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DC Field | Value | Language |
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dc.contributor.author | Kumar, Ashwani | en_US |
dc.contributor.author | DEBNATH, BHARATI et al. | en_US |
dc.date.accessioned | 2021-11-18T11:43:38Z | |
dc.date.available | 2021-11-18T11:43:38Z | |
dc.date.issued | 2021-12 | en_US |
dc.identifier.citation | Energy & Environmental Science, 14(12), 6494-6505. | en_US |
dc.identifier.issn | 1754-5692 | en_US |
dc.identifier.issn | 1754-5706 | en_US |
dc.identifier.uri | http://dr.iiserpune.ac.in:8080/xmlui/handle/123456789/6384 | |
dc.identifier.uri | https://doi.org/10.1039/D1EE02603H | en_US |
dc.description.abstract | Single-atom-catalysts (SACs) have recently gained significant attention in energy conversion/storage applications, while the low-loading amount due to their easy-to-migrate tendency causes a major bottleneck. For energy-saving H2 generation, replacing the sluggish oxygen evolution reaction with the thermodynamically favorable urea oxidation reaction (UOR) offers great promise, additionally mitigating the issue of urea-rich water contamination. However, the lack of efficient catalysts to overcome the intrinsically slow kinetics limits its scalable applications. Herein, we discover that incorporating tensile-strain on the surface of a Co3O4 (strained-Co3O4; S-Co3O4) support by the liquid N2-quenching method can significantly inhibit the migration tendency of Rh single-atoms (RhSA), thereby stabilizing an ∼200% higher loading of RhSA sites (RhSA-S-Co3O4; bulk loading ∼6.6 wt%/surface loading ∼11.6 wt%) compared to pristine-Co3O4 (P-Co3O4). Theoretical calculations revealed a significantly increased migration energy barrier of RhSA on the S-Co3O4 surface than on P-Co3O4, inhibiting their migration/agglomeration. Surprisingly, RhSA-S-Co3O4 exhibited exceptional pH-universal UOR activity, requiring record-low working potentials and surpassing Pt/Rh-C, this was due to superior urea adsorption and stabilization of CO*/NH* intermediates, revealed by DFT simulations. Meanwhile, the assembled urea-electrolyzer delivered 10 mA cm−2 at only 1.33 V with robust stability in alkaline media. This work provides a general methodology towards high-loading SACs for scalable applications. | en_US |
dc.language.iso | en | en_US |
dc.publisher | Royal Society of Chemistry | en_US |
dc.subject | Physics | en_US |
dc.subject | 2021-NOV-WEEK3 | en_US |
dc.subject | TOC-NOV-2021 | en_US |
dc.subject | 2021 | en_US |
dc.title | Discovering ultrahigh loading of single-metal-atoms via surface tensile-strain for unprecedented urea electrolysis | en_US |
dc.type | Article | en_US |
dc.contributor.department | Dept. of Physics | en_US |
dc.identifier.sourcetitle | Energy & Environmental Science | en_US |
dc.publication.originofpublisher | Foreign | en_US |
Appears in Collections: | JOURNAL ARTICLES |
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