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  1. AU=van Turnhout Lars
  2. AU="Wondergem, Maurits"
  3. AU="Arazi-Caillaud, Solange"
  4. AU="Lindner, Ariel"
  5. AU="Nawarskas, James"
  6. AU="Uluorman, Funda"
  7. AU="J.D.Callaghan, "
  8. AU="Villegas Arenas, Dolly"
  9. AU="Brown, Jared"
  10. AU="Yasuharu Tokuda"
  11. AU="Kiviharju, Elina"
  12. AU="Gromov, Anton"

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  1. Artikel ; Online: Aza-Cibalackrot: Turning on Singlet Fission Through Crystal Engineering.

    Purdy, Michael / Walton, Jessica R / Fallon, Kealan J / Toolan, Daniel T W / Budden, Peter / Zeng, Weixuan / Corpinot, Merina K / Bučar, Dejan-Krešimir / van Turnhout, Lars / Friend, Richard / Rao, Akshay / Bronstein, Hugo

    Journal of the American Chemical Society

    2023  Band 145, Heft 19, Seite(n) 10712–10720

    Abstract: Singlet fission is a photophysical process that provides a pathway for more efficient harvesting of solar energy in photovoltaic devices. The design of singlet fission candidates is non-trivial and requires careful optimization of two key criteria: (1) ... ...

    Abstract Singlet fission is a photophysical process that provides a pathway for more efficient harvesting of solar energy in photovoltaic devices. The design of singlet fission candidates is non-trivial and requires careful optimization of two key criteria: (1) correct energetic alignment and (2) appropriate intermolecular coupling. Meanwhile, this optimization must not come at the cost of molecular stability or feasibility for device applications. Cibalackrot is a historic and stable organic dye which, although it has been suggested to have ideal energetics, does not undergo singlet fission due to large interchromophore distances, as suggested by single crystal analysis. Thus, while the energetic alignment is satisfactory, the molecule does not have the desired intermolecular coupling. Herein, we improve this characteristic through molecular engineering with the first synthesis of an aza-cibalackrot and show, using ultrafast transient spectroscopy, that singlet fission is successfully "turned on."
    Sprache Englisch
    Erscheinungsdatum 2023-05-03
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.3c00971
    Datenquelle MEDical Literature Analysis and Retrieval System OnLINE

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  2. Artikel ; Online: Direct Observation of a Plasmon-Induced Hot Electron Flow in a Multimetallic Nanostructure.

    van Turnhout, Lars / Hattori, Yocefu / Meng, Jie / Zheng, Kaibo / Sá, Jacinto

    Nano letters

    2020  Band 20, Heft 11, Seite(n) 8220–8228

    Abstract: Plasmon hot carriers are interesting for photoredox chemical synthesis but their direct utilization is limited by their ultrafast thermalization. Therefore, they are often transferred to suitable accepting materials that expedite their lifetime. Solid- ... ...

    Abstract Plasmon hot carriers are interesting for photoredox chemical synthesis but their direct utilization is limited by their ultrafast thermalization. Therefore, they are often transferred to suitable accepting materials that expedite their lifetime. Solid-state photocatalysts are technologically more suitable than their molecular counterparts, but their photophysical processes are harder to follow due to the absence of clear optical fingerprints. Herein, the journey of hot electrons in a solid-state multimetallic photocatalyst is revealed by a combination of ultrafast visible and infrared spectroscopy. Dynamics showed that electrons formed upon silver plasmonic excitation reach the gold catalytic site within 700 fs and the electron flow could also be reversed. Gold is the preferred site until saturation of its 5d band occurs. Silver-plasmon hot electrons increased the rate of nitrophenol reduction 16-fold, confirming the preponderant role of hot electrons in the overall catalytic activity and the importance to follow hot carriers' journeys in solid-state photosystems.
    Schlagwörter covid19
    Sprache Englisch
    Erscheinungsdatum 2020-10-23
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ISSN 1530-6992
    ISSN (online) 1530-6992
    DOI 10.1021/acs.nanolett.0c03344
    Datenquelle MEDical Literature Analysis and Retrieval System OnLINE

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  3. Artikel ; Online: Ketone Synthesis by a Nickel-Catalyzed Dehydrogenative Cross-Coupling of Primary Alcohols.

    Verheyen, Thomas / van Turnhout, Lars / Vandavasi, Jaya Kishore / Isbrandt, Eric S / De Borggraeve, Wim M / Newman, Stephen G

    Journal of the American Chemical Society

    2019  Band 141, Heft 17, Seite(n) 6869–6874

    Abstract: An intermolecular coupling of primary alcohols and organotriflates has been developed to provide ketones by the action of a Ni(0) catalyst. This oxidative transformation is proposed to occur by the union of three distinct catalytic cycles. Two ... ...

    Abstract An intermolecular coupling of primary alcohols and organotriflates has been developed to provide ketones by the action of a Ni(0) catalyst. This oxidative transformation is proposed to occur by the union of three distinct catalytic cycles. Two competitive oxidation processes generate aldehyde in situ via hydrogen transfer oxidation or (pseudo)dehalogenation pathways. As aldehyde forms, a Ni-catalyzed carbonyl-Heck process enables formation of the key carbon-carbon bond. The utility of this rare alcohol to ketone transformation is demonstrated through the synthesis of diverse complex and bioactive molecules.
    Sprache Englisch
    Erscheinungsdatum 2019-04-18
    Erscheinungsland United States
    Dokumenttyp Journal Article ; Research Support, Non-U.S. Gov't
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.9b03280
    Datenquelle MEDical Literature Analysis and Retrieval System OnLINE

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  4. Artikel ; Online: An automated real-time microfluidic platform to probe single NK cell heterogeneity and cytotoxicity on-chip.

    Subedi, Nikita / Van Eyndhoven, Laura C / Hokke, Ayla M / Houben, Lars / Van Turnhout, Mark C / Bouten, Carlijn V C / Eyer, Klaus / Tel, Jurjen

    Scientific reports

    2021  Band 11, Heft 1, Seite(n) 17084

    Abstract: Cytotoxicity is a vital effector mechanism used by immune cells to combat pathogens and cancer cells. While conventional cytotoxicity assays rely on averaged end-point measures, crucial insights on the dynamics and heterogeneity of effector and target ... ...

    Abstract Cytotoxicity is a vital effector mechanism used by immune cells to combat pathogens and cancer cells. While conventional cytotoxicity assays rely on averaged end-point measures, crucial insights on the dynamics and heterogeneity of effector and target cell interactions cannot be extracted, emphasizing the need for dynamic single-cell analysis. Here, we present a fully automated droplet-based microfluidic platform that allowed the real-time monitoring of effector-target cell interactions and killing, allowing the screening of over 60,000 droplets identifying 2000 individual cellular interactions monitored over 10 h. During the course of incubation, we observed that the dynamics of cytotoxicity within the Natural Killer (NK) cell population varies significantly over the time. Around 20% of the total NK cells in droplets showed positive cytotoxicity against paired K562 cells, most of which was exhibited within first 4 h of cellular interaction. Using our single cell analysis platform, we demonstrated that the population of NK cells is composed of individual cells with different strength in their effector functions, a behavior masked in conventional studies. Moreover, the versatility of our platform will allow the dynamic and resolved study of interactions between immune cell types and the finding and characterization of functional sub-populations, opening novel ways towards both fundamental and translational research.
    Mesh-Begriff(e) Automation, Laboratory/methods ; Cells, Cultured ; Cytotoxicity, Immunologic ; Humans ; K562 Cells ; Killer Cells, Natural/immunology ; Lab-On-A-Chip Devices ; Microfluidics/methods ; Single-Cell Analysis/methods
    Sprache Englisch
    Erscheinungsdatum 2021-08-24
    Erscheinungsland England
    Dokumenttyp Journal Article ; Research Support, Non-U.S. Gov't
    ZDB-ID 2615211-3
    ISSN 2045-2322 ; 2045-2322
    ISSN (online) 2045-2322
    ISSN 2045-2322
    DOI 10.1038/s41598-021-96609-9
    Datenquelle MEDical Literature Analysis and Retrieval System OnLINE

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  5. Artikel ; Online: An automated real-time microfluidic platform to probe single NK cell heterogeneity and cytotoxicity on-chip

    Nikita Subedi / Laura C. Van Eyndhoven / Ayla M. Hokke / Lars Houben / Mark C. Van Turnhout / Carlijn V. C. Bouten / Klaus Eyer / Jurjen Tel

    Scientific Reports, Vol 11, Iss 1, Pp 1-

    2021  Band 11

    Abstract: Abstract Cytotoxicity is a vital effector mechanism used by immune cells to combat pathogens and cancer cells. While conventional cytotoxicity assays rely on averaged end-point measures, crucial insights on the dynamics and heterogeneity of effector and ... ...

    Abstract Abstract Cytotoxicity is a vital effector mechanism used by immune cells to combat pathogens and cancer cells. While conventional cytotoxicity assays rely on averaged end-point measures, crucial insights on the dynamics and heterogeneity of effector and target cell interactions cannot be extracted, emphasizing the need for dynamic single-cell analysis. Here, we present a fully automated droplet-based microfluidic platform that allowed the real-time monitoring of effector-target cell interactions and killing, allowing the screening of over 60,000 droplets identifying 2000 individual cellular interactions monitored over 10 h. During the course of incubation, we observed that the dynamics of cytotoxicity within the Natural Killer (NK) cell population varies significantly over the time. Around 20% of the total NK cells in droplets showed positive cytotoxicity against paired K562 cells, most of which was exhibited within first 4 h of cellular interaction. Using our single cell analysis platform, we demonstrated that the population of NK cells is composed of individual cells with different strength in their effector functions, a behavior masked in conventional studies. Moreover, the versatility of our platform will allow the dynamic and resolved study of interactions between immune cell types and the finding and characterization of functional sub-populations, opening novel ways towards both fundamental and translational research.
    Schlagwörter Medicine ; R ; Science ; Q
    Thema/Rubrik (Code) 612
    Sprache Englisch
    Erscheinungsdatum 2021-08-01T00:00:00Z
    Verlag Nature Portfolio
    Dokumenttyp Artikel ; Online
    Datenquelle BASE - Bielefeld Academic Search Engine (Lebenswissenschaftliche Auswahl)

    Volltext online

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  6. Artikel: Ketone Synthesis by a Nickel-Catalyzed Dehydrogenative Cross-Coupling of Primary Alcohols

    Verheyen, Thomas / van Turnhout, Lars / Vandavasi, Jaya Kishore / Isbrandt, Eric S / De Borggraeve, Wim M / Newman, Stephen G

    Journal of the American Chemical Society. 2019 Apr. 15, v. 141, no. 17

    2019  

    Abstract: An intermolecular coupling of primary alcohols and organotriflates has been developed to provide ketones by the action of a Ni(0) catalyst. This oxidative transformation is proposed to occur by the union of three distinct catalytic cycles. Two ... ...

    Abstract An intermolecular coupling of primary alcohols and organotriflates has been developed to provide ketones by the action of a Ni(0) catalyst. This oxidative transformation is proposed to occur by the union of three distinct catalytic cycles. Two competitive oxidation processes generate aldehyde in situ via hydrogen transfer oxidation or (pseudo)dehalogenation pathways. As aldehyde forms, a Ni-catalyzed carbonyl-Heck process enables formation of the key carbon–carbon bond. The utility of this rare alcohol to ketone transformation is demonstrated through the synthesis of diverse complex and bioactive molecules.
    Schlagwörter bioactive compounds ; catalysts ; chemical bonding ; cross-coupling reactions ; dehalogenation ; dehydrogenation ; hydrogen ; ketones ; nickel ; oxidation
    Sprache Englisch
    Erscheinungsverlauf 2019-0415
    Umfang p. 6869-6874.
    Erscheinungsort American Chemical Society
    Dokumenttyp Artikel
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.9b03280
    Datenquelle NAL Katalog (AGRICOLA)

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  7. Artikel: Immobilization of [VCl₃(N-2,6-Me₂C₆H₃)] Complex on Silica Supports: Synthesis and Catalytic Testing for Ethylene Polymerization

    Fiorentino, Antonio / Panariti, Persi / van Turnhout, Lars / Spronck, Mitch / Klein, Axel / Schmitz, Simon / Rastogi, Sanjay / Blom, Burgert / Romano, Dario

    Industrial & engineering chemistry process design and development. 2020 June 19, v. 59, no. 28

    2020  

    Abstract: The heterogenization of 2,6-dimethylarylimido–vanadium(V) dichloride via chemical tethering on insoluble silica supports is reported. The effects of the silica particle size, drying conditions, and the reaction time were investigated. The drying ... ...

    Abstract The heterogenization of 2,6-dimethylarylimido–vanadium(V) dichloride via chemical tethering on insoluble silica supports is reported. The effects of the silica particle size, drying conditions, and the reaction time were investigated. The drying conditions of the support were found to be a crucial parameter: drying temperatures over 400 °C were needed to achieve successful catalysis. The supported catalytic systems were characterized by Fourier-transform infrared (FT-IR) spectroscopy, transmission electron microscopy–energy-dispersive X-ray (TEM-EDX), and inductively coupled plasma mass spectroscopy (ICP-MS), while the polymers were characterized by FT-IR, differential scanning calorimetry (DSC), and rheology. Ethylene polymerization tests were performed employing the prepared heterogenized catalysts with methylaluminoxane/diethylaluminum chloride as a cocatalyst. The supported catalyst precursor, when activated with diethylaluminum chloride, promotes the synthesis of polyethylene with seemingly controlled particle size in the absence of reactor fouling, suggesting the successful immobilization of the complex over the inert support. The resulting polymer shows features of ultrahigh-molecular-weight polyethylene (UHMWPE). These findings present a proof-of-concept for a new approach toward the heterogenization of arylimido–vanadium complexes.
    Schlagwörter X-radiation ; catalysts ; catalytic activity ; chlorides ; ethylene ; mass spectrometry ; particle size ; polyethylene ; polymerization ; process design ; rheology ; silica
    Sprache Englisch
    Erscheinungsverlauf 2020-0619
    Umfang p. 12710-12718.
    Erscheinungsort American Chemical Society
    Dokumenttyp Artikel
    Anmerkung NAL-AP-2-clean
    ZDB-ID 1484436-9
    ISSN 1520-5045 ; 0888-5885
    ISSN (online) 1520-5045
    ISSN 0888-5885
    DOI 10.1021/acs.iecr.0c01908
    Datenquelle NAL Katalog (AGRICOLA)

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