Engineering the electronic structure of platinum single-atom sites via tailored porous carbon nanofibers for large-scale hydrogen production

• Published in: Applied catalysis. B, Environmental Environmental, 2023-10, Vol.335, p.122898, Article 122898
• Main Authors: Han, Ying, Duan, Hengli, Liu, Wei, Zhou, Chenhui, Wang, Baoshun, Jiang, Qinyuan, Feng, Sihua, Yan, Wensheng, Tan, Ting, Zhang, Rufan
• Format: Article
• Language: English
• Subjects: Carbon nanofibers; Electronic structure; Electrospinning; Hydrogen evolution reaction; Pt single-atom catalysts
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2023.122898

Pt single-atom catalysts are promising for efficient hydrogen evolution reactions (HER) due to their ultra-high catalytic activity and atomic utilization. However, developing a scalable preparation method of binder-free Pt single-atom catalysts with optimal electronic structures for large-scale hydrogen production is still a serious challenge. In this work, we fabricated tailored nitrogen-doped porous carbon nanofibers as a support for engineering the electronic structure of Pt single-atom sites via initial micropore trapping and subsequent optimized nitrogen/carbon anchoring. The as-prepared Pt single-atom catalysts exhibited impressively enhanced HER activity and satisfactory stability, superior to the state-of-the-art single-atom catalysts. X-ray absorption structure analysis combined with theoretical simulation demonstrated the mechanisms for HER performance improvement. In particular, the free-standing Pt single-atom catalysts for a binder-free electrode showed a low overpotential of 64 mV even at 500 mA cm−2, indicating promising application for the large-scale hydrogen production. [Display omitted] •Tailored nitrogen-doped porous carbon nanofibers were proposed for engineering the electronic structure of Pt single-atom.•The Pt single-atom catalyst exhibited impressively enhanced HER performance, superior to the state-of-the-art catalysts.•Experimental investigations and theoretical calculations revealed the mechanism of Pt single-atom for efficient HER.•The as-prepared Pt single-atom catalyst as a binder-free electrode achieved efficient large-scale hydrogen production.