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

Nano-Micro Letters 2022年第3期14卷 308-321页

作者： Huiyan Piao Goeun Choi Xiaoyan Jin Seong‑Ju Hwang Young Jae Song Sung‑Pyo Cho Jin‑Ho Choy Intelligent Nanohybrid Materials Laboratory(INML) Institute of Tissue Regeneration Engineering(ITREN)Dankook UniversityCheonan 31116Republic of Korea College of Science and Technology Dankook UniversityCheonan 31116Republic of Korea Department of Nanobiomedical Science and BK21 PLUS NBM Global Research Center for Regenerative Medicine Dankook UniversityCheonan 31116Republic of Korea Department of Materials Science and Engineering College of EngineeringYonsei UniversitySeoul 03722Republic of Korea SKKU Advanced Institute of Nanotechnology(SAINT) Sungkyunkwan University(SKKU)Suwon 440‑746Republic of Korea Department of Nano Engineering Sungkyunkwan University(SKKU)Suwon 440‑746Republic of Korea National Center for Inter‑University Research Facilities(NCIRF) Seoul National UniversitySeoul 08826Republic of Korea Graphene Research Center Advanced Institute of Convergence TechnologySuwon 16229Republic of Korea Department of Pre‑Medical Course College of MedicineDankook UniversityCheonan 31116Republic of Korea Tokyo Tech World Research Hub Initiative(WRHI) Institute of Innovative ResearchTokyo Institute of TechnologyYokohama 226‑8503Japan

The exfoliation of bulk graphitic carbon nitride(g-C_(3)N_(4))into monolayer has been intensively studied to induce maximum sur-face area for fundamental studies,but ended in failure to realize chemi-cally and physically well-defined monolayer of g-C_(3)N_(4)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-C_(3)N_(4)with perfect two-dimensional limit”was successfully prepared by the chemically well-defined two-step routes.The atomically resolved monolayer of g-C_(3)N_(4)was also confirmed by spectroscopic and micro-scopic 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-C_(3)N_(4)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-C_(3)N_(4),the present g-C_(3)N_(4)monolayer showed significantly higher photocatalytic gen-eration 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-C_(3)N_(4)nanomaterials,underscoring the remarkable advantage of monolayer formation in optimizing the catalyst performance of g-C_(3)N_(4).

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

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