Simultaneous Electrocatalytic Oxidation and Hydrogenation of Biomass‐Derived Aldehydes on Single‐Atom Ru Catalysts
Yuchen Wang, Bin Liu, Yan Duan, Bo Da, Zhuofeng Hu, Huiming Wen, Wanrong Bu, Hao Luo, Suyu Zhang, Hector F. Garcés, Changlong Wang, Tiancheng Mu, Hao Li, Kai Yan
Abstract
Abstract Simultaneous electrocatalytic oxidation (ECO) and hydrogenation (ECH) of biomass‐derived aldehydes offers a promising strategy for high‐value chemical production at both sides in a single electrolytic system. Herein, single‐atom Ru is anchored on Co(OH) 2 (Ru SAs/Co(OH) 2 ) to enable efficient ECO and ECH of 5‐hydroxymethylfurfural (HMF) yielding 2,5‐furandicarboxylic acid (FDCA) and 2,5‐dihydroxymethylfuran (DHMF) as target products. Comparative studies with pristine Co(OH) 2 reveal that Ru─N 4 sites enhance d‐p orbital hybridization, thereby strengthening HMF adsorption, reducing the activation energy of C═O bond, and improving the stability of Co active sites, as confirmed by theory and experiments. Thus, the yield of FDCA and DHMF over the Ru SAs/Co(OH) 2 electrode increases by 23.4% and 24.2% in comparison with its counterpart. In a symmetrical flow‐cell reactor equipped with Ru SAs/Co(OH) 2 catalyst, a remarkable combined yield of 177.7% (FDCA 92.3% + DHMF 85.4%) with perfect conversion of HMF is achieved within 6 h, and the high efficiency is stable over 240 h. The durability of this symmetrical system surpasses most reported systems (<50 h). Furthermore, the revenue of $5812.4 per FDCA ton is estimated for this symmetrical system, demonstrating enormous potential for industrial applications. This coupling work establishes a one‐stone‐two‐birds paradigm for biomass refinery using single‐atom catalysts.