Enhanced hydrogen evolution reactions: Regulating Pt-Ox bonds on bluecoke-based electrocatalyst through simple iron doping

• Published in: International journal of hydrogen energy 2024-09, Vol.81, p.632-642
• Main Authors: Yang, Rongrong, Zhou, Jun, Shi, Yuanqing, Xiao, Yafeng, Wu, Lei, Liew, Rock Keey, Naushad, Mu, Lam, Su Shiung
• Format: Article
• Language: English
• Subjects: Electrocatalyst; Hydrogen evolution reaction; Oxygen-rich activated bluecoke; Ultralow Pt loading
• ISSN: 0360-3199
• DOI: 10.1016/j.ijhydene.2024.07.312

The reconstruction of local electronic states in Pt-Ox is an effective strategy for balancing charge distribution and enhancing the intrinsic activity of noble metals. This study presents the use of highly porous and oxygen-rich activated bluecoke powders as a desirable carbon support, and regulates Pt-Ox bonds by incorporating the Fe as transition metal, leading to the development of an efficient bluecoke-based electrocatalyst characterized (Fe/Pt–O@MKABC) by exceptionally low Pt loading. The loading amount of Pt in Fe/Pt–O@MKABC is only 0.98 wt%, which is less than the 5% reported for commercial Pt/C catalyst, yet its hydrogen evolution performance is comparable. The developed catalyst presents exciting catalytic ability with overpotential of only 17 mV at 10 mA/cm2, a high mass activity of 8.3 A/(cm2·mgpt) at 50 mV, a large turnover frequency of 8.29 H2/s, and outstanding durability with a mere increase of 5 mV over 10000 cycles in acidic electrolyte. Detailed spectroscopic analysis and theoretical calculation results demonstrate that the abundant oxygen on activated bluecoke powders provides an opportunity for the construction of Fe-Oy and Pt-Ox. The introduction of Fe leads to electron rearrangement in Fe/Pt–O@MKABC, promoting electron transfer and reducing the adsorption free energy of H*, and the interaction between Fe-Oy and Pt-Ox enhances the hydrogen evolution reaction (HER) performance. [Display omitted] •Utilizing highly porous and oxygen-rich activated bluecoke powders as defect carbon support.•The introduction of Fe optimizes the Pt-Ox bonds and significantly reduces the Pt loading.•The loading amount of Pt in the developed Fe/Pt–O@MKABC electrocatalyst is only 0.98 wt%.•The interaction between Fe-Oy and Pt-Ox accelerates the Volmer-Heyrovsky process.