Abstract
A titanium carbide (Ti3C2Tx) MXene is employed as an efficient solid support to host a nitrogen (N) and sulfur (S) coordinated ruthenium single atom (RuSA) catalyst, which displays superior activity toward the hydrogen evolution reaction (HER). X-ray absorption fine structure spectroscopy and aberration corrected scanning transmission electron microscopy reveal the atomic dispersion of Ru on the Ti3C2Tx MXene support and the successful coordination of RuSA with the N and S species on the Ti3C2Tx MXene. The resultant RuSA-N-S-Ti3C2Tx catalyst exhibits a low overpotential of 76 mV to achieve the current density of 10 mA cm−2. Furthermore, it is shown that integrating the RuSA-N-S-Ti3C2Tx catalyst on n+np+-Si photocathode enables photoelectrochemical hydrogen production with exceptionally high photocurrent density of 37.6 mA cm−2 that is higher than the reported precious Pt and other noble metals catalysts coupled to Si photocathodes. Density functional theory calculations suggest that RuSA coordinated with N and S sites on the Ti3C2Tx MXene support is the origin of this enhanced HER activity. This work would extend the possibility of using the MXene family as a solid support for the rational design of various single atom catalysts.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 1903841 |
| Journal | Advanced Materials |
| Volume | 31 |
| Issue number | 48 |
| DOIs | |
| State | Published - Oct 17 2019 |
Bibliographical note
KAUST Repository Item: Exported on 2020-10-01Acknowledgements: This work was supported by the King Abdullah University of Science and Technology (KAUST). The authors acknowledge the startup fund of City University of Hong Kong. The authors thank the Australian Research Council for funding this work under the Discovery Grant program. This research was undertaken on the supercomputers in the National Computational Infrastructure (NCI) in Canberra, Australia, which was supported by the Australian Commonwealth Government, and the Pawsey Supercomputing Centre in Perth with funding from the Australian government and the Government of Western Australia.
