Journal
ADVANCED MATERIALS
Volume 29, Issue 40, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201703399
Keywords
2D materials; conjugated microporous polymers; donor-acceptor; membranes; triazine
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Funding
- Czech Science Foundation (GA CR) [CAMs - 16-21151Y]
- European Research Council (ERC) [BEGMAT - 678462]
- Charles University Centre of Advanced Materials (CUCAM) (OP VVV Excellent Research Teams) [CZ.02.1.01/0.0/0.0/15_003/0000417]
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Design and synthesis of ordered, metal-free layered materials is intrinsically difficult due to the limitations of vapor deposition processes that are used in their making. Mixed-dimensional (2D/3D) metal-free van der Waals (vdW) heterostructures based on triazine (C3N3) linkers grow as large area, transparent yellow-orange membranes on copper surfaces from solution. The membranes have an indirect band gap (E-g,E-opt = 1.91 eV, E-g,E-elec = 1.84 eV) and are moderately porous (124 m(2) g(-1)). The material consists of a crystalline 2D phase that is fully sp(2) hybridized and provides structural stability, and an amorphous, porous phase with mixed sp(2)-sp hybridization. Interestingly, this 2D/3D vdW heterostructure grows in a twinned mechanism from a one-pot reaction mixture: unprecedented for metal-free frameworks and a direct consequence of on-catalyst synthesis. Thanks to the efficient type I heterojunction, electron transfer processes are fundamentally improved and hence, the material is capable of metal-free, light-induced hydrogen evolution from water without the need for a noble metal cocatalyst (34 mu mol h(-1) g(-1) without Pt). The results highlight that twinned growth mechanisms are observed in the realm of wet chemistry, and that they can be used to fabricate otherwise challenging 2D/3D vdW heterostructures with composite properties.
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