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Author de la Croix, T.; Claes, N.; Eyley, S.; Thielemans, W.; Bals, S.; De Vos, D. pdf  url
doi  openurl
  Title Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene Type A1 Journal Article
  Year (down) 2023 Publication Catalysis Science & Technology Abbreviated Journal Catal. Sci. Technol.  
  Volume Issue Pages  
  Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;  
  Abstract The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt–Sn/C catalysts were prepared<italic>via</italic>a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored<italic>via</italic>gas-phase FTIR, and distribution of liquid products was analyzed<italic>via</italic>GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn<sub>2</sub>/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 001104905100001 Publication Date 2023-11-09  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2044-4753 ISBN Additional Links UA library record; WoS full record  
  Impact Factor 5 Times cited Open Access Not_Open_Access  
  Notes T. de la Croix gratefully acknowledges the support of the Flanders Research Foundation (FWO) under project 11F6622N. D. De Vos is grateful to FWO for support of project G0D3721N, and to KU Leuven for the iBOF project 21/016/C3. S. Bals and N. Claes acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grant No. 815128- REALNANO). W. Thielemans and S. Eyley thank KU Leuven (grant C14/18/061) and FWO (G0A1219N) for financial support. Approved Most recent IF: 5; 2023 IF: 5.773  
  Call Number EMAT @ emat @c:irua:201010 Serial 8968  
Permanent link to this record
 

 
Author Zhang, Y.; van Schayck, J.P.; Pedrazo-Tardajos, A.; Claes, N.; Noteborn, W.E.M.; Lu, P.-H.; Duimel, H.; Dunin-Borkowski, R.E.; Bals, S.; Peters, P.J.; Ravelli, R.B.G. pdf  url
doi  openurl
  Title Charging of vitreous samples in cryogenic electron microscopy mitigated by graphene Type A1 Journal article
  Year (down) 2023 Publication ACS nano Abbreviated Journal  
  Volume 17 Issue 16 Pages 15836-15846  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Cryogenic electronmicroscopy can provide high-resolution reconstructionsof macromolecules embedded in a thin layer of ice from which atomicmodels can be built de novo. However, the interactionbetween the ionizing electron beam and the sample results in beam-inducedmotion and image distortion, which limit the attainable resolutions.Sample charging is one contributing factor of beam-induced motionsand image distortions, which is normally alleviated by including partof the supporting conducting film within the beam-exposed region.However, routine data collection schemes avoid strategies wherebythe beam is not in contact with the supporting film, whose rationaleis not fully understood. Here we characterize electrostatic chargingof vitreous samples, both in imaging and in diffraction mode. We mitigatesample charging by depositing a single layer of conductive grapheneon top of regular EM grids. We obtained high-resolution single-particleanalysis (SPA) reconstructions at 2 & ANGS; when the electron beamonly irradiates the middle of the hole on graphene-coated grids, usingdata collection schemes that previously failed to produce sub 3 & ANGS;reconstructions without the graphene layer. We also observe that theSPA data obtained with the graphene-coated grids exhibit a higher b factor and reduced particle movement compared to dataobtained without the graphene layer. This mitigation of charging couldhave broad implications for various EM techniques, including SPA andcryotomography, and for the study of radiation damage and the developmentof future sample carriers. Furthermore, it may facilitate the explorationof more dose-efficient, scanning transmission EM based SPA techniques.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 001041649900001 Publication Date 2023-08-02  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record  
  Impact Factor 17.1 Times cited Open Access OpenAccess  
  Notes We thank H. Nguyen for editing the manuscript. We warmly thank the M4i Microscopy CORE Lab team of FHML Maastricht University (MU) for their support and collaboration and Eve Timlin and Ye Gao (MU) for providing protein samples. Members of the Amsterdam Scientific Instruments team are acknowledged for their Timepix detector support. This work benefited from access to The Netherlands Centre for Electron Nanoscopy (NeCEN) with assistance from Ludovic Renault and Meindert Lamers. The authors acknowledge financial support of the Netherlands Electron Microscopy Infrastructure (NEMI), project number 184.034.014 of the National Roadmap for Large-Scale Research Infrastructure of the Dutch Research Council (NWO), the PPP Allowance made available by Health-Holland, Top Sector Life Sciences & Health, to stimulate public-private partnerships, project 4DEM, number LSHM21029, and the LINK program from the Province of Limburg, The Netherlands, as well as financial support from the European Commission under the Horizon 2020 Programme by grant no. 815128 (REALNANO). Approved Most recent IF: 17.1; 2023 IF: 13.942  
  Call Number UA @ admin @ c:irua:198376 Serial 8840  
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Author Muravev, V.; Parastaev, A.; van den Bosch, Y.; Ligt, B.; Claes, N.; Bals, S.; Kosinov, N.; Hensen, E.J.M. pdf  url
doi  openurl
  Title Size of cerium dioxide support nanocrystals dictates reactivity of highly dispersed palladium catalysts Type A1 Journal Article
  Year (down) 2023 Publication Science Abbreviated Journal  
  Volume 380 Issue 6650 Pages 1174-1179  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract The catalytic performance of heterogeneous catalysts can be tuned by modulation of the size and structure of supported transition metals, which are typically regarded as the active sites. In single-atom metal catalysts, the support itself can strongly affect the catalytic properties. Here, we demonstrate that the size of cerium dioxide (CeO2) support governs the reactivity of atomically dispersed palladium (Pd) in carbon monoxide (CO) oxidation. Catalysts with small CeO2 nanocrystals (~4 nanometers) exhibit unusually high activity in a CO-rich reaction feed, whereas catalysts with medium-size CeO2 (~8 nanometers) are preferred for lean conditions. Detailed spectroscopic investigations reveal support size–dependent redox properties of the Pd-CeO2 interface.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 001010846100008 Publication Date 2023-06-16  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0036-8075 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 56.9 Times cited 22 Open Access OpenAccess  
  Notes We thank the staff of the MAX IV Laboratory for time on beamline SPECIES under proposals 20200412 and 20190983; E. Kokkonen and A. Klyushin for assistance with NAP-XPS and RPES experiments conducted at SPECIES; staff of the MAX IV Laboratory for time on beamline BALDER under proposal 20200378; K. Klementiev for assistance with XAS measurements; J. Drnec at the ESRF for providing assistance in using beamline ID31; and V. Perez-Dieste and I. Villar Garcia at the CIRCE beamline at ALBA Synchrotron for help with acquiring preliminary RPES data obtained under proposal 2020024219. The synchrotron-based XRD measurements were performed on beamline ID31 at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. Funding: This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), a NWO Gravitation program funded by the Ministry of Education, Culture and Science of the Government of the Netherlands (V.M. and E.J.M.H.); the European Research Council (ERC consolidator grant 815128 REALNANO to S.B. and N.C.); and the European Union’s Horizon 2020 Research and Innovation Program (grant 823717–ESTEEM to S.B. and N.C). Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496 (VM). Approved Most recent IF: 56.9; 2023 IF: 37.205  
  Call Number EMAT @ emat @c:irua:197199 Serial 8801  
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Author Kavak, S.; Kadu, A.A.; Claes, N.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Batenburg, K.J.; Bals, S. pdf  url
doi  openurl
  Title Quantitative 3D Investigation of Nanoparticle Assemblies by Volumetric Segmentation of Electron Tomography Data Sets Type A1 Journal Article
  Year (down) 2023 Publication The journal of physical chemistry: C : nanomaterials and interfaces Abbreviated Journal  
  Volume 127 Issue 20 Pages 9725-9734  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Morphological characterization of nanoparticle assemblies and hybrid nanomaterials is critical in determining their structure-property relationships as well as in the development of structures with desired properties. Electron tomography has become a widely utilized technique for the three-dimensional characterization of nanoparticle assemblies. However, the extraction of quantitative morphological parameters from the reconstructed volume can be a complex and labor-intensive task. In this study, we aim to overcome this challenge by automating the volumetric segmentation process applied to three-dimensional reconstructions of nanoparticle assemblies. The key to enabling automated characterization is to assess the performance of different volumetric segmentation methods in accurately extracting predefined quantitative descriptors for morphological characterization. In our methodology, we compare the quantitative descriptors obtained through manual segmentation with those obtained through automated segmentation methods, to evaluate their accuracy and effectiveness. To show generality, our study focuses on the characterization of assemblies of CdSe/CdS quantum dots, gold nanospheres and CdSe/CdS encapsulated in polymeric micelles, and silica-coated gold nanorods decorated with both CdSe/CdS or PbS quantum dots. We use two unsupervised segmentation algorithms: the watershed transform and the spherical Hough transform. Our results demonstrate that the choice of automated segmentation method is crucial for accurately extracting the predefined quantitative descriptors. Specifically, the spherical Hough transform exhibits superior performance in accurately extracting quantitative descriptors, such as particle size and interparticle distance, thereby allowing for an objective, efficient, and reliable volumetric segmentation of complex nanoparticle assemblies.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000991752700001 Publication Date 2023-05-25  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 3.7 Times cited 2 Open Access OpenAccess  
  Notes Fonds Wetenschappelijk Onderzoek, 1181122N ; Horizon 2020 Framework Programme, 861950 ; H2020 European Research Council, 815128 ; Approved Most recent IF: 3.7; 2023 IF: 4.536  
  Call Number EMAT @ emat @c:irua:196971 Serial 8793  
Permanent link to this record
 

 
Author Heyvaert, W.; Pedrazo-Tardajos, A.; Kadu, A.; Claes, N.; González-Rubio, G.; Liz-Marzán, L.M.; Albrecht, W.; Bals, S. pdf  url
doi  openurl
  Title Quantification of the Helical Morphology of Chiral Gold Nanorods Type A1 Journal article
  Year (down) 2022 Publication ACS materials letters Abbreviated Journal ACS Materials Lett.  
  Volume 4 Issue Pages 642-649  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Chirality in inorganic nanoparticles and nanostructures has gained increasing scientific interest, because of the possibility to tune their ability to interact differently with left- and right-handed circularly polarized light. In some cases, the optical activity is hypothesized to originate from a chiral morphology of the nanomaterial. However, quantifying the degree of chirality in objects with sizes of tens of nanometers is far from straightforward. Electron tomography offers the possibility to faithfully retrieve the three-dimensional morphology of nanomaterials, but only a qualitative interpretation of the morphology of chiral nanoparticles has been possible so far. We introduce herein a methodology that enables us to quantify the helicity of complex chiral nanomaterials, based on the geometrical properties of a helix. We demonstrate that an analysis at the single particle level can provide significant insights into the origin of chiroptical properties.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000784490000013 Publication Date 2022-03-08  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2639-4979 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor Times cited 11 Open Access OpenAccess  
  Notes S.B. and A.P.-T. gratefully acknowledge funding by the European Research Council (ERC Consolidator Grant #815128-REALNANO) the European Union’s Horizon 2020 research and innovation program under grant agreement #823717ESTEEM3. L.M.L.-M. acknowledges funding from MCIN/ AEI /10.13039/501100011033, grant # PID2020- 117779RB-I00 and the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). G.G.-R. thanks the Spanish Spanish Ministerio de Ciencia e Innovación for an FPI (BES-2014- 068972) fellowship.; SygmaSB; esteem3reported; esteem3jra Approved Most recent IF: NA  
  Call Number EMAT @ emat @c:irua:186959 Serial 6956  
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Author Zhang, Y.; Qin, S.; Claes, N.; Schilling, W.; Sahoo, P.K.; Ching, H.Y.V.; Jaworski, A.; Lemière, F.; Slabon, A.; Van Doorslaer, S.; Bals, S.; Das, S. pdf  url
doi  openurl
  Title Direct Solar Energy-Mediated Synthesis of Tertiary Benzylic Alcohols Using a Metal-Free Heterogeneous Photocatalyst Type A1 Journal article
  Year (down) 2022 Publication ACS Sustainable Chemistry and Engineering Abbreviated Journal Acs Sustain Chem Eng  
  Volume 10 Issue 1 Pages 530-540  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Organic synthesis (ORSY)  
  Abstract Direct hydroxylation via the functionalization of tertiary benzylic C(sp3)-H bond is of great significance for obtaining tertiary alcohols which find wide applications in pharmaceuticals as well as in fine chemical industries. However, current synthetic procedures use toxic reagents and therefore, the development of a sustainable strategy for the synthesis of tertiary benzyl alcohols is highly desirable. To solve this problem, herein, we report a metal-free

heterogeneous photocatalyst to synthesize the hydroxylated products using oxygen as the key reagent. Various benzylic substrates were employed into our mild reaction conditions to afford the desirable products in good to excellent yields. More importantly, gram-scale reaction was achieved via harvesting direct solar energy and exhibited high quantity of the product. The high stability of the catalyst was proved via recycling the catalyst and spectroscopic analyses. Finally, a possible mechanism was proposed based on the EPR and other experimental

evidence.
 
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000736518000001 Publication Date 2022-01-10  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2168-0485 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 8.4 Times cited 24 Open Access OpenAccess  
  Notes We thank BOF joint PhD grant (to Y. Z.), Francqui Foundation and FWO research grant (to S.D.), Chinese Scholarship Council (to Y.Z.). A.S. would like to thank the Swedish Energy Agency for financial support (project nr: 5050-1). The SEM microscope was partly funded by the Hercules Fund from the Flemish Government. Approved Most recent IF: 8.4  
  Call Number EMAT @ emat @c:irua:184744 Serial 6900  
Permanent link to this record
 

 
Author Rogolino, A.; Claes, N.; Cizaurre, J.; Marauri, A.; Jumbo-Nogales, A.; Lawera, Z.; Kruse, J.; Sanroman-Iglesias, M.; Zarketa, I.; Calvo, U.; Jimenez-Izal, E.; Rakovich, Y.P.; Bals, S.; Matxain, J.M.; Grzelczak, M. url  doi
openurl 
  Title Metal-polymer heterojunction in colloidal-phase plasmonic catalysis Type A1 Journal article
  Year (down) 2022 Publication The journal of physical chemistry letters Abbreviated Journal J Phys Chem Lett  
  Volume 13 Issue 10 Pages 2264-2272  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Plasmonic catalysis in the colloidal phase requires robust surface ligands that prevent particles from aggregation in adverse chemical environments and allow carrier flow from reagents to nanoparticles. This work describes the use of a water-soluble conjugated polymer comprising a thiophene moiety as a surface ligand for gold nanoparticles to create a hybrid system that, under the action of visible light, drives the conversion of the biorelevant NAD+ to its highly energetic reduced form NADH. A combination of advanced microscopy techniques and numerical simulations revealed that the robust metal-polymer heterojunction, rich in sulfonate functional groups, directs the interaction of electron-donor molecules with the plasmonic photocatalyst. The tight binding of polymer to the gold surface precludes the need for conventional transition-metal surface cocatalysts, which were previously shown to be essential for photocatalytic NAD(+) reduction but are known to hinder the optical properties of plasmonic nanocrystals. Moreover, computational studies indicated that the coating polymer fosters a closer interaction between the sacrificial electron-donor triethanolamine and the nanoparticles, thus enhancing the reactivity.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000776518000001 Publication Date 0000-00-00  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1948-7185 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 5.7 Times cited 1 Open Access OpenAccess  
  Notes This work was supported by grant PID2019-111772RB-I00 funded by MCIN/AEI/10.13039/501100011033 and grant IT 1254-19 funded by Basque Government. The authors acknowledge the financial support of the European Commission (EUSMI, Grant 731019). S.B. is grateful to the European Research Council (ERC-CoG-2019 815128). The authors acknowledge the contributions by Dr. Adrian Pedrazo Tardajos related to sample support and electron microscopy experiments.; realnano;sygmaSB Approved Most recent IF: 5.7  
  Call Number UA @ admin @ c:irua:188008 Serial 7062  
Permanent link to this record
 

 
Author Walters, A.A.; Santacana-Font, G.; Li, J.; Routabi, N.; Qin, Y.; Claes, N.; Bals, S.; Tzu-Wen Wang, J.; Al-Jamal, K.T. pdf  url
doi  openurl
  Title Nanoparticle-MediatedIn SituMolecular Reprogramming of Immune Checkpoint Interactions for Cancer Immunotherapy Type A1 Journal article
  Year (down) 2021 Publication Acs Nano Abbreviated Journal Acs Nano  
  Volume 15 Issue 11 Pages 17549-17564  
  Keywords A1 Journal article; Pharmacology. Therapy; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Immune checkpoint blockade involves targeting immune

regulatory molecules with antibodies. Preclinically, complex multiantibody

regimes of both inhibitory and stimulatory targets are a promising

candidate for the next generation of immunotherapy. However, in this

setting, the antibody platform may be limited due to excessive toxicity

caused by off target effects as a result of systemic administration. RNA

can be used as an alternate to antibodies as it can both downregulate

immunosuppressive checkpoints (siRNA) or induce expression of

immunostimulatory checkpoints (mRNA). In this study, we demonstrate

that the combination of both siRNA and mRNA in a single

formulation can simultaneously knockdown and induce expression of

immune checkpoint targets, thereby reprogramming the tumor

microenvironment from immunosuppressive to immunostimulatory

phenotype. To achieve this, RNA constructs were synthesized and

formulated into stable nucleic acid lipid nanoparticles (SNALPs); the SNALPs produced were 140−150 nm in size with >80%

loading efficiency. SNALPs could transfect macrophages and B16F10 cells in vitro resulting in 75% knockdown of inhibitory

checkpoint (PDL1) expression and simultaneously express high levels of stimulatory checkpoint (OX40L) with minimal

toxicity. Intratumoral treatment with the proposed formulation resulted in statistically reduced tumor growth, a greater

density of CD4+ and CD8+ infiltrates in the tumor, and immune activation within tumor-draining lymph nodes. These data

suggest that a single RNA-based formulation can successfully reprogram multiple immune checkpoint interactions on a

cellular level. Such a candidate may be able to replace future immune checkpoint therapeutic regimes composed of both

stimulatory- and inhibitory-receptor-targeting antibodies.
 
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000747115200039 Publication Date 2021-11-23  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 11 Open Access OpenAccess  
  Notes A.A.W. is the grateful recipient of a Maplethorpe Fellowship. K.A.J. acknowledges funding from the British Council (Newton Fund, 337313), Wellcome Trust (WT103913), and the Cancer Research UK King’s Health Partners Centre at King’s College London. Financial support is acknowledged from the European Commission under the Horizon 2020 Programme, by means of Grant Agreement No. 731019 (EUSMI). Images were drawn on BioRender.com. Approved Most recent IF: 13.942  
  Call Number EMAT @ emat @c:irua:183950 Serial 6829  
Permanent link to this record
 

 
Author Boschker, H.T.S.; Cook, P.L.M.; Polerecky, L.; Eachambadi, R.T.; Lozano, H.; Hidalgo-Martinez, S.; Khalenkow, D.; Spampinato, V.; Claes, N.; Kundu, P.; Wang, D.; Bals, S.; Sand, K.K.; Cavezza, F.; Hauffman, T.; Bjerg, J.T.; Skirtach, A.G.; Kochan, K.; McKee, M.; Wood, B.; Bedolla, D.; Gianoncelli, A.; Geerlings, N.M.J.; Van Gerven, N.; Remaut, H.; Geelhoed, J.S.; Millan-Solsona, R.; Fumagalli, L.; Nielsen, L.P.; Franquet, A.; Manca, J.V.; Gomila, G.; Meysman, F.J.R. url  doi
openurl 
  Title Efficient long-range conduction in cable bacteria through nickel protein wires Type A1 Journal article
  Year (down) 2021 Publication Nature Communications Abbreviated Journal Nat Commun  
  Volume 12 Issue 1 Pages 3996  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Filamentous cable bacteria display long-range electron transport, generating electrical currents over centimeter distances through a highly ordered network of fibers embedded in their cell envelope. The conductivity of these periplasmic wires is exceptionally high for a biological material, but their chemical structure and underlying electron transport mechanism remain unresolved. Here, we combine high-resolution microscopy, spectroscopy, and chemical imaging on individual cable bacterium filaments to demonstrate that the periplasmic wires consist of a conductive protein core surrounded by an insulating protein shell layer. The core proteins contain a sulfur-ligated nickel cofactor, and conductivity decreases when nickel is oxidized or selectively removed. The involvement of nickel as the active metal in biological conduction is remarkable, and suggests a hitherto unknown form of electron transport that enables efficient conduction in centimeter-long protein structures.  
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  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000669944900006 Publication Date 2021-06-28  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 12.124 Times cited 23 Open Access OpenAccess  
  Notes The authors thank Marlies Neiemeisland for assistance with Raman microscopy, Michiel Kienhuis for assistance with NanoSIMS analysis, Peter Hildebrandt and Diego Millo for helping with the interpretation of the Raman spectra, IONTOF for the Orbitrap Hybrid- SIMS analysis, and Rene Fabregas for helping with finite-element numerical modeling for SDM. H.T.S.B. and F.J.R.M. were financially supported by the Netherlands Organization for Scientific Research (VICI grant 016.VICI.170.072). Research Foundation Flanders supported F.J.R.M., J.V.M., and R.T.E. through FWO grant G031416N, and F.J.R.M. and J.S.G. through FWO grant G038819N. N.M.J.G. is the recipient of a Ph.D. scholarship for teachers from NWO in the Netherlands (grant 023.005.049). The NanoSIMS facility at Utrecht University was financed through a large infrastructure grant by the Netherlands Organization for Scientific Research (NWO, grant no. 175.010.2009.011) and through a Research Infrastructure Fund by the Utrecht University Board. A.G.S. is supported by the Special Research Fund (BOF) of Ghent University (BOF14/IOP/003, BAS094-18, 01IO3618) and FWO (G043219). The ToF-SIMS was funded by FWO Hercules grant (ZW/13/07) to J.V.M. and A.F. H.L., R.M.S., and G.G. were funded by the European Union H2020 Framework Programme (MSCA-ITN-2016) under grant agreement n 721874.EU, the Spanish Agencia Estatal de Investigación and EU FEDER under grant agreements TEC2016-79156-P and TEC2015-72751-EXP, the Generalitat de Catalunya through 2017-SGR1079 grant and CERCA Program. G.G. was recipient of an ICREA Academia Award, and H.L. of a FPI fellowship (BES-2015-074799) from the Agencia Estatal de Investigación/Fondo Social Europeo. L.F. received funding from the European Research Council (grant agreement No. 819417) under the European Union’s Horizon 2020 research and innovation programme. Approved Most recent IF: 12.124  
  Call Number EMAT @ emat @c:irua:179813 Serial 6803  
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Author Reclusa, P.; Verstraelen, P.; Taverna, S.; Gunasekaran, M.; Pucci, M.; Pintelon, I.; Claes, N.; de Miguel-Pérez, D.; Alessandro, R.; Bals, S.; Kaushal, S.; Rolfo, C. pdf  url
doi  openurl
  Title Improving extracellular vesicles visualization: From static to motion Type A1 Journal article
  Year (down) 2020 Publication Scientific Reports Abbreviated Journal Sci Rep-Uk  
  Volume 10 Issue 10 Pages 6494  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract In the last decade extracellular vesicles (EVs) have become a hot topic. The findings on EVs content and effects have made them a major field of interest in cancer research. EVs, are able to be internalized through integrins expressed in parental cells, in a tissue specific manner, as a key step of cancer progression and pre-metastatic niche formation. However, this specificity might lead to new opportunities in cancer treatment by using EVs as devices for drug delivery. For future applications of EVs in cancer, improved protocols and methods for EVs isolation and visualization are required. Our group has put efforts on developing a protocol, able to track the EVs for in vivo internalization analysis. We showed, for the first time, the videos of labeled EVs uptake by living lung cancer cells.  
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  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000562145000002 Publication Date 2020-04-16  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2045-2322 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.6 Times cited 25 Open Access OpenAccess  
  Notes Marzia Pucci is supported by a “AIRC” (Associazione Italiana Ricerca sul Cancro) fellowship. “The Leica SP 8 (Hercules grant AUHA.15.12) microscope was funded by the Hercules Foundation of the Flemish Government.” DdM-P is funded by the University of Granada PhD grant and University of Granada international mobility grant 2018/19. Approved Most recent IF: 4.6; 2020 IF: 4.259  
  Call Number EMAT @ emat @c:irua:169234 Serial 6362  
Permanent link to this record
 

 
Author Cremers, V.; Rampelberg, G.; Baert, K.; Abrahami, S.; Claes, N.; de Oliveira, T.M.; Terryn, H.; Bals, S.; Dendooven, J.; Detavernier, C. pdf  url
doi  openurl
  Title Corrosion protection of Cu by atomic layer deposition Type A1 Journal article
  Year (down) 2019 Publication Journal of vacuum science and technology: A: vacuum surfaces and films Abbreviated Journal J Vac Sci Technol A  
  Volume 37 Issue 37 Pages 060902  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Atomic layer deposition (ALD) is a vapor phase technique that is able to deposit uniform, conformal thin films with an excellent thickness control at the atomic scale. 18 nm thick Al2O3 and TiO2 coatings were deposited conformaly and pinhole-free onto micrometer-sized Cu powder, using trimethylaluminum and tetrakis(dimethylamido)titanium(IV), respectively, as a precursor and de-ionized water as a reactant. The capability of the ALD coating to protect the Cu powder against corrosion was investigated. Therefore, the stability of the coatings was studied in solutions with different pH in the range of 0–14, and in situ raman spectroscopy was used to detect the emergence of corrosion products of Cu as an indication that the protective coating starts to fail. Both ALD coatings provide good protection at standard pH values in the range of 5–7. In general, the TiO2 coating shows a better barrier protection against corrosion than the Al2O3 coating. However, for the most extreme pH conditions, pH 0 and pH 14, the TiO2 coating starts also to degrade.  
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  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000517925800003 Publication Date 2019-09-19  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0734-2101 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 1.374 Times cited 7 Open Access OpenAccess  
  Notes The authors acknowledge financial support from the Strategic Initiative Materials in Flanders (SIM, SBO-FUNC project) and the Special Research Fund BOF of Ghent University (No. GOA 01G01513). J.D. acknowledges the Research Foundation Flanders (FWO-Vlaanderen) for a postdoctoral fellowship. Approved Most recent IF: 1.374  
  Call Number EMAT @ emat @c:irua:162640 Serial 5361  
Permanent link to this record
 

 
Author Asapu, R.; Claes, N.; Ciocarlan, R.-G.; Minjauw, M.; Detavernier, C.; Cool, P.; Bals, S.; Verbruggen, S.W. pdf  url
doi  openurl
  Title Electron Transfer and Near-Field Mechanisms in Plasmonic Gold-Nanoparticle-Modified TiO2Photocatalytic Systems Type A1 Journal article
  Year (down) 2019 Publication ACS applied nano materials Abbreviated Journal ACS Appl. Nano Mater.  
  Volume 2 Issue 2 Pages 4067-4074  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL)  
  Abstract The major mechanism responsible for plasmonic enhancement of titanium dioxide photocatalysis using gold nanoparticles is still under contention. This work introduces an experimental strategy to disentangle the significance of the charge transfer and near-field mechanisms in plasmonic photocatalysis. By controlling the thickness and conductive nature of a nanoparticle shell that acts as a spacer layer separating the plasmonic metal core from the TiO2 surface, field enhancement or charge transfer effects can be selectively repressed or evoked. Layer-by-layer and in situ polymerization methods are used to synthesize gold core–polymer shell nanoparticles with shell thickness control up to the sub-nanometer level. Detailed optical and electrical characterization supported by near-field simulation models corroborate the trends in photocatalytic activity of the different systems. This approach mainly points at an important contribution of the enhanced near field.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000477917700006 Publication Date 2019-05-31  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2574-0970 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor Times cited 32 Open Access OpenAccess  
  Notes This work was supported by Research Foundation Flanders (FWO). P.C. and R-G.C. acknowledge financial support from FWO (Project No. G038215N). N.C. and S.B. acknowledge financial support from the European Research Council (ERC Starting Grant No. 335078-COLOURATOM). Approved Most recent IF: NA  
  Call Number EMAT @ emat @UA @ admin @ c:irua:160579 Serial 5184  
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Author Cremers, V.; Rampelberg, G.; Barhoum, A.; Walters, P.; Claes, N.; Oliveira, T.M. de; Assche, G.V.; Bals, S.; Dendooven, J.; Detavernier, C. pdf  url
doi  openurl
  Title Oxidation barrier of Cu and Fe powder by Atomic Layer Deposition Type A1 Journal article
  Year (down) 2018 Publication Surface and coatings technology Abbreviated Journal Surf Coat Tech  
  Volume 349 Issue 349 Pages 1032-1041  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Atomic layer deposition (ALD) is a vapor based technique which allows to deposit uniform, conformal films with a thickness control at the atomic scale. In this research, Al 2 O 3 coatings were deposited on micrometer-sized Fe and Cu powder (particles) using the thermal trimethylaluminum (TMA)/ water (H 2 O) process in a rotary pump-type ALD reactor. Rotation of the powder during deposition was required to obtain a pinhole-free ALD coating. The protective nature of the coating was evaluated by quantifying its effectiveness in protecting the metal particles during oxidative annealing treatments. The Al 2 O 3 coated powders were annealed in ambient air while in-situ thermogravimetric analysis (TGA) and in-situ x-ray diffraction (XRD) data were acquired. The thermal stability of a series of Cu and Fe powder with different Al 2 O 3 thicknesses were determined with TGA. In both samples a clear shift in oxidation temperature is visible. For Cu and Fe powder coated with 25 nm Al 2 O 3 , we observed an increase of the oxidation temperature with 300-400°C. For the Cu powder a thin film of only 8 nm is required to obtain an initial increase in oxidation temperature of 200°C. In contrast, for Fe powder a thicker coating of 25 nm is required. In both cases, the oxidation temperature increases with increasing thickness of the Al 2 O 3 coating. These results illustrate that the Al 2 O 3 thin film, deposited by the thermal ALD process (TMA/H 2 O) can be an efficient and pinhole-free barrier layer for micrometer-sized powder particles, provided that the powder is properly agitated during the process to ensure sufficient vapour-solid interaction.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000441492600108 Publication Date 2018-06-25  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0257-8972 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 2.589 Times cited 10 Open Access OpenAccess  
  Notes The authors acknowledge financial support from the Strategic Initiative Materials in Flanders (SIM, SBO-FUNC project) and the Special Research Fund BOF of Ghent University (GOA 01G01513). J. D. acknowledges the Research Foundation Flanders (FWO-Vlaanderen) for a postdoctoral fellowship. N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant 335078-COLOURATOMS). The authors acknowledge S. Goeteyn for the assistance in preliminary depositions. (ROMEO:green; preprint:; postprint:can ; pdfversion:cannot); ecas_sara Approved Most recent IF: 2.589  
  Call Number EMAT @ emat @c:irua:152174UA @ admin @ c:irua:152174 Serial 4994  
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Author Claes, N.; Asapu, R.; Blommaerts, N.; Verbruggen, S.W.; Lenaerts, S.; Bals, S. pdf  url
doi  openurl
  Title Characterization of silver-polymer core–shell nanoparticles using electron microscopy Type A1 Journal article
  Year (down) 2018 Publication Nanoscale Abbreviated Journal Nanoscale  
  Volume 10 Issue 10 Pages 9186-9191  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)  
  Abstract Silver-polymer core–shell nanoparticles show interesting optical properties, making them widely applicable in the field of plasmonics. The uniformity, thickness and homogeneity of the polymer shell will affect the properties of the system which makes a thorough structural characterization of these core–shell silver-polymer nanoparticles of great importance. However, visualizing the shell and the particle simultaneously is far from straightforward due to the sensitivity of the polymer shell towards the electron beam. In this study, we use different 2D and 3D electron microscopy techniques to investigate different structural aspects of the polymer coating.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000437007700028 Publication Date 2018-04-16  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 7.367 Times cited 11 Open Access OpenAccess  
  Notes N. C. and S. B. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOMS) and from the FWO through project funding (G038116N). R. A. and S. L. acknowledge the Research Foundation Flanders (FWO) for financial support. (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); ECAS_Sara Approved Most recent IF: 7.367  
  Call Number EMAT @ emat @c:irua:151290UA @ admin @ c:irua:151290 Serial 4959  
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Author Kumar, J.; Eraña, H.; López-Martínez, E.; Claes, N.; Martín, V.F.; Solís, D.M.; Bals, S.; Cortajarena, A.L.; Castilla, J.; Liz-Marzán, L.M. pdf  url
doi  openurl
  Title Detection of amyloid fibrils in Parkinson’s disease using plasmonic chirality Type A1 Journal article
  Year (down) 2018 Publication Proceedings of the National Academy of Sciences of the United States of America Abbreviated Journal P Natl Acad Sci Usa  
  Volume 115 Issue 115 Pages 3225-3230  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Amyloid fibrils, which are closely associated with various neurodegenerative

diseases, are the final products in many protein aggregation pathways. The identification of fibrils at low concentration is, therefore, pivotal in disease diagnosis and development of therapeutic strategies. We report a methodology for the specific identification of amyloid fibrils using chiroptical effects in plasmonic nanoparticles. The formation of amyloid fibrils based on α-synuclein was probed using gold nanorods, which showed no

apparent interaction with monomeric proteins but effective adsorption onto fibril structures via noncovalent interactions. The amyloid structure drives a helical nanorod arrangement, resulting in intense optical activity at the surface plasmon resonance wavelengths. This sensing technique was successfully applied to human brain homogenates of patients affected by Parkinson’s disease,

wherein protein fibrils related to the disease were identified through chiral signals from Au nanorods in the visible and near IR, whereas healthy brain samples did not exhibit any meaningful optical activity. The technique was additionally extended to the specific detection of infectious amyloids formed by prion proteins, thereby confirming the wide potential of the technique. The intense chiral response driven by strong dipolar coupling in helical Au nanorod arrangements allowed us to detect amyloid fibrils down to nanomolar concentrations.
 
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000428382400032 Publication Date 2018-03-12  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0027-8424 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.661 Times cited 187 Open Access OpenAccess  
  Notes We thank Prof. Dr. J.-P. Timmermans and the Antwerp Centre of Advanced Microscopy for providing access to the Tecnai G2 Spirit BioTWIN TEM. We also thank the Basque Biobank (Basque Foundation for Health Innovation and Research, BIOEF) for providing us with Parkinson’s disease-affected brain samples. J.K. acknowledges financial support from the European Commission under Marie Sklodowska-Curie Program H2020- MSCA-IF-2015708321. S.B. and A.L.C. acknowledge European Research Council Grants 335078 COLOURATOM and 648071 ProNANO. S.B. and L.M.L.-M. acknowledge funding from European Commission Grant EUSMI 731019. A.L.C., J.C., and L.M.L.-M. acknowledge funding from Spanish Ministry of Economy and Competitiveness (MINECO) Grants MAT2013-46101- R, AGL2015-65046-C2-1-R, and BIO2016-77367-C2-1-R. (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:restricted); saraecas; ECASSara; Approved Most recent IF: 9.661  
  Call Number EMAT @ emat @c:irua:150355UA @ admin @ c:irua:150355 Serial 4918  
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Author Sánchez-Iglesias, A.; Claes, N.; Solís, D.M.; Taboada, J.M.; Bals, S.; Liz-Marzán, L.M.; Grzelczak, M. pdf  url
doi  openurl
  Title Reversible Clustering of Gold Nanoparticles under Confinement Type A1 Journal article
  Year (down) 2018 Publication Angewandte Chemie: international edition in English Abbreviated Journal Angew Chem Int Edit  
  Volume 57 Issue 57 Pages 3183-3186  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract A limiting factor of solvent-induced nanoparticle self-assembly is the need for constant sample dilution in assembly/disassembly cycles. Changes in the nanoparticle concentration alter the kinetics of the subsequent assembly process, limiting optical signal recovery. Herein, we show that upon confining hydrophobic nanoparticles in permeable silica nanocapsules, the number of nanoparticles participating in cyclic aggregation remains constant despite bulk changes in solution, leading to highly reproducible plasmon band shifts at different solvent compositions.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000426759900031 Publication Date 2018-02-21  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1433-7851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 11.994 Times cited 53 Open Access OpenAccess  
  Notes L.M.L.-M. and M.G. acknowledge funding from the Spanish MINECO (Grant #MAT2013-46101R). N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOM). D.M.S., and J.M.T, acknowledge funding from the European Regional Development Fund (ERDF) and the Spanish MINECO (Projects TEC2017-85376-C2-1-R, TEC2017-85376-C2-2-R), and from the ERDF and the Galician Regional Government under agreement for funding the Atlantic Research Center for Information and Communication Technologies (AtlantTIC). (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); ECAS_Sara Approved Most recent IF: 11.994  
  Call Number EMAT @ emat @c:irua:149558UA @ admin @ c:irua:149558 Serial 4911  
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Author Liao, T.-W.; Verbruggen, S.; Claes, N.; Yadav, A.; Grandjean, D.; Bals, S.; Lievens, P. pdf  url
doi  openurl
  Title TiO2 Films Modified with Au Nanoclusters as Self-Cleaning Surfaces under Visible Light Type A1 Journal article
  Year (down) 2018 Publication Nanomaterials Abbreviated Journal Nanomaterials-Basel  
  Volume 8 Issue 8 Pages 30  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)  
  Abstract In this study, we applied cluster beam deposition (CBD) as a new approach for fabricating efficient plasmon-based photocatalytic materials. Au nanoclusters (AuNCs) produced in the gas phase were deposited on TiO2 P25-coated silicon wafers with coverage ranging from 2 to 8 atomic monolayer (ML) equivalents. Scanning Electron Microscopy (SEM) images of the AuNCs modified TiO2 P25 films show that the surface is uniformly covered by the AuNCs that remain isolated at low coverage (2 ML, 4 ML) and aggregate at higher coverage (8 ML). A clear relationship between AuNCs coverage and photocatalytic activity towards stearic acid photo-oxidation was measured, both under ultraviolet and green light illumination. TiO2 P25 covered with 4 ML AuNCs showed the best stearic acid photo-oxidation performance under green light illumination (Formal Quantum Efficiency 1.6 x 10-6 over a period of 93 h). These results demonstrate the large potential of gas-phase AuNCs beam deposition technology for the fabrication of visible light active plasmonic photocatalysts.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000424131600030 Publication Date 2018-01-08  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2079-4991 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 3.553 Times cited 29 Open Access OpenAccess  
  Notes The research leading to these results has received funding from the European Union’s Seventh Framework Programme (FP7/2007-2013) under grant agreement n 607417 (Catsense). We also thank the Research Foundation—Flanders (FWO, Belgium), the Flemish Concerted Action (BOF KU Leuven, Project No. GOA/14/007) research program, and the microscope was partly funded by the Hercules Fund from the Flemish Government for the support. N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOM). ECAS_Sara (ROMEO:green; preprint:; postprint:can ; pdfversion:can); Approved Most recent IF: 3.553  
  Call Number EMAT @ emat @c:irua:147898UA @ admin @ c:irua:147898 Serial 4805  
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Author Claes, N. url  openurl
  Title 3D characterization of coated nanoparticles and soft-hard nanocomposites Type Doctoral thesis
  Year (down) 2018 Publication Abbreviated Journal  
  Volume Issue Pages  
  Keywords Doctoral thesis; Electron microscopy for materials research (EMAT)  
  Abstract  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Antwerpen Editor  
  Language Wos Publication Date  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN ISBN Additional Links UA library record  
  Impact Factor Times cited Open Access  
  Notes Approved Most recent IF: NA  
  Call Number UA @ lucian @ c:irua:154146 Serial 5075  
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Author Asapu, R.; Ciocarlan, R.-G.; Claes, N.; Blommaerts, N.; Minjauw, M.; Ahmad, T.; Dendooven, J.; Cool, P.; Bals, S.; Denys, S.; Detavernier, C.; Lenaerts, S.; Verbruggen, S.W. pdf  url
doi  openurl
  Title Plasmonic Near-Field Localization of Silver Core–Shell Nanoparticle Assemblies via Wet Chemistry Nanogap Engineering Type A1 Journal article
  Year (down) 2017 Publication ACS applied materials and interfaces Abbreviated Journal Acs Appl Mater Inter  
  Volume 9 Issue 9 Pages 41577-41585  
  Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)  
  Abstract Silver nanoparticles are widely used in the field of plasmonics because of their unique optical properties. The wavelength-dependent surface plasmon resonance gives rise to a strongly enhanced electromagnetic field, especially at so-called hot spots located in the nanogap in-between metal nanoparticle assemblies. Therefore, the interparticle distance is a decisive factor in plasmonic applications, such as surface-enhanced Raman spectroscopy (SERS). In this study, the aim is to engineer this interparticle distance for silver nanospheres using a convenient wet-chemical approach and to predict and quantify the corresponding enhancement factor using both theoretical and experimental tools. This was done by building a tunable ultrathin polymer shell around the nanoparticles using the layer-by-layer method, in which the polymer shell acts as the separating interparticle spacer layer. Comparison of different theoretical approaches and corroborating the results with SERS analytical experiments using silver and silver−polymer core−shell nanoparticle clusters as SERS substrates was also done. Herewith, an approach is provided to estimate the extent of plasmonic near-field enhancement both theoretically as well as experimentally.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000417005900057 Publication Date 2017-11-29  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 7.504 Times cited 29 Open Access OpenAccess  
  Notes financial support through a research fellowship. C.D. wishes to thank the Hercules foundation for the financial support (SPINAL). P.C. and R.-G.C. acknowledge financial support by FWO Vlaanderen (project no. G038215N). N.C. and S.B. acknowledge the financial support from the European Research Council (ERC starting grant #335078-COLOURATOM). (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); saraecas; ECAS_Sara; Approved Most recent IF: 7.504  
  Call Number EMAT @ emat @c:irua:147243 Serial 4804  
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Author Blommaerts, N.; Asapu, R.; Claes, N.; Bals, S.; Lenaerts, S.; Verbruggen, S.W. pdf  url
doi  openurl
  Title Gas phase photocatalytic spiral reactor for fast and efficient pollutant degradation Type A1 Journal article
  Year (down) 2017 Publication Chemical engineering journal Abbreviated Journal Chem Eng J  
  Volume 316 Issue 316 Pages 850-856  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)  
  Abstract Photocatalytic reactors for the degradation of gaseous organic pollutants often suffer from major limitations such as small reaction area, sub-optimal irradiation conditions and thus limited reaction rate. In this work, an alternative solution is presented that involves a glass tube coated on the inside with (silvermodified) TiO2 and spiraled around a UVA lamp. First, the spiral reactor is coated from the inside with TiO2 using an experimentally verified procedure that is optimized toward UV light transmission. This procedure is kept as simple as possible and involves a single casting step of a 1 wt% suspension of TiO2 in ethanol through the spiral. This results in a coated tube that absorbs nearly all incident UV light under the experimental conditions used. The optimized coated spiral reactor is then benchmarked to a conventional annular photoreactor of the same outer dimensions and total catalyst loading over a broad range of experimental conditions. Although residence time distribution experiments indicate slightly longer dwelling of molecules in the spiral reactor, no significant difference in by-passing of gas between the spiral reactor and the annular reactor can be claimed. Acetaldehyde degradation efficiency of 100% is obtained with the spiral reactor for a residence time as low as 60 s, whereas the annular reactor could not achieve full degradation even at 1000 s residence time. In a final case study, addition of long-term stable silver nanoparticles, protected by an ultra-thin polymer shell applied via the layer-by-layer (LbL) method, to the spiral reactor coating is shown to double the degradation efficiency and provides an interesting strategy to cope with higher pollutant concentrations without changing the overall dimensions.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000398985200089 Publication Date 2017-02-08  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 6.216 Times cited 30 Open Access OpenAccess  
  Notes N.B. wishes to thank the University of Antwerp – Belgium for financial support. N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant #335078- COLOURATOM). S.W.V. acknowledges the Research Foundation – Flanders (FWO) for a postdoctoral fellowship. (ROMEO:green; preprint:; postprint:can ; pdfversion:cannot); ecas_sara Approved Most recent IF: 6.216  
  Call Number EMAT @ emat @ c:irua:140925UA @ admin @ c:irua:140925 Serial 4481  
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Author Garzia Trulli, M.; Claes, N.; Pype, J.; Bals, S.; Baert, K.; Terryn, H.; Sardella, E.; Favia, P.; Vanhulsel, A. pdf  url
doi  openurl
  Title Deposition of aminosilane coatings on porous Al2O3microspheres by means of dielectric barrier discharges Type A1 Journal article
  Year (down) 2017 Publication Plasma processes and polymers Abbreviated Journal Plasma Process Polym  
  Volume 14 Issue 14 Pages 1600211  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)  
  Abstract Advances in the synthesis of porous microspheres and in their functionalization are increasing the interest in applications of alumina. This paper deals with coatings plasma deposited from 3-aminopropyltriethoxysilane by means of dielectric barrier discharges on alumina porous microspheres, shaped by a vibrational droplet coagulation technique. Aims of the work are the functionalization of the particles with active amino groups, as well as the evaluation of their surface coverage and of the penetration of the coatings into their pores. A multi-diagnostic approach was used for the chemical/morphological characterization of the particles. It was found that 5 min exposure to plasma discharges promotes the deposition of homogeneous coatings onto the microspheres and within their pores, down to 1 μm.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000410773200003 Publication Date 2017-01-05  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1612-8850 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 2.846 Times cited 8 Open Access OpenAccess  
  Notes The technical assistance of the VITO staff (Materials Dpt.) is gratefully acknowledged, especially D. Havermans, E. Van Hoof, R. Kemps (SEM-EDX), and A. De Wilde (Hg Porosimetry). Drs. S. Mullens and G. Scheltjens are kindly acknowledged for constructive discussions. Strategic Initiative Materials in Flanders (SIM) is gratefully acknowledged for its financial support. This research was carried out in the framework of the SIM-TRAP program (Tools for rational processing of nano-particles: controlling and tailoring nanoparticle based or nanomodified particle based materials). N. Claes and S. Bals acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOM). (ROMEO:white; preprint:; postprint:restricted ; pdfversion:cannot); saraecas; ECAS_Sara; Approved Most recent IF: 2.846  
  Call Number EMAT @ emat @ c:irua:139511UA @ admin @ c:irua:139511 Serial 4342  
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Author Asapu, R.; Claes, N.; Bals, S.; Denys, S.; Detavernier, C.; Lenaerts, S.; Verbruggen, S.W. pdf  url
doi  openurl
  Title Silver-polymer core-shell nanoparticles for ultrastable plasmon-enhanced photocatalysis Type A1 Journal article
  Year (down) 2017 Publication Applied catalysis : B : environmental Abbreviated Journal Appl Catal B-Environ  
  Volume 200 Issue 200 Pages 31-38  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)  
  Abstract Affordable silver-polymer core-shell nanoparticles are prepared using the layer-by-layer (LbL) technique. The metallic silver core is encapsulated with an ultra-thin protective shell that prevents oxidation and clustering without compromising the plasmonic properties. The core-shell nanoparticles retain their plasmonic near field enhancement effect, as studied from finite element numerical simulations. Control over the shell thickness up to the sub-nanometer level is there for key. The particles are used to prepare a plasmonic Ag-TiO2 photocatalyst of which the gas phase photocatalytic activity is monitored over a period of four months. The described system outperforms pristine TiO2 and retains its plasmonic enhancement in contrast to TiO2 modified with bare silver nanoparticles. With this an important step is made toward the development of long-term stable plasmonic (photocatalytic) applications.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000384775600004 Publication Date 2016-06-28  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0926-3373 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.446 Times cited 45 Open Access OpenAccess  
  Notes CD, SL and SWV acknowledge the Research Foundation − Flanders (FWO) for financial support. CD further acknowledges BOF-UGent (GOA 01G01513) and the Hercules Foundation (AUGE/09/014). SB acknowledges the European Research Council for the ERC Starting Grant #335078-COLOURATOM.; ECAS_Sara; (ROMEO:green; preprint:; postprint:can ; pdfversion:cannot); Approved Most recent IF: 9.446  
  Call Number c:irua:134384 c:irua:134384UA @ admin @ c:irua:134384 Serial 4104  
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Author Liu, Y.; Claes, N.; Trepka, B.; Bals, S.; Lang, P.R. pdf  url
doi  openurl
  Title A combined 3D and 2D light scattering study on aqueous colloidal model systems with tunable interactions Type A1 Journal article
  Year (down) 2016 Publication Soft matter Abbreviated Journal Soft Matter  
  Volume 12 Issue 12 Pages 8485-8494  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract In this article we report on the synthesis and characterization of a system of colloidal spheres suspended in an aqueous solvent which can be refractive index-matched, thus allowing for investigations of the particle near-wall dynamics by evanescent wave dynamic light scattering at concentrations up to the isotropic to ordered transition and beyond. The particles are synthesized by copolymerization of a fluorinated acrylic ester monomer with a polyethylene-glycol (PEG) oligomer by surfactant free emulsion polymerization. Static and dynamic light scattering experiments in combination with cryo transmission electron microscopy reveal that the particles have a core shell structure with a significant enrichment of the PEG chains on the particles surface. In index-matching DMSO/water suspensions the particles arrange in an ordered phase at volume fraction above 7%, if no additional electrolyte is present. The near-wall dynamics at low volume fraction are quantitatively described by the combination of electrostatic repulsion and hydrodynamic interaction between the particles and the wall. At volume fractions close to the isotropic to ordered transition, the near-wall dynamics are more complex and qualitatively reminiscent of the behaviour which was observed in hard sphere suspensions at high concentrations.  
  Address Forschugszentrum Julich, Institute of Complex Systems ICS-3, Julich, Germany. p.lang@fz-juelich.de and Heinrich-Heine Universitat, Dusseldorf, Germany  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000386247100004 Publication Date 2016-08-22  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1744-683X ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 3.889 Times cited 2 Open Access OpenAccess  
  Notes The authors thank Prof. J. K. G. Dhont and the ICS-3 group for useful discussions and support. YL would like to thank the Marie Sklodowska Curie Initial Training Network SOMATAI under the EU Grant Agreement No. 316866 for financial support. BT contributed to this work during an internship at Forschungszentrum Ju¨lich supported by the International Helmholtz Research School of Biophysics and Soft Matter (IHRS BioSoft), which is gratefully acknowledged. SB and NC acknowledge financial support from the European Research Council (ERC Starting Grant No. 335078-COLOURATOMS).; ECAS_Sara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); Approved Most recent IF: 3.889  
  Call Number EMAT @ emat @ c:irua:136166 Serial 4292  
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Author Hill, E.H.; Claes, N.; Bals, S.; Liz-Marzán, L.M. pdf  url
doi  openurl
  Title Layered Silicate Clays as Templates for Anisotropic Gold Nanoparticle Growth Type A1 Journal article
  Year (down) 2016 Publication Chemistry of materials Abbreviated Journal Chem Mater  
  Volume 28 Issue 28 Pages 5131-5139  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Clay minerals are abundant natural materials arising in the presence of water and are composed of small particles of different sizes and shapes. The interlamellar space between layered silicate clays can also be used to host a variety of different organic and inorganic guest molecules or particles. Recent studies of clay−metal hybrids formed by impregnation of nanoparticles into the interlayer spaces of the clays have not demonstrated the ability for templated growth following the shape of the particles. Following this line of interest, a method for the synthesis of gold nanoparticles on the synthetic layered silicate clay laponite was developed. This approach can be used to make metal−clay nanoparticles with a variety of morphologies while retaining the molecular adsorption properties of the clay. The surface enhanced Raman scattering enhancement of these particles was also found to be greater than that obtained from other metal nanoparticles of a similar morphology, likely due to increased dye adsorption by the presence of the clay. The hybrid particles presented herein will contribute to further study of plasmonic

sensing, catalysis, dye aggregation, and novel composite materials.
 
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000380576700031 Publication Date 2016-07-02  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.466 Times cited 13 Open Access OpenAccess  
  Notes This work has been supported by the European Research Council (ERC Advanced Grant No. 267867, PLASMAQUO). E.H.H. thanks the Spanish Ministry of Economy and Competitiveness for providing a Juan de la Cierva Fellowship (FJCI-2014-22598). N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOM). We gratefully acknowledge A. B. Serrano-Montes for providing the seed-mediated Au nanostars.; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 9.466  
  Call Number c:irua:135178 c:irua:135178 Serial 4117  
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Author Yuan, R.; Claes, N.; Verheyen, E.; Tuel, A.; Bals, S.; Breynaert, E.; Martens, J.; Kirschhock, C.E.A. pdf  url
doi  openurl
  Title Synthesis of IWW-type germanosilicate zeolite using 5-azonia-spiro[4, 4]nonane as structure directing agent Type A1 Journal article
  Year (down) 2016 Publication New journal of chemistry Abbreviated Journal New J Chem  
  Volume 40 Issue 40 Pages 4319-4324  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract IWW-type zeolite with Si/Ge of 4.9 is obtained using 5-azonia-spiro[4,4]nonane as template in fluoride-free medium under hydrothermal conditions at 175 °C. In an otherwise identical synthesis, using the related 5-azonia-spiro[4,5]decane as structure directing agent, a mixture of IWW and NON zeolite types was formed. In absence of GeO2 from the reactant mixture, pure NON formed. The IWW zeolite was characterized by XRD, SEM, and HRTEM. IWW zeolite displayed a unique morphology and could be calcined at 600 °C without loss of crystallinity. The Si/Ge ratio of the IWW zeolite was increased by postsynthesis modification. Part of the germanium could be eliminated from the as-synthesized IWW zeolite by acid leaching using 6 M HCl solution. Also the calcined material could be degermanated. Here the presence of a silicon source in the acidic leaching solution minimized structural damage. This way the Si/Ge ratio of the IWW zeolite was increased from 4.9 up to 10.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000375586400038 Publication Date 2016-02-19  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1144-0546 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 3.269 Times cited 8 Open Access OpenAccess  
  Notes The authors acknowledge FWO/NWO and ESRF for providing beam time at the DUBBLE and SNBL beamlines (ESRF, Grenoble) and P. Abdala for her assistance during the use of the beamline. The authors are grateful to L. Van Tendeloo for taking SEM images. I. Cuppens and K. Houthoofd are thanked for the ICP and AAS measurements. R.Y. acknowledges Chinese Scholarship Council for a CSC doctoral fellowship. JAM and CEAK acknowledge the Flemish government for long-term structural funding (Methusalem). N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOMS).; ECAS_Sara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); Approved Most recent IF: 3.269  
  Call Number c:irua:133671 Serial 4027  
Permanent link to this record
 

 
Author Percebom, A.M.M.; Giner-casares, J.J.; Claes, N.; Bals, S.; Loh, W.; Liz-Marzan, L.M. pdf  url
doi  openurl
  Title Janus Gold Nanoparticles Obtained via Spontaneous Binary Polymer Shell Segregation Type A1 Journal article
  Year (down) 2016 Publication Chemical communications Abbreviated Journal Chem Commun  
  Volume 52 Issue 52 Pages 4278-4281  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Janus gold nanoparticles are of high interest because they allow directed self-assembly and display plasmonic properties. We succeeded in coating gold nanoparticles with two different polymers that form a Janus shell. The spontaneous segregation of two immiscible polymers at the surface of the nanoparticles was verified by NOESY NMR and most importantly by electron microscopy analysis in two and three dimensions. The Janus structure is additionally shown to affect the aggregation behavior of the nanoparticles.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000372176500003 Publication Date 2016-02-09  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1359-7345 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 6.319 Times cited 44 Open Access OpenAccess  
  Notes Funding is acknowledged from the European Research Council (ERC Advanced Grant #267867 Plasmaquo, and ERC Starting Grant #335078 Colouratom). A.M.P. thanks the Brazilian FAPESP for financial support (FAPESP 2012/21930-3 and 2014/01807-8) and J.J. G.-C. acknowledges the Spanish MINECO for a Juan de la Cierva fellowship (#JCI-2012-12517). We thank Ada Herrero Ruiz and Daniel Padró for help with NMR measurements, Malou Henriksen for cell experiments and the Brazilian Synchrotron Laboratory (LNLS) for allocation of SAXS beamtime.; ECAS_Sara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); Approved Most recent IF: 6.319  
  Call Number c:irua:133168 Serial 4009  
Permanent link to this record
 

 
Author De Schouwer, F.; Claes, L.; Claes, N.; Bals, S.; Degrève, J.; De Vos, D.E. pdf  url
doi  openurl
  Title Pd-catalyzed decarboxylation of glutamic acid and pyroglutamic acid to bio-based 2-pyrrolidone Type A1 Journal article
  Year (down) 2015 Publication Green chemistry : cutting-edge research for a greener sustainable future Abbreviated Journal Green Chem  
  Volume 17 Issue 17 Pages 2263-2270  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract In order to recycle nitrogen from nitrogen-rich waste streams, particularly protein waste, we studied the decarboxylation of pyroglutamic acid and glutamic acid in a one-pot reaction to bio-based 2-pyrrolidone. After the screening of a wide range of supported Pd and Pt catalysts, 5 wt% Pd/Al2O3 displayed the highest yield (70%) and selectivity (81%) for the decarboxylation of pyroglutamic acid in water at 250 °C and under an inert atmosphere. Side products originate from consecutive reactions of 2-pyrrolidone; different reaction pathways are proposed to explain the presence of degradation products like propionic acid, γ-hydroxybutyric acid, γ-butyrolactone and methylamine. An extensive study of the reaction parameters was performed to check their influence on selectivity and conversion. This heterogeneous catalytic system was successfully extended to the conversion of glutamic acid.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication London Editor  
  Language Wos 000352724200027 Publication Date 2015-02-17  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1463-9262;1463-9270; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.125 Times cited 47 Open Access OpenAccess  
  Notes 335078 Colouratom; ECAS_Sara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); Approved Most recent IF: 9.125; 2015 IF: 8.020  
  Call Number c:irua:125378 Serial 2564  
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