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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  <identifier identifierType="URL">https://zenodo.org/record/1405554</identifier>
  <creators>
    <creator>
      <creatorName>Kochergin, Yaroslav S.</creatorName>
      <givenName>Yaroslav S.</givenName>
      <familyName>Kochergin</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-9060-6350</nameIdentifier>
      <affiliation>Charles University in Prague</affiliation>
    </creator>
    <creator>
      <creatorName>Schwarz, Dana</creatorName>
      <givenName>Dana</givenName>
      <familyName>Schwarz</familyName>
      <affiliation>Charles University in Prague</affiliation>
    </creator>
    <creator>
      <creatorName>Acharjya, Amitava</creatorName>
      <givenName>Amitava</givenName>
      <familyName>Acharjya</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-0998-171X</nameIdentifier>
      <affiliation>Technische Universität Berlin</affiliation>
    </creator>
    <creator>
      <creatorName>Ichangi, Arun</creatorName>
      <givenName>Arun</givenName>
      <familyName>Ichangi</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-3094-4331</nameIdentifier>
      <affiliation>Institute of Organic Chemistry and Biochemistry of the CAS</affiliation>
    </creator>
    <creator>
      <creatorName>Kulkarni, Ranjit</creatorName>
      <givenName>Ranjit</givenName>
      <familyName>Kulkarni</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-8251-1407</nameIdentifier>
      <affiliation>Humboldt-Universität zu Berlin</affiliation>
    </creator>
    <creator>
      <creatorName>Eliášová, Pavla</creatorName>
      <givenName>Pavla</givenName>
      <familyName>Eliášová</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-9473-8414</nameIdentifier>
      <affiliation>Charles University in Prague</affiliation>
    </creator>
    <creator>
      <creatorName>Vacek, Jaroslav</creatorName>
      <givenName>Jaroslav</givenName>
      <familyName>Vacek</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-2610-4444</nameIdentifier>
      <affiliation>Institute of Organic Chemistry and Biochemistry of the CAS</affiliation>
    </creator>
    <creator>
      <creatorName>Schmidt, Johannes</creatorName>
      <givenName>Johannes</givenName>
      <familyName>Schmidt</familyName>
      <affiliation>Technische Universität Berlin</affiliation>
    </creator>
    <creator>
      <creatorName>Thomas, Arne</creatorName>
      <givenName>Arne</givenName>
      <familyName>Thomas</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-2130-4930</nameIdentifier>
      <affiliation>Technische Universität Berlin</affiliation>
    </creator>
    <creator>
      <creatorName>Bojdys, Michael J.</creatorName>
      <givenName>Michael J.</givenName>
      <familyName>Bojdys</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-2592-4168</nameIdentifier>
      <affiliation>Humboldt-Universität zu Berlin</affiliation>
    </creator>
  </creators>
  <titles>
    <title>Exploring the "Goldilocks Zone" of Semiconducting Polymer Photocatalysts via Donor-Acceptor Interactions</title>
  </titles>
  <publisher>Zenodo</publisher>
  <publicationYear>2018</publicationYear>
  <subjects>
    <subject>conjugated microporous polymers</subject>
    <subject>donor-acceptor systems</subject>
    <subject>fluorescence sensing</subject>
    <subject>photocatalysis</subject>
    <subject>triazine</subject>
  </subjects>
  <dates>
    <date dateType="Issued">2018-08-28</date>
  </dates>
  <resourceType resourceTypeGeneral="Text">Journal article</resourceType>
  <alternateIdentifiers>
    <alternateIdentifier alternateIdentifierType="url">https://zenodo.org/record/1405554</alternateIdentifier>
  </alternateIdentifiers>
  <relatedIdentifiers>
    <relatedIdentifier relatedIdentifierType="DOI" relationType="IsIdenticalTo">10.1002/anie.201809702</relatedIdentifier>
  </relatedIdentifiers>
  <rightsList>
    <rights rightsURI="https://creativecommons.org/licenses/by-sa/4.0/legalcode">Creative Commons Attribution Share Alike 4.0 International</rights>
    <rights rightsURI="info:eu-repo/semantics/openAccess">Open Access</rights>
  </rightsList>
  <descriptions>
    <description descriptionType="Abstract">&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;</description>
  </descriptions>
  <fundingReferences>
    <fundingReference>
      <funderName>European Commission</funderName>
      <funderIdentifier funderIdentifierType="Crossref Funder ID">10.13039/501100000780</funderIdentifier>
      <awardNumber awardURI="info:eu-repo/grantAgreement/EC/H2020/678462/">678462</awardNumber>
      <awardTitle>Layered functional materials - beyond 'graphene'</awardTitle>
    </fundingReference>
  </fundingReferences>
</resource>
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