Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 2, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202113067
Keywords
covalent organic frameworks; hydrogen evolution reaction; near-equilibrium growth; two-dimensional nanomaterials
Categories
Funding
- Chinese Academy of Sciences (Hundred Talents Plan)
- Chinese Academy of Sciences (Strategic Priority Research Program of Sciences) [XDB30000000]
- National Natural Science Foundation of China [52173211, 51873216, 61890940, 91833306, 21922511, 21633012]
- Beijing National Laboratory for Molecular Sciences (BNLMS)
- Croucher Foundation [121111KYSB20200036]
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The facile synthesis and post-processing of chemically stable aza-fused COFs BPT-COF and PT-COF have been achieved using a liquid-phase method. The near-equilibrium growth of COF domains at a low monomer concentration allows for in situ assembly of COFs, resulting in a uniform conducting film on arbitrary substrates. The membranes as electrocatalysts exhibit fast hydrogen evolution reaction with low overpotential and small Tafel slope, making them the best among metal-free catalysts.
Facile synthesis and post-processing of covalent organic frameworks (COFs) under mild synthetic conditions are highly sought after and important for widespread utilizations in catalysis and energy storage. Here we report the synthesis of the chemically stable aza-fused COFs BPT-COF and PT-COF by a liquid-phase method. The process involves the spontaneous polycondensation of vicinal diamines and vicinal diketones, and is driven by the near-equilibrium growth of COF domains at a very low monomer concentration. The method permits in situ assembly of COFs and COF-GO hybrid materials and leads to the formation of a uniform conducting film on arbitrary substrates on vacuum filtration. When used as electrocatalysts, the as-prepared membranes show a fast hydrogen evolution reaction (HER) with a low overpotential (45 mV at 10 mA cm(-2)) and a small Tafel slope (53 mV dec(-1)), which are the best among metal-free catalysts. Our results may open a new route towards the preparation of highly p-conjugated COFs for multifunctional applications.
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