Robust route to highly porous graphitic carbon nitride microtubes with preferred adsorption ability via rational design of one-dimension supramolecular precursors for efficient photocatalytic CO2 conversion

Qiong Liu, Chengcheng Chen, Kunjie Yuan, Chris D. Sewell, Zhengguo Zhang, Xiaoming Fang, Zhiqun Lin

Research output: Contribution to journalArticlepeer-review

74 Scopus citations

Abstract

The ability to create well-ordered graphitic carbon nitride (g-C3N4) assemblies with good surface adsorption for CO2 represents an important endeavor towards achieving high photocatalytic CO2 reduction activity that yet remains a significant challenge. Herein, a simple yet robust double-solvent-induced self-assembly strategy is, for the first time, developed to yield supramolecular precursors using a single monomer for crafting one-dimensional (1D), highly porous g-C3N4 microtubes that possess remarkable photocatalytic CO2 conversion performance. Intriguingly, the introduction of water and isopropanol triggers the self-assembly of dicyandiamide under hydrothermal conditions to form a melamine-cyanaurate-like complex (MCC) composed of 1D hexagon-shaped, micron-sized crystals with outstanding thermal stability. Subsequent thermal pyrolysis converts these pillar-like crystals into 1D mesoporous g-C3N4 microtubes (denoted MCNM) comprising well-packed nano-leaf-like frameworks (i.e., hierarchical structure). Such unique microtubes are oxygen-doped g-C3N4 and mechanically stable, exhibiting improved visible-light harvesting ability, enhanced charge transfer, increased active sites, and preferred adsorption and activation for CO2, as revealed by a suite of characterization techniques. Consequently, in sharp contrast to bulk g-C3N4, the MCNM manifests a markedly improved photocatalytic activity with a CO evolution rate of 45.16 μmolh−1, reflecting an 11.0-fold enhancement and an apparent quantum efficiency of 2.55% at 420 nm. As such, the double-solvent-induced self-assembly may stand out an effective route to organized supramolecular precursors for preparing hierarchically structured g-C3N4 for efficient photocatalysis.

Original languageEnglish
Article number105104
JournalNano Energy
Volume77
DOIs
StatePublished - Nov 2020

Bibliographical note

Funding Information:
This work was financially supported by the National Natural Science Foundation of China ( 21276088 and U1507201 ), Natural Science Foundation of Guangdong Province ( 2014A030312009 ), China Postdoctoral Science Foundation ( 2020M672638 ) and China Scholarship Council . The authors would like to thank Qian Liu from Shiyanjia Lab ( http://www.shiyanjia.com ) for the support of EPR analysis.

Funding Information:
This work was financially supported by the National Natural Science Foundation of China (21276088 and U1507201), Natural Science Foundation of Guangdong Province (2014A030312009), China Postdoctoral Science Foundation (2020M672638) and China Scholarship Council. The authors would like to thank Qian Liu from Shiyanjia Lab (http://www.shiyanjia.com) for the support of EPR analysis.

Publisher Copyright:
© 2020 Elsevier Ltd

Keywords

  • Double-solvent-induced self-assembly
  • Graphitic carbon nitride
  • One-dimensional mesoporous microtube
  • Photocatalytic CO reduction
  • Surface adsorption

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