Heteroatom-mediated interactions between ruthenium single atoms and an MXene support for efficient hydrogen evolution.

Ramalingam, Vinoth; Varadhan, Purushothaman; Fu, Hui Chun; Kim, Hyunho; Zhang, Daliang; Chen, Shuangming; Song, Li; Ma, Ding; Wang, Yun; Alshareef, Husam N.; He, Jr Hau

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.

Citation

RAMALINGAM, V., VARADHAN, P., FU, H.-C., KIM, H., ZHANG, D., CHEN, S., SONG, L., MA, D., WANG, Y., ALSHAREEF, H.N. and HE, J.-H. 2019. Heteroatom-mediated interactions between ruthenium single atoms and an MXene support for efficient hydrogen evolution. Advanced materials [online], 31(48), article number 1903841. Available from: https://doi.org/10.1002/adma.201903841

• Journal Article Type: Article
• Acceptance Date: Sep 12, 2019
• Online Publication Date: Oct 17, 2019
• Publication Date: Nov 28, 2019
• Deposit Date: Oct 24, 2023
• Publicly Available Date: Dec 11, 2023
• Journal: Advanced materials
• Print ISSN: 0935-9648
• Electronic ISSN: 1521-4095
• Publisher: Wiley
• Peer Reviewed: Peer Reviewed
• Volume: 31
• Issue: 48
• Article Number: 1903841
• DOI: https://doi.org/10.1002/adma.201903841
• Keywords: Hydrogen evolution; Photocathodes; Single atom catalysts
• Public URL: https://rgu-repository.worktribe.com/output/2120440