期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 328, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2023.122530
关键词
Kirkendall effect; Hollow palladium-copper alloy; Biomass oxidation reaction; Oxygen reduction reaction; Hydrogen generation with electricity output
In this study, interconnected hollow PdCu alloy networks (H-PdCu ANs) were fabricated to generate hydrogen (H2) with low energy consumption. The catalyst shows high efficiency in furfural oxidation and oxygen reduction, achieving the simultaneous generation of H2, biomass upgrading, and power output. Density functional theory calculations were performed to elucidate the reaction mechanisms.
It is of sustainable prominence for building an electrocatalytic system to generate hydrogen (H2) with low energy consumption. Herein, interconnected hollow PdCu alloy networks (H-PdCu ANs) are fabricated via Kirkendalleffect during the cyanogel-reduction procedure. The H-PdCu ANs catalyze furfural oxidation at ultralow potential (0.1 VRHE), and facilitate hydrogen atom releasing from the aldehyde groups, eventually harvesting H2. Likewise, the typical catalyst exhibits superior oxygen reduction activity with a positive onset potential of 1.0 VRHE and half-wave potential of 0.88 VRHE. Density functional theory calculations are carried out to illustrate the reaction mechanisms. Subtle integration of the two half-reactions, the catalyst-assembled electrocatalytic system concurrently generate H2 (5 mmol A-1 g-1 h-1), high value-added furoic acid (93.3% of Faraday efficiency) and electricity (16.2 mW cm-2), overturning conventional H2 generation system with electricity input. This work provides transformative insights into developing bifunctional electrocatalysts to synchronously realize H2 generation, biomass upgrading and power output.
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