Nanocages of Polymeric Carbon Nitride from Low‐Temperature Supramolecular Preorganization for Photocatalytic CO2 Reduction,Solar RRL

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Nanocages of Polymeric Carbon Nitride from Low‐Temperature Supramolecular Preorganization for Photocatalytic CO2 Reduction
Solar RRL ( IF 6.0 ) Pub Date : 2019-12-03 , DOI: 10.1002/solr.201900469
Jiu Wang ₁ , Shaowen Cao ₁ , Jiaguo Yu _{1,

2}

Affiliation

Polymeric carbon nitride (CN) is considered as one of the most promising photocatalysts to solve energy and environmental crises by solar‐to‐fuel conversion. However, the traditional thermal condensation of monomers usually leads to the disorganized agglomerate structure with a high recombination rate of electron–hole pairs. Herein, the effective synthesis of CN using supramolecular complexes of melamine and cyanuric acid with strengthened hydrogen bonding is presented, which are treated under freeze‐drying conditions as precursors. The as‐prepared CN exhibits a unique nanocage structure, which facilitates the scattering and reflection of incident light and improves the light‐harvesting efficiency. The charge transfer and CO₂ adsorption of CNs is improved because of the extended π‐delocalization, conjugated aromatic system with more exposed lone‐pair electrons and a relatively enlarged specific surface area, caused by the more stretchable and distorted structure of CNs. Consequently, the nanocage‐like CN shows improved performance for photocatalytic CO₂ reduction. This work provides a protocol for tailoring the microstructure of CNs via tuning the weak intermolecular interaction, with the aim of designing high‐performance CN‐based photocatalysts.

中文翻译：

低温超分子预组织的碳氮化物纳米笼对光催化还原CO 2的影响

聚合氮化碳（CN）被认为是解决太阳能和燃料转化带来的能源和环境危机的最有前途的光催化剂之一。但是，传统的单体热缩合通常会导致杂乱的团聚体结构，并具有很高的电子-空穴对复合率。本文介绍了使用三聚氰胺和氰尿酸的超分子配合物增强氢键有效合成CN，将其在冷冻干燥条件下作为前体进行处理的方法。所制备的CN具有独特的纳米笼结构，可促进入射光的散射和反射并提高光收集效率。电荷转移和CO ₂由于CNs的更易拉伸和扭曲的结构而导致π-离域的扩展，共轭芳烃系统具有更多暴露的孤对电子和相对较大的比表面积，因此CNs的吸附得以改善。因此，类似纳米笼的CN表现出了改善的光催化CO ₂还原性能。这项工作为通过设计弱的分子间相互作用调节CNs的微观结构提供了一个协议，目的是设计高性能的基于CN的光催化剂。

更新日期：2019-12-03

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