Deciphering the Electrocatalytic Reactivity of Glucose Anomers at Bare Gold Electrocatalysts for Biomass-Fueled Electrosynthesis
نویسندگان
چکیده
One of the questions not yet elucidated in electrocatalytic oxidation glucose is whether first step dehydrogenating proton-coupled electron transfer (PCET) concerns hydrogen directly bound to an anomeric carbon (β-anomer) or that oxygen (α-anomer). The knowledge necessary for renewable-energy-powered electrosynthesis chemicals/fuels. To decipher that, we have used α-d-, β-d-, and d-glucose models interrogate electrocatalysis anomers neutral alkaline pHs. We also optimized a pulse methodology grow surfactant- binder-free gold particles onto gas diffusion electrode (GDE) as free-standing electrocatalysts bridge scales between fundamental applied research fuel cells electrolysis. Cyclic voltammetry measurements show electrooxidation all starts at potential region, where surface fully oxidized dominated by adsorption glucose, which rules out hypothesis adsorbs on hydroxylated surface. results pHs highlight better reactivity α-anomer over β-anomer opposite pHs, invalidates traditional thoughts would always be most reactive. Potential-dependent energy profiles computed density functional theory (DFT) mainly confirm promoted approach OH deciphering GDE-Au electrocatalysts, gluconate main product high selectivity faradaic efficiency (>80%), opens opportunities stimulate renewable platform chemicals from cellulosic biomass. toward gluconate, commodity chemical, open biomass-fueled electrosynthesis.
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ژورنال
عنوان ژورنال: ACS Catalysis
سال: 2022
ISSN: ['2155-5435']
DOI: https://doi.org/10.1021/acscatal.2c03399