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.
{ "description": "<p>Crystalline and amorphous organic materials are an<br>\nemergent class of heterogeneous photocatalysts for the generation of<br>\nhydrogen from water, but a direct correlation between their structures<br>\nand the resulting properties has not been achieved so far. To make a<br>\nmeaningful comparison between structurally different, yet chemically<br>\nsimilar porous polymers, we present two porous polymorphs of a<br>\ntriazine-based graphdiyene (TzG) framework from a simple, one-pot<br>\nreaction using Cu(I) for TzG<sub>Cu</sub> and Pd(II)/Cu(I) for TzG<sub>Pd/Cu</sub> catalyzed<br>\nhomocoupling polymerization. The polymers form via irreversible<br>\ncoupling reactions and give rise to a crystalline (TzG<sub>Cu</sub>) and an<br>\namorphous (TzG<sub>Pd/Cu</sub>) polymorph. Notably, the crystalline and<br>\namorphous polymorphs are narrow-gap semiconductors with<br>\npermanent surface areas of 660 m<sup>2</sup> g<sup>-1</sup> and 392 m<sup>2</sup> g<sup>-1</sup>, respectively.<br>\nHence, both polymers are ideal heterogeneous photocatalysts for<br>\nwater splitting with some of the highest hydrogen evolution rates<br>\nreported thus far up to 972 μmol h<sup>-1</sup> g<sup>-1</sup> with and 276 μmol h<sup>-1</sup> g<sup>-1</sup><br>\nwithout Pt co-catalyst. We conclude, that crystalline order improves<br>\ndelocalisation, while the amorphous polymorph requires a co-catalyst<br>\nfor efficient charge transfer; this will need to be considered in future<br>\nrational design of polymer catalysts and organic electronics.</p>", "license": "https://creativecommons.org/licenses/by-nc-nd/4.0/legalcode", "creator": [ { "affiliation": "", "@type": "Person", "name": "Schwarz, Dana" }, { "@id": "https://orcid.org/0000-0002-0998-171X", "@type": "Person", "name": "Acharjya, Amitava" }, { "@id": "https://orcid.org/0000-0002-3094-4331", "@type": "Person", "name": "Ichangi, Arun" }, { "@id": "https://orcid.org/0000-0002-9060-6350", "@type": "Person", "name": "Kochergin, Yaroslav" }, { "@type": "Person", "name": "Lyu, Pengbo" }, { "@type": "Person", "name": "Opanasenko, Maksym V." }, { "@type": "Person", "name": "Tar\u00e1bek, Jan" }, { "@type": "Person", "name": "Vacek Chocholou\u0161ov\u00e1, Jana" }, { "@type": "Person", "name": "Vacek, Jaroslav" }, { "@type": "Person", "name": "Schmidt, Johannes" }, { "@type": "Person", "name": "Nachtigall, Petr" }, { "affiliation": "0000-0002-2130-4930", "@type": "Person", "name": "Thomas, Arne" }, { "affiliation": "Humboldt-Universit\u00e4t zu Berlin", "@id": "https://orcid.org/0000-0002-2592-4168", "@type": "Person", "name": "Bojdys, Michael J." } ], "headline": "Tuning the porosity and photocatalytic performance of triazinebased graphdiyene polymers via polymorphism", "image": "https://zenodo.org/static/img/logos/zenodo-gradient-round.svg", "datePublished": "2018-10-18", "url": "https://zenodo.org/record/1471618", "keywords": [ "graphdiyene", "photocatalysis", "covalent organic frameworks", "conjugated microporous polymers", "semiconductors" ], "@context": "https://schema.org/", "identifier": "https://doi.org/10.1002/cssc.201802034", "@id": "https://doi.org/10.1002/cssc.201802034", "@type": "ScholarlyArticle", "name": "Tuning the porosity and photocatalytic performance of triazinebased graphdiyene polymers via polymorphism" }
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