Journal article Open Access
Tuning the porosity and photocatalytic performance of triazinebased graphdiyene polymers via polymorphism
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.
DCAT Export
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<dct:title>Tuning the porosity and photocatalytic performance of triazinebased graphdiyene polymers via polymorphism</dct:title>
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<dcat:keyword>graphdiyene</dcat:keyword>
<dcat:keyword>photocatalysis</dcat:keyword>
<dcat:keyword>covalent organic frameworks</dcat:keyword>
<dcat:keyword>conjugated microporous polymers</dcat:keyword>
<dcat:keyword>semiconductors</dcat:keyword>
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<dct:description><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></dct:description>
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Indexed in
- Publication date:
- October 18, 2018
- DOI:
-
- Keyword(s):
- graphdiyene photocatalysis covalent organic frameworks conjugated microporous polymers semiconductors
- Grants:
-
European Commission:
- BEGMAT - Layered functional materials - beyond 'graphene' (678462)
- License (for files):
- Creative Commons Attribution Non Commercial No Derivatives 4.0 International