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Abstract The electrosynthesis from 5-hydroxymethylfurfural (HMF) is considered a green strategy to achieve biomass-derived high-value chemicals. As the molecular structure of HMF is relatively complicated, understanding the HMF adsorption/catalysis behavior on electrocatalysts is vital for biomass-based electrosynthesis. The electrocatalysis behavior can be modulated by tuning the adsorption energy of the reactive molecules. In this work, the HMF adsorption behavior on spinel oxide, Co O is discovered. Correspondingly, the adsorption energy of HMF on Co O is successfully tuned by decorating with single-atom Ir. It is observed that compared with bare Co O , single-atom-Ir-loaded Co O (Ir-Co O ) can enhance adsorption with the C-C groups of HMF. The synergetic adsorption can enhance the overall conversion of HMF on electrocatalysts. With the modulated HMF adsorption, the as-designed Ir-Co O exhibits a record performance (with an onset potential of 1.15 V ) for the electrosyn ....