A one-pot, bottom-up assembly of a pyrimidine-containing porous-organic polymer (PyPOP) was conducted to homogenously deposit the PyPOP atop unmodified graphene sheets, affording a composite material PyPOP@G. The PyPOP demonstrated an appreciable affinity toward CO capture but was found to be largely insulating, hindering its usage in potential electrochemical conversion of CO. However, its composite with graphene was found to be microporous, with maintained affinity toward CO and furthermore demonstrated significant electrochemical activity toward CO reduction (5 mA cm at -1.6 V), not observed in either of its two components separately.
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