Journal article Open Access
Schwarz, Dana;
Acharjya, Amitava;
Ichangi, Arun;
Kochergin, Yaroslav;
Lyu, Pengbo;
Opanasenko, Maksym V.;
Tarábek, Jan;
Vacek Chocholoušová, Jana;
Vacek, Jaroslav;
Schmidt, Johannes;
Nachtigall, Petr;
Thomas, Arne;
Bojdys, Michael J.
<?xml version='1.0' encoding='UTF-8'?> <record xmlns="http://www.loc.gov/MARC21/slim"> <leader>00000nam##2200000uu#4500</leader> <datafield tag="540" ind1=" " ind2=" "> <subfield code="u">https://creativecommons.org/licenses/by-nc-nd/4.0/legalcode</subfield> <subfield code="a">Creative Commons Attribution Non Commercial No Derivatives 4.0 International</subfield> </datafield> <datafield tag="260" ind1=" " ind2=" "> <subfield code="c">2018-10-18</subfield> </datafield> <controlfield tag="005">20200120174142.0</controlfield> <controlfield tag="001">1471618</controlfield> <datafield tag="909" ind1="C" ind2="O"> <subfield code="p">openaire</subfield> <subfield code="o">oai:zenodo.org:1471618</subfield> </datafield> <datafield tag="520" ind1=" " ind2=" "> <subfield code="a"><p>Crystalline and amorphous organic materials are an<br> emergent class of heterogeneous photocatalysts for the generation of<br> hydrogen from water, but a direct correlation between their structures<br> and the resulting properties has not been achieved so far. To make a<br> meaningful comparison between structurally different, yet chemically<br> similar porous polymers, we present two porous polymorphs of a<br> triazine-based graphdiyene (TzG) framework from a simple, one-pot<br> reaction using Cu(I) for TzG<sub>Cu</sub> and Pd(II)/Cu(I) for TzG<sub>Pd/Cu</sub> catalyzed<br> homocoupling polymerization. The polymers form via irreversible<br> coupling reactions and give rise to a crystalline (TzG<sub>Cu</sub>) and an<br> amorphous (TzG<sub>Pd/Cu</sub>) polymorph. Notably, the crystalline and<br> amorphous polymorphs are narrow-gap semiconductors with<br> permanent surface areas of 660 m<sup>2</sup> g<sup>-1</sup> and 392 m<sup>2</sup> g<sup>-1</sup>, respectively.<br> Hence, both polymers are ideal heterogeneous photocatalysts for<br> water splitting with some of the highest hydrogen evolution rates<br> reported thus far up to 972 &mu;mol h<sup>-1</sup> g<sup>-1</sup> with and 276 &mu;mol h<sup>-1</sup> g<sup>-1</sup><br> without Pt co-catalyst. We conclude, that crystalline order improves<br> delocalisation, while the amorphous polymorph requires a co-catalyst<br> for efficient charge transfer; this will need to be considered in future<br> rational design of polymer catalysts and organic electronics.</p></subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="0">(orcid)0000-0002-0998-171X</subfield> <subfield code="a">Acharjya, Amitava</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="0">(orcid)0000-0002-3094-4331</subfield> <subfield code="a">Ichangi, Arun</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="0">(orcid)0000-0002-9060-6350</subfield> <subfield code="a">Kochergin, Yaroslav</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="a">Lyu, Pengbo</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="a">Opanasenko, Maksym V.</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="a">Tarábek, Jan</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="a">Vacek Chocholoušová, Jana</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="a">Vacek, Jaroslav</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="a">Schmidt, Johannes</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="a">Nachtigall, Petr</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="u">0000-0002-2130-4930</subfield> <subfield code="a">Thomas, Arne</subfield> </datafield> <datafield tag="700" ind1=" " ind2=" "> <subfield code="u">Humboldt-Universität zu Berlin</subfield> <subfield code="0">(orcid)0000-0002-2592-4168</subfield> <subfield code="a">Bojdys, Michael J.</subfield> </datafield> <datafield tag="856" ind1="4" ind2=" "> <subfield code="s">1012588</subfield> <subfield code="z">md5:28e2c94b2fcc951114c3a091115b7978</subfield> <subfield code="u">https://zenodo.org/record/1471618/files/20180904_TzG_OA.pdf</subfield> </datafield> <datafield tag="856" ind1="4" ind2=" "> <subfield code="s">2435260</subfield> <subfield code="z">md5:539deb91f7a6ffcb2be4809eaae5c9e2</subfield> <subfield code="u">https://zenodo.org/record/1471618/files/20180904_TzG_SI_OA.pdf</subfield> </datafield> <datafield tag="542" ind1=" " ind2=" "> <subfield code="l">open</subfield> </datafield> <datafield tag="980" ind1=" " ind2=" "> <subfield code="a">publication</subfield> <subfield code="b">article</subfield> </datafield> <datafield tag="100" ind1=" " ind2=" "> <subfield code="a">Schwarz, Dana</subfield> </datafield> <datafield tag="653" ind1=" " ind2=" "> <subfield code="a">graphdiyene</subfield> </datafield> <datafield tag="653" ind1=" " ind2=" "> <subfield code="a">photocatalysis</subfield> </datafield> <datafield tag="653" ind1=" " ind2=" "> <subfield code="a">covalent organic frameworks</subfield> </datafield> <datafield tag="653" ind1=" " ind2=" "> <subfield code="a">conjugated microporous polymers</subfield> </datafield> <datafield tag="653" ind1=" " ind2=" "> <subfield code="a">semiconductors</subfield> </datafield> <datafield tag="024" ind1=" " ind2=" "> <subfield code="a">10.1002/cssc.201802034</subfield> <subfield code="2">doi</subfield> </datafield> <datafield tag="245" ind1=" " ind2=" "> <subfield code="a">Tuning the porosity and photocatalytic performance of triazinebased graphdiyene polymers via polymorphism</subfield> </datafield> <datafield tag="536" ind1=" " ind2=" "> <subfield code="c">678462</subfield> <subfield code="a">Layered functional materials - beyond 'graphene'</subfield> </datafield> <datafield tag="650" ind1="1" ind2="7"> <subfield code="a">cc-by</subfield> <subfield code="2">opendefinition.org</subfield> </datafield> </record>
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