TY - JOUR
T1 - A Tour-Guide through Carbon Nitride-Land
T2 - Structure- and Dimensionality-Dependent Properties for Photo(Electro)Chemical Energy Conversion and Storage
AU - Lau, Vincent Wing hei
AU - Lotsch, Bettina V.
N1 - Funding Information:
The authors thank Julia Kröger for insightful discussions. Financial support by the Max Planck Society, the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Program (grant agreement no. 639233, COFLeaf), the Deutsche Forschungsgemeinschaft (DFG) via the Cluster of Excellence “e‐conversion” (project number EXC2089/1–390776260) and by the Center for NanoScience (CENS) is gratefully acknowledged. V.W.‐h.L. was funded by the “First Research in Lifetime” grant from the National Research Foundation of Korea (NRF) under grant number NRF‐2018R1C1B5047313.
Publisher Copyright:
© 2021 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH
PY - 2022/1/27
Y1 - 2022/1/27
N2 - 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.
AB - 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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U2 - 10.1002/aenm.202101078
DO - 10.1002/aenm.202101078
M3 - Review article
AN - SCOPUS:85109397202
SN - 1614-6832
VL - 12
JO - Advanced Energy Materials
JF - Advanced Energy Materials
IS - 4
M1 - 2101078
ER -