合理设计
氮化碳
氰胺
部分
石墨氮化碳
材料科学
光催化
氮化物
催化作用
纳米技术
化学
有机化学
图层(电子)
作者
Vincent Wing‐hei Lau,Igor L. Moudrakovski,Tiago Botari,Simon Weinberger,Maria B. Mesch,Viola Düppel,Jürgen Senker,Volker Blüm,Bettina V. Lotsch
摘要
The heptazine-based polymer melon (also known as graphitic carbon nitride, g-C3N4) is a promising photocatalyst for hydrogen evolution. Nonetheless, attempts to improve its inherently low activity are rarely based on rational approaches because of a lack of fundamental understanding of its mechanistic operation. Here we employ molecular heptazine-based model catalysts to identify the cyanamide moiety as a photocatalytically relevant 'defect'. We exploit this knowledge for the rational design of a carbon nitride polymer populated with cyanamide groups, yielding a material with 12 and 16 times the hydrogen evolution rate and apparent quantum efficiency (400 nm), respectively, compared with the unmodified melon. Computational modelling and material characterization suggest that this moiety improves coordination (and, in turn, charge transfer kinetics) to the platinum co-catalyst and enhances the separation of the photogenerated charge carriers. The demonstrated knowledge transfer for rational catalyst design presented here provides the conceptual framework for engineering high-performance heptazine-based photocatalysts.
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