| Autor: |
Tian, Bailin, Wang, Fangyuan, Ran, Pan, Dai, Luhan, Lv, Yang, Sun, Yuxia, Mu, Zhangyan, Sun, Yamei, Tang, Lingyu, Goddard III, William A., Ding, Mengning |
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| Zdroj: |
Nature Communications; 11/22/2024, Vol. 15 Issue 1, p1-14, 14p |
| Abstrakt: |
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 and reaction between organic and oxygen intermediates remain unclear. Here we systematically study the electro-oxidation of aldehydes, alcohols, and amines on Co/Ni-oxyhydroxides with multiple characterizations. Utilizing Fourier transformed alternating current voltammetry (FTacV) measurements, we show the identification and quantification of two key operando parameters (ΔIharmonics/IOER and ΔVharmonics) that can be fundamentally linked to the altered surface coverage (Δ θ OH * / θ OH * OER ) and the changes in adsorption energy of vital oxygenated intermediates ( Δ G OH * EOOR − Δ G OH * OER ), under the influence of organic adsorption/oxidation. Mechanistic analysis based on these descriptors reveals distinct optimal oxyhydroxide surface states for each organics, and elucidates the critical catalyst design principles: balancing organic and M3+δ−OH* coverages and fine-tuning ΔG for key elementary steps, e.g., via precise modulation of chemical compositions, crystallinity, defects, electronic structures, and/or surface bimolecular interactions. Water-assisted electro-catalytic selective oxidation is promising for sustainable production of value-added chemicals. Here the authors quantify two key physio-chemical parameters for efficient mechanistic investigation and rational catalyst design. [ABSTRACT FROM AUTHOR] |
| Databáze: |
Complementary Index |
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