Internal Interactions within the Complex Type-II Heterojunction of a Graphitic Carbon Nitride/Black Phosphorus Hybrid Decorated with Graphene Quantum Dots: Implications for Photooxidation Performance


Eroglu Z., Metin O.

ACS Applied Nano Materials, cilt.6, sa.9, ss.7960-7974, 2023 (SCI-Expanded) identifier identifier

  • Yayın Türü: Makale / Tam Makale
  • Cilt numarası: 6 Sayı: 9
  • Basım Tarihi: 2023
  • Doi Numarası: 10.1021/acsanm.3c01187
  • Dergi Adı: ACS Applied Nano Materials
  • Derginin Tarandığı İndeksler: Science Citation Index Expanded (SCI-EXPANDED), Scopus, Compendex
  • Sayfa Sayıları: ss.7960-7974
  • Anahtar Kelimeler: black phosphorus, graphene quantum dots, graphitic carbon nitride, heterojunction, photodegradation
  • Atatürk Üniversitesi Adresli: Evet

Özet

In this study, Fermi levels of graphitic carbon nitride (CN), black phosphorus (BP), and graphene quantum dots (GQDs) were rationally combined and tuned through a band engineering approach. The structure-activity relationship of the resulting heterojunction was characterized by using a combination of X-ray diffraction, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, and solid-state nuclear magnetic resonance techniques. The results revealed that CN and BP were in contact through the formed P-N bridges, while the polar functional groups of GQDs interacted with BP and CN via P-O and N-O interactions, respectively. The superior degradation efficiency is attributed to the synergistic effect of the strong coupling at the interfaces where GQDs@CNBP was tested in removal of organic pollutants [methyl orange (MO) and tetracycline (TC)]. The degradation intermediates in both cases were enlightened by NMR experiments showing no trace of either pollutant or photocatalyst in wastewater. The photogenerated charge migration mechanism was experimentally elucidated as a complex-type-II, which is based on the usage of the farthest charges on the band edges. Scavenger experiments and photooxidation of glucose confirmed the in situ generation of oxidative species of •O2-, H2O2, and •OH, which played a vital role in the photooxidation reactions. A GQDs@CNBP heterojunction with the kinetic rate constants of 0.1415 min-1 (30 min) for MO and 0.0371 min-1 (120 min) for TC is one of the highest kinetics that has been reported in the literature so far.