TY - JOUR
T1 - Facile Soft-Templated Synthesis of High-Surface Area and Highly Porous Carbon Nitrides
AU - Peer, Maryam
AU - Lusardi, Marcella
AU - Jensen, Klavs F.
N1 - Funding Information:
We gratefully acknowledge the financial support from the Massachusetts Institute of Technology (MIT) Energy Initiative through its seed fund program. This work made use of the MRSEC Shared Experimental Facilities at MIT, supported by the National Science Foundation via Grant DMR-1419807. We appreciate the technical help from the MIT CMSE staff, the members of the Stephanopoulos group, and Lisi Xie for help with UV−vis spectrometry. We are also grateful to the Román group and Strano group at MIT for sharing their instrumentation. We thank Dr. Baris Unal for helpful discussions regarding carbon nitride materials and templating techniques in the early parts of this effort.
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/2/28
Y1 - 2017/2/28
N2 - Mesoporous carbon nitride is synthesized in a one-pot approach using different nonionic surfactants (Pluronic F-127, Pluronic P-123, and Triton X-100) and a melamine cyanurate hydrogen-bonded complex using just water as the solvent. We obtain three-dimensional assembled nanostructures from low-dimensional carbon nitride sheets by taking advantage of supramolecular assembly of melamine and cyanuric acid, moderate interactions between the surfactant and precursors, structure directing effects of the surfactants, and the good thermal stability of the melamine cyanurate sheets formed around the micelles. Different morphologies, including sheetlike, hollow spherical, and tubular or highly porous networks, result depending upon the synthesis approach and the surfactant/precursor ratio. Pseudoternary phase diagrams map the composition of the starting solution to the resultant carbon nitride morphology. Increasing the amount of surfactant leads to a higher carbon residue (C/N ∼ 1) and large BET surface areas (≤300 m2/g). Further tuning of the synthesis parameters as well as addition of HCl produces uniformly porous nanostructures with a high porosity (up to 0.8 cm3/g), a high surface area (>200 m2/g), and yet a stoichiometric C/N ratio (∼0.75). The synthesized high-surface area carbon nitrides show improved light absorption and enhanced photocatalytic activity in a rhodamine B dye degradation reaction under visible light irradiation compared to those of bulk melamine-derived carbon nitride.
AB - Mesoporous carbon nitride is synthesized in a one-pot approach using different nonionic surfactants (Pluronic F-127, Pluronic P-123, and Triton X-100) and a melamine cyanurate hydrogen-bonded complex using just water as the solvent. We obtain three-dimensional assembled nanostructures from low-dimensional carbon nitride sheets by taking advantage of supramolecular assembly of melamine and cyanuric acid, moderate interactions between the surfactant and precursors, structure directing effects of the surfactants, and the good thermal stability of the melamine cyanurate sheets formed around the micelles. Different morphologies, including sheetlike, hollow spherical, and tubular or highly porous networks, result depending upon the synthesis approach and the surfactant/precursor ratio. Pseudoternary phase diagrams map the composition of the starting solution to the resultant carbon nitride morphology. Increasing the amount of surfactant leads to a higher carbon residue (C/N ∼ 1) and large BET surface areas (≤300 m2/g). Further tuning of the synthesis parameters as well as addition of HCl produces uniformly porous nanostructures with a high porosity (up to 0.8 cm3/g), a high surface area (>200 m2/g), and yet a stoichiometric C/N ratio (∼0.75). The synthesized high-surface area carbon nitrides show improved light absorption and enhanced photocatalytic activity in a rhodamine B dye degradation reaction under visible light irradiation compared to those of bulk melamine-derived carbon nitride.
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U2 - 10.1021/acs.chemmater.6b03570
DO - 10.1021/acs.chemmater.6b03570
M3 - Article
AN - SCOPUS:85014057174
SN - 0897-4756
VL - 29
SP - 1496
EP - 1506
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 4
ER -