Monolayer Graphitic Carbon Nitride as Metal-Free Catalyst with Enhanced Performance in Photo- and Electro-Catalysis

Nano-Micro Letters

Article

Xiaoyan Jin¹  Seong-Ju Hwang¹  Huiyan Piao²  Goeun Choi³  Jin-Ho Choy⁴  Sung-Pyo Cho⁵  Young Jae Song⁶ 

[1] Department of Materials Science and Engineering, College of Engineering, Yonsei University, 03722, Seoul, Republic of Korea;Intelligent Nanohybrid Materials Laboratory (INML), Institute of Tissue Regeneration Engineering (ITREN), Dankook University, 31116, Cheonan, Republic of Korea;Intelligent Nanohybrid Materials Laboratory (INML), Institute of Tissue Regeneration Engineering (ITREN), Dankook University, 31116, Cheonan, Republic of Korea;College of Science and Technology, Dankook University, 31116, Cheonan, Republic of Korea;Department of Nanobiomedical Science and BK21 PLUS NBM Global Research Center for Regenerative Medicine, Dankook University, 31116, Cheonan, Republic of Korea;Intelligent Nanohybrid Materials Laboratory (INML), Institute of Tissue Regeneration Engineering (ITREN), Dankook University, 31116, Cheonan, Republic of Korea;Department of Pre-Medical Course, College of Medicine, Dankook University, 31116, Cheonan, Republic of Korea;Tokyo Tech World Research Hub Initiative (WRHI), Institute of Innovative Research, Tokyo Institute of Technology, 226-8503, Yokohama, Japan;National Center for Inter-University Research Facilities (NCIRF), Seoul National University, 08826, Seoul, Republic of Korea;Graphene Research Center, Advanced Institute of Convergence Technology, 16229, Suwon, Republic of Korea;SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU), 440-746, Suwon, Republic of Korea;Department of Nano Engineering, Sungkyunkwan University (SKKU), 440-746, Suwon, Republic of Korea;

关键词: Graphitic carbon nitride;    Monolayer;    Atomic image;    Electro- and photo-catalysis;   

DOI  :  10.1007/s40820-022-00794-9

 received in 2021-11-08, accepted in 2021-12-28,  发布年份 2021

来源: Springer

【 摘 要 】

tsThe g-C3N4 monolayer in the perfect 2D limit was successfully realized, for the first time, by the well-defined chemical strategy based on the bottom-up process.The most striking evidence was made from Cs–high resolution transmission electron microscopy measurements by observing directly the atomic structure of g-C3N4 unit cell, which was again supported by the corresponding high resolution transmission electron microscopy image simulation results.We demonstrated that the newly prepared g-C3N4 monolayer showed outstanding photocatalytic activity for H2O2 generation as well as excellent electrocatalytic activity for oxygen reduction reaction.AbstractThe exfoliation of bulk graphitic carbon nitride (g-C3N4) into monolayer has been intensively studied to induce maximum surface area for fundamental studies, but ended in failure to realize chemically and physically well-defined monolayer of g-C3N4 mostly due to the difficulty in reducing the layer thickness down to an atomic level. It has, therefore, remained as a challenging issue in two-dimensional (2D) chemistry and physics communities. In this study, an “atomic monolayer of g-C3N4 with perfect two-dimensional limit” was successfully prepared by the chemically well-defined two-step routes. The atomically resolved monolayer of g-C3N4 was also confirmed by spectroscopic and microscopic analyses. In addition, the experimental Cs-HRTEM image was collected, for the first time, which was in excellent agreement with the theoretically simulated; the evidence of monolayer of g-C3N4 in the perfect 2D limit becomes now clear from the HRTEM image of orderly hexagonal symmetry with a cavity formed by encirclement of three adjacent heptazine units. Compared to bulk g-C3N4, the present g-C3N4 monolayer showed significantly higher photocatalytic generation of H2O2 and H2, and electrocatalytic oxygen reduction reaction. In addition, its photocatalytic efficiency for H2O2 production was found to be the best for any known g-C3N4 nanomaterials, underscoring the remarkable advantage of monolayer formation in optimizing the catalyst performance of g-C3N4.

【 授权许可】

CC BY   
© The Author(s) 2022

【 图 表 】

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