Parameterization and quantification of two key operando physio-chemical descriptors for water-assisted electro-catalytic organic oxidation DOI Creative Commons
Bailin Tian, Fangyuan Wang, Pan Ran

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 22, 2024

Electro-selective-oxidation using water as a green oxygen source demonstrates promising potential towards efficient and sustainable chemical upgrading. However, surface micro-kinetics regarding co-adsorption reaction between organic intermediates remain unclear. Here we systematically study the electro-oxidation of aldehydes, alcohols, amines on Co/Ni-oxyhydroxides with multiple characterizations. Utilizing Fourier transformed alternating current voltammetry (FTacV) measurements, show identification quantification two key operando parameters (ΔIharmonics/IOER ΔVharmonics) that can be fundamentally linked to altered coverage ( $$\Delta {\theta }_{{{{{\rm{OH}}}}}^{*}}/{\theta }_{{{{{\rm{OH}}}}}^{*}}^{{{{\rm{OER}}}}}$$ ) changes in adsorption energy vital oxygenated $${\Delta G}_{{{{\rm{OH}}}}*}^{{{{\rm{EOOR}}}}}-{\Delta G}_{{{{\rm{OH}}}}*}^{{{{\rm{OER}}}}}$$ ), under influence adsorption/oxidation. Mechanistic analysis based these descriptors reveals distinct optimal oxyhydroxide states for each organics, elucidates critical catalyst design principles: balancing M3+δ−OH* coverages fine-tuning ΔG elementary steps, e.g., via precise modulation compositions, crystallinity, defects, electronic structures, and/or bimolecular interactions. Water-assisted electro-catalytic selective oxidation is production value-added chemicals. authors quantify physio-chemical mechanistic investigation rational design.

Language: Английский

Transfer learning across different photocatalytic organic reactions DOI Creative Commons
Naoki Noto,

Ryuga Kunisada,

Tabea Rohlfs

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: April 10, 2025

Language: Английский

Citations

1
Parameterization and quantification of two key operando physio-chemical descriptors for water-assisted electro-catalytic organic oxidation DOI Creative Commons
Bailin Tian, Fangyuan Wang, Pan Ran

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 22, 2024

Electro-selective-oxidation using water as a green oxygen source demonstrates promising potential towards efficient and sustainable chemical upgrading. However, surface micro-kinetics regarding co-adsorption reaction between organic intermediates remain unclear. Here we systematically study the electro-oxidation of aldehydes, alcohols, amines on Co/Ni-oxyhydroxides with multiple characterizations. Utilizing Fourier transformed alternating current voltammetry (FTacV) measurements, show identification quantification two key operando parameters (ΔIharmonics/IOER ΔVharmonics) that can be fundamentally linked to altered coverage ( $$\Delta {\theta }_{{{{{\rm{OH}}}}}^{*}}/{\theta }_{{{{{\rm{OH}}}}}^{*}}^{{{{\rm{OER}}}}}$$ ) changes in adsorption energy vital oxygenated $${\Delta G}_{{{{\rm{OH}}}}*}^{{{{\rm{EOOR}}}}}-{\Delta G}_{{{{\rm{OH}}}}*}^{{{{\rm{OER}}}}}$$ ), under influence adsorption/oxidation. Mechanistic analysis based these descriptors reveals distinct optimal oxyhydroxide states for each organics, elucidates critical catalyst design principles: balancing M3+δ−OH* coverages fine-tuning ΔG elementary steps, e.g., via precise modulation compositions, crystallinity, defects, electronic structures, and/or bimolecular interactions. Water-assisted electro-catalytic selective oxidation is production value-added chemicals. authors quantify physio-chemical mechanistic investigation rational design.

Language: Английский

Citations

2