期刊
ADVANCED ENERGY MATERIALS
卷 12, 期 4, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202101078
关键词
graphitic carbon nitride; material characterization; photocatalysis; solar fuel conversion; structure-property-activity relationship
类别
资金
- Max Planck Society
- European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Program [639233]
- Deutsche Forschungsgemeinschaft (DFG) via the Cluster of Excellence e-conversion [EXC2089/1-390776260]
- Center for NanoScience (CENS)
- First Research in Lifetime grant from the National Research Foundation of Korea (NRF) [NRF-2018R1C1B5047313]
- Projekt DEAL
Research on the structure-property relationship of graphitic carbon nitride materials is still ongoing, with individual molecular moieties shown to impact their chemical and opto-electronic properties. Rational molecular design based on these insights can significantly improve photocatalytic reactivity and lead to new paradigms in solar energy storage.
Despite the explosion in the number of publications on the graphitic carbon nitride family of materials, much still remains unknown about their structure and the underlying properties responsible for their various applications. This critical review covers the state-of-the-art in the understanding of their structure-property-photocatalysis relationship, from their molecular constituents to stacking as a (quasi) two-dimensional structure, highlighting the areas in which there is wide agreement and those still unresolved. This review first recounts how the structural understanding of these materials has evolved since the 19th century, followed by a commentary on the best practice for unambiguously characterizing their molecular structure and two-dimensional stacking arrangements. The recent literature is then examined to elucidate how individual molecular moieties affect their various material properties, particularly their chemical and opto-electronic properties, carrier dynamics, and catalytic reactivity, and how their use for energy applications can be impacted by the structural features across each dimension. Lastly, the translation of the aforementioned fundamental insights to rational molecular design is demonstrated, highlighting the synthesis of heptazine-based materials for order-of-magnitude improvement in photocatalytic reactivity, as well as the unusual phenomenon of stabilization of light-induced electrons, an effect currently exploited for a new paradigm in solar energy storage.
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