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Exploring the "Goldilocks Zone" of Semiconducting Polymer Photocatalysts via Donor-Acceptor Interactions

Kochergin, Yaroslav S.; Schwarz, Dana; Acharjya, Amitava; Ichangi, Arun; Kulkarni, Ranjit; Eliášová, Pavla; Vacek, Jaroslav; Schmidt, Johannes; Thomas, Arne; Bojdys, Michael J.


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{
  "description": "<p>Water splitting using polymer photocatalysts is a key technology to a truly sustainable hydrogen-based energy economy. Synthetic chemists have intuitively tried to enhance photocatalytic activity by tuning the length of &pi;-conjugated domains of their semiconducting polymers, but the increasing flexibility and hydrophobicity of ever-larger organic building blocks leads to adverse effects such as structural collapse and inaccessible catalytic sites. To reach the ideal optical bandgap of ~2.3&nbsp;eV, we synthesised a library of eight sulphur and nitrogen containing porous polymers (SNPs) with similar geometries but with optical bandgaps ranging from 2.07 to 2.60&nbsp;eV using Stille coupling. These polymers combine &pi;-conjugated electron-withdrawing triazine- (C<sub>3</sub>N<sub>3</sub>) and electron donating, sulphur-containing moieties as covalently-bonded donor-acceptor frameworks with permanent porosity. The remarkable optical properties of SNPs enable fluorescence on-off sensing of volatile organic compounds and illustrate intrinsic charge-transfer effects. Moreover, obtained polymers effectively evolve H<sub>2</sub> gas from water under visible light irradiation with hydrogen evolution rates up to 3158&nbsp;&micro;mol&nbsp;h<sup>-1</sup>&nbsp;g<sup>-1</sup> and high apparent quantum efficiency which is the highest value obtained for microporous organic polymers to-date. The design principles demonstrated here are transferable to a new field of high-performance polymer photocatalysts based on efficient donor-acceptor dyads.</p>", 
  "license": "https://creativecommons.org/licenses/by-sa/4.0/legalcode", 
  "creator": [
    {
      "affiliation": "Charles University in Prague", 
      "@id": "https://orcid.org/0000-0002-9060-6350", 
      "@type": "Person", 
      "name": "Kochergin, Yaroslav S."
    }, 
    {
      "affiliation": "Charles University in Prague", 
      "@type": "Person", 
      "name": "Schwarz, Dana"
    }, 
    {
      "affiliation": "Technische Universit\u00e4t Berlin", 
      "@id": "https://orcid.org/0000-0002-0998-171X", 
      "@type": "Person", 
      "name": "Acharjya, Amitava"
    }, 
    {
      "affiliation": "Institute of Organic Chemistry and Biochemistry of the CAS", 
      "@id": "https://orcid.org/0000-0002-3094-4331", 
      "@type": "Person", 
      "name": "Ichangi, Arun"
    }, 
    {
      "affiliation": "Humboldt-Universit\u00e4t zu Berlin", 
      "@id": "https://orcid.org/0000-0002-8251-1407", 
      "@type": "Person", 
      "name": "Kulkarni, Ranjit"
    }, 
    {
      "affiliation": "Charles University in Prague", 
      "@id": "https://orcid.org/0000-0002-9473-8414", 
      "@type": "Person", 
      "name": "Eli\u00e1\u0161ov\u00e1, Pavla"
    }, 
    {
      "affiliation": "Institute of Organic Chemistry and Biochemistry of the CAS", 
      "@id": "https://orcid.org/0000-0002-2610-4444", 
      "@type": "Person", 
      "name": "Vacek, Jaroslav"
    }, 
    {
      "affiliation": "Technische Universit\u00e4t Berlin", 
      "@type": "Person", 
      "name": "Schmidt, Johannes"
    }, 
    {
      "affiliation": "Technische Universit\u00e4t Berlin", 
      "@id": "https://orcid.org/0000-0002-2130-4930", 
      "@type": "Person", 
      "name": "Thomas, Arne"
    }, 
    {
      "affiliation": "Humboldt-Universit\u00e4t zu Berlin", 
      "@id": "https://orcid.org/0000-0002-2592-4168", 
      "@type": "Person", 
      "name": "Bojdys, Michael J."
    }
  ], 
  "headline": "Exploring the \"Goldilocks Zone\" of Semiconducting Polymer Photocatalysts via Donor-Acceptor Interactions", 
  "image": "https://zenodo.org/static/img/logos/zenodo-gradient-round.svg", 
  "datePublished": "2018-08-28", 
  "url": "https://zenodo.org/record/1405554", 
  "keywords": [
    "conjugated microporous polymers", 
    "donor-acceptor systems", 
    "fluorescence sensing", 
    "photocatalysis", 
    "triazine"
  ], 
  "@context": "https://schema.org/", 
  "identifier": "https://doi.org/10.1002/anie.201809702", 
  "@id": "https://doi.org/10.1002/anie.201809702", 
  "@type": "ScholarlyArticle", 
  "name": "Exploring the \"Goldilocks Zone\" of Semiconducting Polymer Photocatalysts via Donor-Acceptor Interactions"
}
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