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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    <subfield code="a">&lt;p&gt;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 &amp;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&amp;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&amp;nbsp;eV using Stille coupling. These polymers combine &amp;pi;-conjugated electron-withdrawing triazine- (C&lt;sub&gt;3&lt;/sub&gt;N&lt;sub&gt;3&lt;/sub&gt;) 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&lt;sub&gt;2&lt;/sub&gt; gas from water under visible light irradiation with hydrogen evolution rates up to 3158&amp;nbsp;&amp;micro;mol&amp;nbsp;h&lt;sup&gt;-1&lt;/sup&gt;&amp;nbsp;g&lt;sup&gt;-1&lt;/sup&gt; 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.&lt;/p&gt;</subfield>
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    <subfield code="u">Charles University in Prague</subfield>
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