TY - JOUR
T1 - Heteroatom-Mediated Interactions between Ruthenium Single Atoms and an MXene Support for Efficient Hydrogen Evolution
AU - Ramalingam, Vinoth
AU - Varadhan, Purushothaman
AU - Fu, Hui-Chun
AU - Kim, Hyunho
AU - Zhang, Daliang
AU - Chen, Shuangming
AU - Song, Li
AU - MA, Ding
AU - Wang, Yun
AU - Alshareef, Husam N.
AU - He, Jr-Hau
N1 - KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: 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.
PY - 2019/10/17
Y1 - 2019/10/17
N2 - 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.
AB - 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.
UR - http://hdl.handle.net/10754/659067
UR - https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.201903841
UR - http://www.scopus.com/inward/record.url?scp=85074097379&partnerID=8YFLogxK
U2 - 10.1002/adma.201903841
DO - 10.1002/adma.201903841
M3 - Article
C2 - 31621970
SN - 0935-9648
VL - 31
SP - 1903841
JO - Advanced Materials
JF - Advanced Materials
IS - 48
ER -
