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.


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    <subfield code="c">2018-10-18</subfield>
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    <subfield code="a">&lt;p&gt;Crystalline and amorphous organic materials are an&lt;br&gt;
emergent class of heterogeneous photocatalysts for the generation of&lt;br&gt;
hydrogen from water, but a direct correlation between their structures&lt;br&gt;
and the resulting properties has not been achieved so far. To make a&lt;br&gt;
meaningful comparison between structurally different, yet chemically&lt;br&gt;
similar porous polymers, we present two porous polymorphs of a&lt;br&gt;
triazine-based graphdiyene (TzG) framework from a simple, one-pot&lt;br&gt;
reaction using Cu(I) for TzG&lt;sub&gt;Cu&lt;/sub&gt; and Pd(II)/Cu(I) for TzG&lt;sub&gt;Pd/Cu&lt;/sub&gt; catalyzed&lt;br&gt;
homocoupling polymerization. The polymers form via irreversible&lt;br&gt;
coupling reactions and give rise to a crystalline (TzG&lt;sub&gt;Cu&lt;/sub&gt;) and an&lt;br&gt;
amorphous (TzG&lt;sub&gt;Pd/Cu&lt;/sub&gt;) polymorph. Notably, the crystalline and&lt;br&gt;
amorphous polymorphs are narrow-gap semiconductors with&lt;br&gt;
permanent surface areas of 660 m&lt;sup&gt;2&lt;/sup&gt; g&lt;sup&gt;-1&lt;/sup&gt; and 392 m&lt;sup&gt;2&lt;/sup&gt; g&lt;sup&gt;-1&lt;/sup&gt;, respectively.&lt;br&gt;
Hence, both polymers are ideal heterogeneous photocatalysts for&lt;br&gt;
water splitting with some of the highest hydrogen evolution rates&lt;br&gt;
reported thus far up to 972 &amp;mu;mol h&lt;sup&gt;-1&lt;/sup&gt; g&lt;sup&gt;-1&lt;/sup&gt; with and 276 &amp;mu;mol h&lt;sup&gt;-1&lt;/sup&gt; g&lt;sup&gt;-1&lt;/sup&gt;&lt;br&gt;
without Pt co-catalyst. We conclude, that crystalline order improves&lt;br&gt;
delocalisation, while the amorphous polymorph requires a co-catalyst&lt;br&gt;
for efficient charge transfer; this will need to be considered in future&lt;br&gt;
rational design of polymer catalysts and organic electronics.&lt;/p&gt;</subfield>
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