Realizing efficient electrochemical oxidation of 5-hydroxymethylfurfural on a freestanding Ni(OH)2/nickel foam catalyst

Abstract

Abstract:

With the continuous improvement of solar energy production capacity, how to effectively use the electricity generated by renewable solar energy for electrochemical conversion of biomass is a hot topic. Electrochemical conversion of 5-hydroxymethylfurfural (HMF) to biofuels and value-added oxygenated commodity chemicals provides a promising and alternative pathway to convert renewable electricity into chemicals. Although nickel-based eletrocatalysts are well-known for HMF oxidation, their relatively low intrinsic activity, poor conductivity and stability still limit the potential applications. Here, we report the fabrication of a freestanding nickel-based electrode, in which Ni(OH)₂ species were in-situ constructed on Ni foam (NF) support using a facile acid-corrosion-induced strategy. The Ni(OH)₂/NF electrocatalyst exhibits stable and efficient electrochemical HMF oxidation into 2,5-furandicarboxylic acid (FDCA) with HMF conversion close to 100% with high Faraday efficiency. In-situ formation strategy results in a compact interface between Ni(OH)₂ and NF, which contributes to good conductivity and stability during electrochemical reactions. The superior performance benefits from dynamic cyclic evolution of Ni(OH)₂ to NiOOH, which acts as the reactive species for HMF oxidation to FDCA. A scaled-up device based on a continuous-flow electrolytic cell was also established, giving stable operation with a high FDCA production rate of 27 mg h^-1 cm^-2. This job offers a straightforward, economical, and scalable design strategy to design efficient and durable catalysts for electrochemical conversion of valuable chemicals.

Key words: Acid-corrosion-induced, 5-Hydroxymethylfurfural, Electrocatalytic oxidation, Ni electrocatalysis

Yunying Huo, Cong Guo, Yongle Zhang, Jingyi Liu, Qiao Zhang, Zhiting Liu, Guangxing Yang, Rengui Li, Feng Peng. Realizing efficient electrochemical oxidation of 5-hydroxymethylfurfural on a freestanding Ni(OH)₂/nickel foam catalyst[J]. Chinese Journal of Catalysis, 2024, 63: 282-291.

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Figures/Tables 5

Fig. 1. (a) The schematic diagram of nickel foam. SEM (b) and TEM (c,d) images of Ni(OH)2/NF. The EDS mapping images (e), Ni 2p (f) and O 1s (g) peaks of NF and Ni(OH)2/NF.

Fig. 2. (a) CV curves of NF and Ni(OH)2/NF in 1 mol L-1 KOH at a scan rate of 10 mV s-1. (b) LSV curves of Ni(OH)2/NF in 1 mol L-1 KOH with and without HMF (10 mmol L-1). (c,d) Tafel plot and the electrochemical double-layer capacitance of NF and Ni(OH)2/NF electrodes. (e) HPLC traces of electrochemical HMF oxidation catalyzed by Ni(OH)2/NF at 1.45 V (vs. RHE). (f) Reactant and products concentration-reaction time plots for electrochemical HMF oxidation catalyzed by Ni(OH)2/NF under a 1.45 V (vs. RHE). (g) The HMF conversion, the yield and Faradaic efficiency FDCA based on Ni(OH)2/NF electrode at different potentials. (h) The HMF conversion, the yield and the Faradaic efficiency of FDCA based on NF and Ni(OH)2/NF at 1.45 V (vs. RHE). (i) The HMF conversion, the yield and Faradaic efficiency of FDCA obtained by Ni(OH)2/NF electrode for five consecutive cycles of HMFOR.

Fig. 3. SEM (a), EDS mapping (b) and HRTEM (c) images of Ni(OH)2/NF after reaction. XRD patterns (d), Ni 2p (e) and O 1s (f) peak of Ni(OH)2/NF before and after electrochemical reaction.

Fig. 4. Bode phase plots of the in-situ EIS on Ni(OH)2/NF without 10 mmol L-1 HMF (a) and with 10 mmol L-1 HMF (b). In situ Raman spectra of Ni(OH)2/NF electrode during OER (without 10 mmol L-1 HMF) (c) and HMFOR (with 10 mmol L-1 HMF) (d) under increasing potential from OCP to 1.55 V. (e) Multipotential step curves of the Ni(OH)2/NF electrode. (f) Schematic illustration of the surface reconstruction and reaction mechanism.

Fig. 5. Continuous-flow electrolysis. (a) Electrolysis setup for HMFOR in a continuous-flow electrolytic cell. (b) FDCA productivity based on Ni(OH)2/NF at different potentials, different volume flows in a continuous-flow electrolytic cell. (c,d) HMF conversion, the yield and the productivity of FDCA obtained by Ni(OH)2/NF electrode for six consecutive cycles of HMFOR in a continuous-flow electrolytic cell.

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Realizing efficient electrochemical oxidation of 5-hydroxymethylfurfural on a freestanding Ni(OH)₂/nickel foam catalyst

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