Abstract:
The electrochemical oxidation of biomass molecules coupling with hydrogen production is a promising strategy to obtain both green energy and value-added chemicals; however, this strategy is limited by the competing oxygen evolution reactions and high energy consumption. Herein, we report a hierarchical CoNi layered double hydroxides (LDHs) electrocatalyst with abundant Ni vacancies for the efficient anodic oxidation of 5-hydroxymethylfurfural (HMF) and cathodic hydrogen evolution. The unique hierarchical nanosheet structure and Ni vacancies provide outstanding activity and selectivity toward several biomass molecules because of the finely regulated electronic structure and highly-exposed active sites. In particular, a high faradaic efficiency (FE) at a high current density (99% at 100 mA cm-2) is achieved for HMF oxidation, and a two-electrode electrolyzer is assembled based on the Ni vacancies-enriched LDH, which realized a continuous synthesis of highly-pure 2,5-furandicarboxylic acid products with high yields (95%) and FE (90%).
摘要:
生物质分子的电化学氧化与制氢耦合是获得绿色能源和增值化学品的有前途的策略;然而,这种策略受到竞争性析氧反应和高能耗的限制。在这里,我们报告了具有丰富Ni空位的分层CoNi层状双氢氧化物(LDHs)电催化剂,用于5-羟甲基糠醛(HMF)的有效阳极氧化和阴极析氢。由于精细调节的电子结构和高度暴露的活性位点,独特的分层纳米片结构和Ni空位对几种生物质分子提供了出色的活性和选择性。特别是,高的法拉第效率(FE)在高电流密度(99%在100mAcm-2)实现HMF氧化,基于富含镍空位的LDH组装了一个双电极电解槽,实现了高纯度2,5-呋喃二羧酸产品的连续合成,收率高(95%)和FE(90%)。