Digital Repository

Discovering ultrahigh loading of single-metal-atoms via surface tensile-strain for unprecedented urea electrolysis

Show simple item record

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


Files in this item

Files Size Format View

There are no files associated with this item.

This item appears in the following Collection(s)

Show simple item record

Search Repository


Advanced Search

Browse

My Account