Boosting The Electrochemical 5-Hydroxymethylfurfural Oxidation by Balancing The Competitive Adsorption of Organic And OH- Over Controllable Reconstructed Ni3 S2 /NiOx.

Abstract

The electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) is a promising method for the efficient production of biomass-derived high-value-added chemicals. However, its practical application is limited by 1) low activity and selectivity caused by the competitive adsorption of HMF and OH- and 2) low operational stability caused by the uncontrollable reconstruction of the catalyst. To overcome these limitations, a series of Ni3 S2 /NiOx -n catalysts with controllable compositions and well-defined structures were synthesized using a novel in-situ controlled surface reconstruction strategy. The adsorption behavior of HMF and OH- could be continuously adjusted by varying the ratio of NiOx to Ni3 S2 on the catalysts surface, as indicated by in-situ characterizations, contact angle analysis and theoretical simulations. Owing to the balanced competitive adsorption of HMF and OH- , the optimized Ni3 S2 /NiOx -15 catalyst exhibited remarkable HMF electrocatalytic oxidation performance, with the current density reaching 366mA cm-2 at 1.5 VRHE and the Faradaic efficiency of the product, 2,5-furanedicarboxylic acid, reaching 98%. Moreover, Ni3 S2 /NiOx -15 exhibited excellent durability, with its activity and structure remaining stable for over 100h of operation. This study provides a new route for the design and construction of catalysts for value-added biomass conversion and offers new insights into enhancing catalytic performance by balancing competitive adsorption. This article is protected by copyright. All rights reserved.