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

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.