the high labeling efficiency of the SNAP-tag with versatile supramolecular moieties.

Published
2013

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