Redox-Switchable Single-Atom Catalyst Enables Efficient Aqueous Hydroxymethylfurfural Oxidation

Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989592%3A15640%2F25%3A73633283" target="_blank" >RIV/61989592:15640/25:73633283 - isvavai.cz</a>
Alternative codes found
RIV/61989100:27640/25:10259337
Result on the web
<a href="https://pubs.acs.org/doi/10.1021/acscatal.5c06280" target="_blank" >https://pubs.acs.org/doi/10.1021/acscatal.5c06280</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1021/acscatal.5c06280" target="_blank" >10.1021/acscatal.5c06280</a>

Result language
angličtina
Original language name
Redox-Switchable Single-Atom Catalyst Enables Efficient Aqueous Hydroxymethylfurfural Oxidation
Original language description
The selective aerobic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) is a pivotal step toward biobased polymers, pharmaceuticals, and fuels. Yet, most high-performance catalysts require noble metals and organic solvents and lose activity in water. Here, we report a robust and recyclable heterogeneous catalyst comprising mixed-valence single-atom iron dimers anchored on nitrogen-doped graphene acid (Fe-NGA), which mimics the powerful oxidation center in nonheme diiron oxidases. Spectroscopic and theoretical studies reveal a redox-flexible Fe2+/Fe3+ manifold that, under basic aqueous conditions, evolves into a Fe3+-Fe4+ ferryl species capable of highly selective proton-coupled two-electron oxidations. Fe-NGA achieves 97% HMF conversion with 95% DFF selectivity, a turnover frequency of 17.3 h-1, and a specific productivity of 12.5 mmolDFF gcat -1 h-1 in pure water, surpassing state-of-the-art homogeneous and heterogeneous catalysts. The catalyst is stable with very low performance loss for at least six reactions. By merging such functionalities within a stable and reusable heterogeneous framework, Fe-NGA provides a benchmark earth-abundant catalyst for the effective oxidation of renewable feedstocks.
Czech name
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Czech description
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Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10403 - Physical chemistry

Project
Result was created during the realization of more than one project. More information in the Projects tab.
Continuities
P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Publication year
2025
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

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