Electrocatalytic hydrogenation (ECH) provides a “green” route to upgrade oxygenated bio-oil under mild conditions, but is still challenged with the issues of low working current density (<60 mA cm⁻²) and low faradaic efficiency (usually 20–60%) that seriously hinder its practical applications. Herein, we present a dual-catalyst electrochemical route that achieves extremely high faradaic efficiency (>99% for many chemicals) and high working current density (up to 800 mA cm⁻²) in the hydrogenation of model bio-oil compounds. More importantly, efficient deoxygenation to alkanes, often thought to be very difficult in conventional ECH, was achieved in the aqueous electrolysis. The dual-catalyst system consists of a suspended noble-metal catalyst and soluble polyoxometalate (POM). The theoretical calculations indicate that the POM functions as a superacid, changing the common hydrogenation route to a carbocation mechanism and resulting in effective electrolytic deoxygenation of oxygenates. Because no current flows through the catalyst, even a non-conductive catalyst can be used, which provides a great opportunity for extension to general applications.

中文翻译：

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超强酸-贵金属颗粒双催化剂体系高效地将生物酚进行电化学加氢脱氧制烃燃料

电催化加氢（ECH）提供了在温和条件下升级含氧生物油的“绿色”途径，但仍面临工作电流密度低（<60 mA cm ^-2）和法拉第效率低（通常为20-60）的问题％）严重阻碍了其实际应用。本文中，我们提出了一种双催化剂电化学途径，该途径可实现极高的法拉第效率（对许多化学品而言> 99％）和高工作电流密度（高达800 mA cm ^-2））在模型生物油化合物的氢化中。更重要的是，在水电解中实现了通常被认为在常规ECH中非常困难的对烷烃的有效脱氧。双催化剂系统由悬浮的贵金属催化剂和可溶性多金属氧酸盐（POM）组成。理论计算表明，POM用作超强酸，将常见的氢化途径转变为碳正离子化机理，并导致含氧化合物的有效电解脱氧。因为没有电流流过催化剂，所以甚至可以使用非导电催化剂，这为扩展常规应用提供了很大的机会。