TY - JOUR
T1 - Tuning the adsorption behaviors of non-noble electrocatalysts to boost valorization of 5-hydroxymethylfurfural
AU - He, Yunpeng
AU - Zhu, Botao
AU - Wang, Feng
AU - Xiong, Jie
AU - Akram, Muhammad Awais
AU - Feng, Lai
N1 - Publisher Copyright:
© 2023 The Royal Society of Chemistry.
PY - 2023/6/6
Y1 - 2023/6/6
N2 - Nickel-based non-noble materials have been widely used as catalysts for a variety of electrosynthesis reactions due to their low cost and tunable surface properties. However, few of them perform well for the 5-hydroxymethylfurfural (HMF) oxidation reaction (HMFOR) due to their weak adsorption capacity for low-concentration reactants. In this work, Ox-NiCuOz derived from mixed metal oxide (NiCuOz) via anodic reconstruction is employed for the HMFOR, which remarkably outperforms Ox-NiCu(OH)z derived from NiCu-hydroxide (NiCu(OH)z). A series of ex/in situ investigations and theoretical calculations reveal that the adsorptions of HMF and intermediates are enhanced on the low-coordinated surface sites of Ox-NiCuOz, which facilitates the dynamic NiII/NiIII transformation and hence boosts the HMFOR. In addition, Red-NiCuOz derived via cathodic reconstruction is employed for the HMF reduction reaction (HMFRR). As a result, a paired HMFOR/HMFRR electrolysis is conducted using Ox-NiCuOz//Red-NiCuOz as the electrode pair, simultaneously yielding value-added products of 2,5-furandicarboxylic acid (FDCA) and 2,5-bishydroxymethylfuran (BHMF) with a combined faradaic efficiency (FE) of nearly 150% at 2 V. This study provides not only a guideline for non-noble catalyst design towards organic electrosynthesis, but also a rational scenario of paired electrolysis for highly efficient biomass utilization.
AB - Nickel-based non-noble materials have been widely used as catalysts for a variety of electrosynthesis reactions due to their low cost and tunable surface properties. However, few of them perform well for the 5-hydroxymethylfurfural (HMF) oxidation reaction (HMFOR) due to their weak adsorption capacity for low-concentration reactants. In this work, Ox-NiCuOz derived from mixed metal oxide (NiCuOz) via anodic reconstruction is employed for the HMFOR, which remarkably outperforms Ox-NiCu(OH)z derived from NiCu-hydroxide (NiCu(OH)z). A series of ex/in situ investigations and theoretical calculations reveal that the adsorptions of HMF and intermediates are enhanced on the low-coordinated surface sites of Ox-NiCuOz, which facilitates the dynamic NiII/NiIII transformation and hence boosts the HMFOR. In addition, Red-NiCuOz derived via cathodic reconstruction is employed for the HMF reduction reaction (HMFRR). As a result, a paired HMFOR/HMFRR electrolysis is conducted using Ox-NiCuOz//Red-NiCuOz as the electrode pair, simultaneously yielding value-added products of 2,5-furandicarboxylic acid (FDCA) and 2,5-bishydroxymethylfuran (BHMF) with a combined faradaic efficiency (FE) of nearly 150% at 2 V. This study provides not only a guideline for non-noble catalyst design towards organic electrosynthesis, but also a rational scenario of paired electrolysis for highly efficient biomass utilization.
UR - http://www.scopus.com/inward/record.url?scp=85163950540&partnerID=8YFLogxK
U2 - 10.1039/d3ta01609a
DO - 10.1039/d3ta01609a
M3 - Article
AN - SCOPUS:85163950540
SN - 2050-7488
VL - 11
SP - 14284
EP - 14293
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
IS - 26
ER -
