Department of Chemistry, Indian Institute of Science Education and Research, Pune, Dr. Homi Bhabha Road, Ward No. 8, NCL Colony, Pashan, Pune, Maharashtra 411008, India.
Department of Chemistry, Indian Institute of Science Education and Research, Pune, Dr. Homi Bhabha Road, Ward No. 8, NCL Colony, Pashan, Pune, Maharashtra 411008, India.
J Colloid Interface Sci. 2023 Jan 15;630(Pt A):477-483. doi: 10.1016/j.jcis.2022.10.007. Epub 2022 Oct 14.
The OH/H dual-ion gradient has a hidden electromotive force of 0.82 V under standard conditions; however, its non-redox nature completely prevents its direct interconversion as electrical driving force. We show by using organic molecules whose heterogeneous electron transfer is pH dependent, OH/H dual-ion energy can be directly harvested as electrical driving force for performing simultaneous electro-organic synthesis and hydrogen fuel production in an electricity effective manner. To demonstrate this dual-ion gradient assisted electro-organic synthesis, 5-hydroxymethylfurfural (HMF) is chosen as the model molecule because of the immense techno commercial applications of its oxidized products. This dual-ion assisted device only required ∼1 V to provide a current density of 50 mA/cm and for achieving the same rate; the traditional state-of-the-art electrolytic cell required a doubling of the applied potential. The dual-ion gradient assisted device can convert biomass-derived HMF to economically important FDCA with ∼90 % yield and ∼87 % Faradaic efficiency with simultaneous H fuel production at a potential as low as 1 V.
在标准条件下,OH/H 双离子梯度具有 0.82 V 的隐藏电动势;然而,其非氧化还原性质完全阻止了其作为电驱动力的直接相互转换。我们通过使用其不均匀电子转移依赖于 pH 值的有机分子,证明了 OH/H 双离子能量可以直接作为电驱动力来有效地进行同时的电有机合成和氢气燃料生产。为了展示这种双离子梯度辅助的电有机合成,选择 5-羟甲基糠醛 (HMF) 作为模型分子,因为其氧化产物具有巨大的技术商业应用价值。该双离子辅助装置仅需约 1 V 的电压即可提供 50 mA/cm 的电流密度,而要达到相同的速率,传统的最先进的电解槽需要将施加的电压提高一倍。双离子梯度辅助装置可以将生物量衍生的 HMF 转化为具有经济重要性的 FDCA,产率约为 90%,同时在 1 V 的低电位下生产 H 燃料,法拉第效率约为 87%。