单糖
电动现象
铜
生物量(生态学)
化学
环境化学
无机化学
分析化学(期刊)
地质学
生物化学
有机化学
物理化学
海洋学
作者
Guanghui Ma,Hasan Al‐Mahayni,Na Jiang,Dandan Song,Bo Qiao,Zheng Xu,Ali Seifitokaldani,Suling Zhao,Zhiqin Liang
标识
DOI:10.1002/anie.202401602
摘要
Electrochemical biomass conversion holds promise to upcycle carbon sources and produce valuable products while reducing greenhouse gas emissions. To this end, deep insight into the interfacial mechanism is essential for the rational design of an efficient electrocatalytic route, which is still an area of active research and development. Herein, we report the reduction of dihydroxyacetone (DHA) – the simplest monosaccharide derived from glycerol feedstock – to acetol, the vital chemical intermediate in industries, with faradaic efficiency of 85 ± 5% on a polycrystalline Cu electrode. DHA reduction follows preceding dehydration by coordination with the carbonyl and hydroxyl groups and the subsequent hydrogenation. The electrokinetic profile indicates that the rate‐determining step (RDS) includes a proton‐coupled electron transfer (PCET) to the dehydrated intermediate, revealed by coverage‐dependent Tafel slope and isotopic labeling experiments. An approximate zero‐order dependence of H+ suggests that water acts as the proton donor for the interfacial PCET process. Leveraging these insights, we formulate microkinetic models to illustrate its origin that Eley‐Rideal (E‐R) dominates over Langmuir‐Hinshelwood (L‐H) in governing Cu‐mediated DHA reduction, offering rational guidance that increasing the concentration of the adsorbed reactant alone would be sufficient to promote the activity in designing practical catalysts.
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