Donor-acceptor dyads hold the key to tuning of electrochemical properties and enhanced mobility of charge carriers, yet their incorporation into a heterogeneous polymer network proves difficulty owing to the fundamentally different chemistry of the donor and acceptor subunits. A family of sulfur- and nitrogen-containing porous polymers (SNPs) are obtained via Sonogashira-Hagihara cross-coupling and combine electron-withdrawing triazine (C3 N3 ) and electron-donating, sulfur-containing linkers. Choice of building blocks and synthetic conditions determines the optical band gap (from 1.67 to 2.58 eV) and nanoscale ordering of these microporous materials with BET surface areas of up to 545 m2 g-1 and CO2 capacities up to 1.56 mmol g-1 . Our results highlight the advantages of the modular design of SNPs, and one of the highest photocatalytic hydrogen evolution rates for a cross-linked polymer without Pt co-catalyst is attained (194 μmol h-1 g-1 ).

Department of Functional Materials Technical University Berlin Hardenbergstr 40 10623 Berlin Germany

Department of Organic Chemistry Charles University Hlavova 8 128 43 Prague 2 Czech Republic

Department of Physical and Macromolecular Chemistry Charles University Hlavova 8 128 43 Prague 2 Czech Republic

Heyrovsky Institute for Physical Chemistry Academy of Science Czech Republic Dolejškova 3 182 23 Prague 8 Czech Republic

Institute of Organic Chemistry and Biochemistry of the CAS Flemingovo nam 2 166 10 Prague 6 Czech Republic

Leibniz Institut fuer Polymerforschung Dresden e 5 Hohe Str 6 01069 Dresden Germany

Technical University Bergakademie Freiberg Gustav Zeuner Str 3 09599 Freiberg Germany

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