Abstract
Electrocatalysis poses many potential advantages for distributed scale biomass valorization. Furanic biomass derivatives such as furfural and 5-hydroxymethylfurfural (HMF) can provide access to a number of value-added chemicals by partial oxidation, including furoic acid, maleic acid, and 2,5-furandicarboxylic acid (FDCA). Here, we have utilized differential reactor studies with online electrochemical mass spectrometry (OLEMS), as well as in-situ attenuated total reflectance surface enhanced infrared reflection absorption spectroscopy (ATR-SEIRAS), to probe these reaction pathways on various metal electrodes. Experimental insights are combined with computational results to piece together plausible mechanisms. We find tradeoffs between decarbonylation activity and self-assembly of furoate intermediates on late transition metals to be critical selectivity-determining and rate-determining process. We also characterize oxidative dehydrogenation paths for furanic aldehydes, which co-produce (anodic) hydrogen gas. Strategies for improved catalyst design will be discussed.
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