Journal article Open Access

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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{
  "DOI": "10.1002/anie.201809702", 
  "author": [
    {
      "family": "Kochergin, Yaroslav S."
    }, 
    {
      "family": "Schwarz, Dana"
    }, 
    {
      "family": "Acharjya, Amitava"
    }, 
    {
      "family": "Ichangi, Arun"
    }, 
    {
      "family": "Kulkarni, Ranjit"
    }, 
    {
      "family": "Eli\u00e1\u0161ov\u00e1, Pavla"
    }, 
    {
      "family": "Vacek, Jaroslav"
    }, 
    {
      "family": "Schmidt, Johannes"
    }, 
    {
      "family": "Thomas, Arne"
    }, 
    {
      "family": "Bojdys, Michael J."
    }
  ], 
  "issued": {
    "date-parts": [
      [
        2018, 
        8, 
        28
      ]
    ]
  }, 
  "abstract": "<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>", 
  "title": "Exploring the \"Goldilocks Zone\" of Semiconducting Polymer Photocatalysts via Donor-Acceptor Interactions", 
  "type": "article-journal", 
  "id": "1405554"
}
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