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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.


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{
  "DOI": "10.1002/cssc.201802034", 
  "author": [
    {
      "family": "Schwarz, Dana"
    }, 
    {
      "family": "Acharjya, Amitava"
    }, 
    {
      "family": "Ichangi, Arun"
    }, 
    {
      "family": "Kochergin, Yaroslav"
    }, 
    {
      "family": "Lyu, Pengbo"
    }, 
    {
      "family": "Opanasenko, Maksym V."
    }, 
    {
      "family": "Tar\u00e1bek, Jan"
    }, 
    {
      "family": "Vacek Chocholou\u0161ov\u00e1,  Jana"
    }, 
    {
      "family": "Vacek, Jaroslav"
    }, 
    {
      "family": "Schmidt, Johannes"
    }, 
    {
      "family": "Nachtigall, Petr"
    }, 
    {
      "family": "Thomas, Arne"
    }, 
    {
      "family": "Bojdys, Michael J."
    }
  ], 
  "issued": {
    "date-parts": [
      [
        2018, 
        10, 
        18
      ]
    ]
  }, 
  "abstract": "<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 &mu;mol h<sup>-1</sup> g<sup>-1</sup> with and 276 &mu;mol 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>", 
  "title": "Tuning the porosity and photocatalytic performance of triazinebased graphdiyene polymers via polymorphism", 
  "type": "article-journal", 
  "id": "1471618"
}
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