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'?> <oai_dc:dc xmlns:dc="http://purl.org/dc/elements/1.1/" xmlns:oai_dc="http://www.openarchives.org/OAI/2.0/oai_dc/" xmlns:xsi="http://www.w3.org/2001/XMLSchema-instance" xsi:schemaLocation="http://www.openarchives.org/OAI/2.0/oai_dc/ http://www.openarchives.org/OAI/2.0/oai_dc.xsd"> <dc:creator>Schwarz, Dana</dc:creator> <dc:creator>Acharjya, Amitava</dc:creator> <dc:creator>Ichangi, Arun</dc:creator> <dc:creator>Kochergin, Yaroslav</dc:creator> <dc:creator>Lyu, Pengbo</dc:creator> <dc:creator>Opanasenko, Maksym V.</dc:creator> <dc:creator>Tarábek, Jan</dc:creator> <dc:creator>Vacek Chocholoušová, Jana</dc:creator> <dc:creator>Vacek, Jaroslav</dc:creator> <dc:creator>Schmidt, Johannes</dc:creator> <dc:creator>Nachtigall, Petr</dc:creator> <dc:creator>Thomas, Arne</dc:creator> <dc:creator>Bojdys, Michael J.</dc:creator> <dc:date>2018-10-18</dc:date> <dc:description>Crystalline and amorphous organic materials are an emergent class of heterogeneous photocatalysts for the generation of hydrogen from water, but a direct correlation between their structures and the resulting properties has not been achieved so far. To make a meaningful comparison between structurally different, yet chemically similar porous polymers, we present two porous polymorphs of a triazine-based graphdiyene (TzG) framework from a simple, one-pot reaction using Cu(I) for TzGCu and Pd(II)/Cu(I) for TzGPd/Cu catalyzed homocoupling polymerization. The polymers form via irreversible coupling reactions and give rise to a crystalline (TzGCu) and an amorphous (TzGPd/Cu) polymorph. Notably, the crystalline and amorphous polymorphs are narrow-gap semiconductors with permanent surface areas of 660 m2 g-1 and 392 m2 g-1, respectively. Hence, both polymers are ideal heterogeneous photocatalysts for water splitting with some of the highest hydrogen evolution rates reported thus far up to 972 μmol h-1 g-1 with and 276 μmol h-1 g-1 without Pt co-catalyst. We conclude, that crystalline order improves delocalisation, while the amorphous polymorph requires a co-catalyst for efficient charge transfer; this will need to be considered in future rational design of polymer catalysts and organic electronics.</dc:description> <dc:identifier>https://zenodo.org/record/1471618</dc:identifier> <dc:identifier>10.1002/cssc.201802034</dc:identifier> <dc:identifier>oai:zenodo.org:1471618</dc:identifier> <dc:relation>info:eu-repo/grantAgreement/EC/H2020/678462/</dc:relation> <dc:rights>info:eu-repo/semantics/openAccess</dc:rights> <dc:rights>https://creativecommons.org/licenses/by-nc-nd/4.0/legalcode</dc:rights> <dc:subject>graphdiyene</dc:subject> <dc:subject>photocatalysis</dc:subject> <dc:subject>covalent organic frameworks</dc:subject> <dc:subject>conjugated microporous polymers</dc:subject> <dc:subject>semiconductors</dc:subject> <dc:title>Tuning the porosity and photocatalytic performance of triazinebased graphdiyene polymers via polymorphism</dc:title> <dc:type>info:eu-repo/semantics/article</dc:type> <dc:type>publication-article</dc:type> </oai_dc:dc>
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