Abstract

Understanding the intrinsic nature of materials is considered as a critical approach to reach the desirable catalytic activity. However, there is still a lack of sufficient research on rational reconstruction of catalyst, especially in the field of 5-hydroxymethylfurfural (HMF) oxidation. This work successfully reconstituted Ni MOF/Ag via surface-electrochemical activation, revealing that Ni3+/Ag+ is the main active species for HMF oxidation. This unique evolution not only acquired high-valence active species, but also stably anchored Ag species to the catalyst surface through the generated NiOOH. Importantly, the initial-potential of activated Ni MOF/Ag for HMF oxidation is much smaller than oxygen evolution reaction (OER), so HMF oxidation is more favorable than OER. Meanwhile, open-circuit potential vs. time experiments well illustrated that Ni3+/Ag+ species exhibited the superior self-healing ability during the conversion of HMF → 2, 5-furandicarboxylic acid (FDCA). Nearly 100% HMF conversion and 98.6% Faraday efficiency of FDCA were obtained at 1.623 V vs. RHE. Therefore, a structure–activity relationship between the reconstructed Ni3+/Ag+ species and HMF oxidation was deeply dissected for efficient production of FDCA.

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