An all-in-one cytosine fused dihydroisoquinoline reaction center with ultralow Pt loading for excellent solar-to-hydrogen production

Abstract

Rationally designed carbon nitride materials for solar-to-hydrogen transformation is a promising alternative to fossil fuels. A cytosine-fused dihydroisoquinoline reaction center is constructed through copolymerization of urea with tyrosine, in which the amine of tyrosine promotes the incorporation of a ketone functionality via a ring-closing reaction, playing an important role in boosting HER activity. This construct represents a unique “all-in-one” reaction center that synergistically enhances visible light responsiveness through π-conjugation, improves charge-carrier spatial separation by forming a donor(melon)―bridge(dihydroisoquinoline)―acceptor(cytosine) architecture, and promotes the formation of Pt―O configuration as a highly efficient reaction center by directly loading Pt onto the photoelectron harvesting cytosine. The assembled construct with ultra-low Pt loading (0.37 %) exhibits a H2 production rate of 35200 μmol/g/h and 44.5 % AQY at 420 nm, which are superior to all reported values in HER photocatalysis and fulfills the demand of environmental friendliness, attesting to the success of an unprecedented “all-in-one” design.