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Enhanced electrocatalytic biomass oxidation at low voltage by Ni2+-O-Pd interfaces

Journal 2024 · IF 14.7 · 15(1): 1-11 · 发表于 2024 年 7 月 13 日
作者: Pei An,Wang Peng,Zhang Shiyi,Zhang Qinghua,Jiang Xiaoyi,Chen Zhaoxi,Zhou Weiwei,Qin Qizhen,Liu Renfeng,Du Ruian,Li Zhengjian,Qiu Yongcai,Yan Keyou,Gu Lin,Ye Jinyu,Waterhouse Geoffrey I. N.,Huang Wei-Hsiang,Chen Chi-Liang,Zhao Yun,Chen Guangxu
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摘要

Challenges in direct catalytic oxidation of biomass-derived aldehyde and alcohol into acid with high activity and selectivity hinder the widespread biomass application. Herein, we demonstrate that a Pd/Ni(OH) 2 catalyst with abundant Ni 2+ -O-Pd interfaces allows electrooxidation of 5-hydroxymethylfurfural to 2, 5-furandicarboxylic acid with a selectivity near 100 % and 2, 5-furandicarboxylic acid yield of 97.3% at 0.6 volts (versus a reversible hydrogen electrode) in 1 M KOH electrolyte under ambient conditions. The rate-determining step of the intermediate oxidation of 5-hydroxymethyl-2-furancarboxylic acid is promoted by the increased OH species and low C–H activation energy barrier at Ni 2+ -O-Pd interfaces. Further, the Ni 2+ -O-Pd interfaces prevent the agglomeration of Pd nanoparticles during the reaction, greatly improving the stability of the catalyst. In this work, Pd/Ni(OH) 2 catalyst can achieve 100% 5-hydroxymethylfurfural conversion and >90% 2, 5-furandicarboxylic acid selectivity in a flow-cell and work stably over 200 h under a fixed cell voltage of 0.85 V.

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