TY - JOUR
T1 - Product Ligand-Modification on Ni(OH)2 for Boosted Electrocatalytic Oxidation of Aromatic Alcohols
AU - Wang, Lijun
AU - Yan, Jiabiao
AU - Shi, Kai
AU - Huang, Bingji
AU - Chen, Lisong
AU - Shi, Jianlin
N1 - Publisher Copyright:
© 2026 Wiley-VCH GmbH.
PY - 2026/3/16
Y1 - 2026/3/16
N2 - The development of active electrocatalysts for converting biomass-derived aromatic alcohols into value-added acids is of great significance. Ni(OH)2 has been employed as a cost-effective catalyst, unfortunately, suffering from rather low catalytic activity due to the considerable energy barrier to transform into active NiOOH and the weak interaction with reactants. To address these limitations, a novel “product ligand-modification” (PLM) strategy has been proposed here simply by adopting the target molecule ligands as modification units, which simultaneously facilitates the Ni(II)/Ni(III) redox kinetics and significantly enriches reactants at the catalytic surface via profound π-π stacking interaction. The PLM strategy has been demonstrated to exhibit exceptionally high performance in electro-oxidizing aromatic alcohols into corresponding acids across various product ligand-Ni(OH)2 (PL-Ni(OH)2) catalysts. As a typical paradigm, the aromatic ligand FDCA-modified Ni(OH)2 catalyst (termed FDCA-Ni(OH)2) demonstrates significantly enhanced BHMF electrocatalytic oxidation activity, featuring a BHMF conversion rate of >99.4%, FDCA selectivity and yield of 99.2% and 98.6%, and Faradaic efficiency of 99.0%. Furthermore, FDCA-Ni(OH)2 features an excellent stability for over 250 h in a flow electrolyzer to produce FDCA with a >99.0% purity. This PLM strategy offers valuable insights into the performance enhancement of Ni(OH)2 catalyst for the targeted conversion of aromatic reactants.
AB - The development of active electrocatalysts for converting biomass-derived aromatic alcohols into value-added acids is of great significance. Ni(OH)2 has been employed as a cost-effective catalyst, unfortunately, suffering from rather low catalytic activity due to the considerable energy barrier to transform into active NiOOH and the weak interaction with reactants. To address these limitations, a novel “product ligand-modification” (PLM) strategy has been proposed here simply by adopting the target molecule ligands as modification units, which simultaneously facilitates the Ni(II)/Ni(III) redox kinetics and significantly enriches reactants at the catalytic surface via profound π-π stacking interaction. The PLM strategy has been demonstrated to exhibit exceptionally high performance in electro-oxidizing aromatic alcohols into corresponding acids across various product ligand-Ni(OH)2 (PL-Ni(OH)2) catalysts. As a typical paradigm, the aromatic ligand FDCA-modified Ni(OH)2 catalyst (termed FDCA-Ni(OH)2) demonstrates significantly enhanced BHMF electrocatalytic oxidation activity, featuring a BHMF conversion rate of >99.4%, FDCA selectivity and yield of 99.2% and 98.6%, and Faradaic efficiency of 99.0%. Furthermore, FDCA-Ni(OH)2 features an excellent stability for over 250 h in a flow electrolyzer to produce FDCA with a >99.0% purity. This PLM strategy offers valuable insights into the performance enhancement of Ni(OH)2 catalyst for the targeted conversion of aromatic reactants.
KW - aromatic alcohols electrocatalytic oxidation
KW - cyclic kinetics
KW - nickel hydroxide electrocatalyst
KW - product ligand-modification
KW - π–π stacking interactions
UR - https://www.scopus.com/pages/publications/105029694728
U2 - 10.1002/anie.202525813
DO - 10.1002/anie.202525813
M3 - 文章
AN - SCOPUS:105029694728
SN - 1433-7851
VL - 65
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 12
M1 - e25813
ER -