Electrocatalytic dual hydrogenation of organic substrates with a Faradaic efficiency approaching 200%
Electrocatalytic dual hydrogenation of organic substrates with a Faradaic efficiency approaching 200%
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DOI：
10.1038/s41929-023-00923-6
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发表时间：
2023-02-20
期刊：
影响因子：
37.8
通讯作者：
Sun, Yujie
中科院分区：
文献类型：
--
作者：
Han, Guanqun;Li, Guodong;Sun, Yujie
电催化氢化的广泛应用可能受到固有限制的阻碍，包括底物溶解度和产物与电解质的难以分离。钯膜电极的使用可以通过物理分离反应性氢原子的形成与不饱和有机底物的氢化来克服上述限制。在这里，通过利用低电位氧化甲醛的钯膜阳极产生的氢气，可以渗透通过膜电极，我们证明了电催化双加氢的不饱和二羧酸是可能的，当另一个钯膜电极也被采用作为阴极。这样的设计使得能够在与电化学电池空间隔离的两个分开的室中在阳极和阴极处电催化氢化相同的底物，理论上最大法拉第效率为200%。
The wide deployment of electrocatalytic hydrogenation may be hindered by intrinsic limitations, including substrate solubility and difficult separation of the products from the electrolyte. The use of palladium membrane electrodes can overcome the aforementioned limitations by physically separating the formation of reactive hydrogen atoms from the hydrogenation of unsaturated organic substrates. Here, by taking advantage of the low-potential oxidation of formaldehyde on a palladium membrane anode to produce hydrogen that can permeate through the membrane electrode, we demonstrate that electrocatalytic dual hydrogenation of unsaturated dicarboxylic acids is possible when another palladium membrane electrode is also adopted as the cathode. Such a design enables the electrocatalytic hydrogenation of the same substrate at both the anode and cathode in two separated chambers spatially isolated from the electrochemical cell with a theoretical maximum Faradaic efficiency of 200%.