- Title
- Tuning the catalytic preference of ruthenium catalysts for nitrogen reduction by atomic dispersion
- Creator
- Yu, Bing; Li, Hao; Ma, Tianyi; White, Jai; Donne, Scott; Yi, Jiabao; Xi, Shibo; Fu, Yang; Henkelman, Graeme; Yu, Hai; Chen, Zuliang
- Relation
- ARC.DE15010306 http://purl.org/au-research/grants/arc/DE150101306 | ARC|LP160100927 http://purl.org/au-research/grants/arc/LP160100927
- Relation
- Advanced Functional Materials Vol. 30, Issue 6, no. 1905665
- Publisher Link
- http://dx.doi.org/10.1002/adfm.201905665
- Publisher
- Wiley
- Resource Type
- journal article
- Date
- 2020
- Description
- Developing cost-effective, high-performance nitrogen reduction reaction (NRR) electrocatalysts is required for the production of green and low-cost ammonia under ambient conditions. Here, a strategy is proposed to adjust the reaction preference of noble metals by tuning the size and local chemical environment of the active sites. This proof-of-concept model is realized by single ruthenium atoms distributed in a matrix of graphitic carbon nitride (Ru SAs/g-C₃N₄). This model is compared, in terms of the NRR activity, to bulk Ru. The as-synthesized Ru SAs/g-C₃N₄ exhibits excellent catalytic activity and selectivity with an NH₃ yield rate of 23.0 μg mgcat⁻¹ h⁻¹ and a Faradaic efficiency as high as 8.3% at a low overpotential (0.05 V vs the reversible hydrogen electrode), which is far better than that of the bulk Ru counterpart. Moreover, the Ru SAs/g-C₃N₄ displays a high stability during five recycling tests and a 12 h potentiostatic test. Density functional theory calculations reveal that compared to bulk Ru surfaces, Ru SAs/g-C₃N₄ has more facile reaction thermodynamics, and the enhanced NRR performance of Ru SAs/g-C₃N₄ originates from a tuning of the d-electron energies from that of the bulk to a single-atom, causing an up-shift of the d-band center toward the Fermi level.
- Subject
- NRR catalysts; nitrogen reduction reaction; cost effectiveness; density functional theory
- Identifier
- http://hdl.handle.net/1959.13/1417965
- Identifier
- uon:37282
- Identifier
- ISSN:1616-301X
- Rights
- This is the peer reviewed version of the following article: Yu, Bing, Hao Li, Jai White, Scott Donne, Jiabao Yi, Shibo Xi, Yang Fu et al. "Tuning the catalytic preference of ruthenium catalysts for nitrogen reduction by atomic dispersion." Advanced Functional Materials 30, no. 6 (2020): 1905665.which has been published in final form at http://dx.doi.org/10.1002/adfm.201905665. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.
- Language
- eng
- Full Text
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