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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<oai_dc:dc xmlns:dc="" xmlns:oai_dc="" xmlns:xsi="" xsi:schemaLocation="">
  <dc:creator>Kochergin, Yaroslav S.</dc:creator>
  <dc:creator>Schwarz, Dana</dc:creator>
  <dc:creator>Acharjya, Amitava</dc:creator>
  <dc:creator>Ichangi, Arun</dc:creator>
  <dc:creator>Kulkarni, Ranjit</dc:creator>
  <dc:creator>Eliášová, Pavla</dc:creator>
  <dc:creator>Vacek, Jaroslav</dc:creator>
  <dc:creator>Schmidt, Johannes</dc:creator>
  <dc:creator>Thomas, Arne</dc:creator>
  <dc:creator>Bojdys, Michael J.</dc:creator>
  <dc:description>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 π-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 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 eV using Stille coupling. These polymers combine π-conjugated electron-withdrawing triazine- (C3N3) 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 H2 gas from water under visible light irradiation with hydrogen evolution rates up to 3158 µmol h-1 g-1 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.</dc:description>
  <dc:subject>conjugated microporous polymers</dc:subject>
  <dc:subject>donor-acceptor systems</dc:subject>
  <dc:subject>fluorescence sensing</dc:subject>
  <dc:title>Exploring the "Goldilocks Zone" of Semiconducting Polymer Photocatalysts via Donor-Acceptor Interactions</dc:title>
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