Title: Rapidly constructed Ru-NiMn sites regulate the –CHO/–CH2OH pathway and deprotonate to elevate biomass-derived molecule electrooxidation

Authors: Yuan, Shaoyu; Huang, Tao; Yu, Zhendong; Zhou, Yao; Li, Zheng; Lin, Lu; Feng, Yunchao; Zeng, Xianhai

Abstract: The lack of catalysts with excellent intrinsic activity and durability has hindered the application of electrooxidation for biomass-derived molecules with abundant functional groups. Taking 5-hydroxymethylfurfural (HMF) as an example, the HMF electrooxidation (HMFOR) process consists of the 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) and the 2,5-furandicarbaldehyde (DFF) routes, which involve oxidation of aldehydes/hydroxymethyl groups that cannot be regulated by catalyst design strategies. Herein, we report rapidly constructed bifunctional Ru-NiMn/NF-IH catalysts using induction heating and reveal the intrinsic connection between HMFOR and hydrogen evolution reaction (HER) with the catalytic interface. Atomic-level Ru promoted the Niδ+ species (δ ≥ 3) formation by facilitating deprotonation, which facilitates the cleavage of the C–H bond. The Ru-Mn site precisely regulates HMFOR from preferential hydroxymethyl oxidation to preferential aldehyde. The HER//HMFOR process catalyzed by Ru-NiMn/NF-IH can be carried out at industrial current densities (∼1,000 mA/cm2 at 1.50 V for 200 mM) in a flowing system. Technical-economic analysis has confirmed the economic viability of this system.

Full-Link: https://www.sciencedirect.com/science/article/pii/S2542435126002291