Catalytic efficiency of synthesized, thermally treated, and oxidized carbon nanotube catalysts for water splitting supported by density functional theory


Najri B. A., Saidi K. M., Caglar A., YILDIZ D., KAYA Ş., Ulaş B., ...Daha Fazla

Journal of Power Sources, cilt.685, 2026 (SCI-Expanded, Scopus) identifier

  • Yayın Türü: Makale / Tam Makale
  • Cilt numarası: 685
  • Basım Tarihi: 2026
  • Doi Numarası: 10.1016/j.jpowsour.2026.240511
  • Dergi Adı: Journal of Power Sources
  • Derginin Tarandığı İndeksler: Science Citation Index Expanded (SCI-EXPANDED), Scopus, Chemical Abstracts Core, Chimica, Compendex, INSPEC
  • Anahtar Kelimeler: CNT, DFT, Hydrogen evolution reaction, Oxygen evolution reaction, Water splitting
  • Van Yüzüncü Yıl Üniversitesi Adresli: Evet

Özet

The development of efficient, low-cost, and noble-metal-free electrocatalysts is crucial for sustainable hydrogen production via alkaline water splitting. Herein, pristine carbon nanotubes (CNT), high-temperature-treated CNT (CNT-HT), and nitric-acid-oxidized CNT (CNT-OX) were systematically engineered to elucidate the effects of surface chemistry and defect modulation on bifunctional electrocatalytic performance. Structural characterization by XRD, Raman spectroscopy, SEM, TEM, and EDS revealed that thermal treatment improved graphitic ordering and intertube connectivity, whereas oxidation introduced uniformly distributed oxygen-containing functional groups and defect sites while preserving the CNT framework. Electrochemical measurements in 1 M KOH demonstrated that CNT-OX exhibited the best catalytic activity, delivering Tafel slopes of 221.20 mV/dec for OER and 82.53 mV/dec for HER, together with reduced onset potentials and lower charge-transfer resistance. In addition, electrochemical double-layer capacitance (Cdl) analysis showed that CNT-OX possessed the highest Cdl value (0.825 mF/cm2), indicating a larger electrochemically active surface area and a greater number of accessible active sites. Chronoamperometric analysis confirmed its superior durability. DFT calculations further showed that oxidation decreases the HOMO-LUMO energy gap from 5.093 to 5.061 eV. This combined experimental and theoretical study identifies surface oxidation as an effective route to activate CNTs for high-performance, metal-free alkaline water splitting.