d-Band center modulation and surface Pt–O bonding promoted Pt nanoparticles with high performance for stable pH-universal hydrogen evolution at ampere-level current densities

Abstract

Developing efficient and stable catalysts capable of driving the electrochemical hydrogen evolution reaction (HER) at ampere-level current densities is crucial for the large-scale production of H₂. This, however, remains a great challenge. This work reports a strategy integrating d-band center modulation and surface Pt–O bonding through carbon nanotube (CNT) support and ultrathin carbon coating to develop Pt-based catalysts for the pH-universal HER with high activity and excellent stability at the ampere-level current densities. Specifically, C@Pt/CNTs-325 consisting of CNT supported Pt nanoparticles with an ultrathin carbon coating is synthesized. The developed catalyst requires overpotentials of only 27.4, 30.3, and 31.1 mV to drive 10.0 mA cm⁻² and exhibits no activity loss at ampere-level current densities for >600 h in acidic, neutral, and alkaline media, respectively. Mechanistic investigations indicate that the CNT support and ultrathin carbon coating can lower the d-band center of Pt and promote surface Pt–O bonding, which optimizes the H atom adsorption and eases the dissociation of H₂O molecules at the catalyst surface to facilitate the HER. More interestingly, C@Pt/CNTs-325 shows great potential for stable overall water splitting (>1000 h) at ampere-level current densities in acidic, neutral, and alkaline media.