Ojha Kasinath, Farber Eliyahu M, Burshtein Tomer Y, Eisenberg David
Schulich Faculty of Chemistry, the Nancy and Stephen Grand Technion Energy Program, the Russell Berrie Nanotechnology Institute, Technion-Israel Institute of Technology, Technion City, Haifa, 3200003, Israel.
Angew Chem Int Ed Engl. 2018 Dec 21;57(52):17168-17172. doi: 10.1002/anie.201810960. Epub 2018 Nov 27.
We report an efficient electrocatalyst for the oxidation of hydrazine, a promising fuel for fuel cells and an important analyte for health and environmental monitoring. To design this material, we emulated natural nitrogen-cycle enzymes, focusing on designing a cooperative, multi-doped active site. The catalytic oxidation occurs on Fe MoC nanoparticles and on edge-positioned nitrogen dopants, all well-dispersed on a hierarchically porous, graphitic carbon matrix that provides active site exposure to mass-transfer and charge flow. The new catalyst is the first carbide with HzOR activity. It operates at the most negative onset potentials reported for carbon-based HzOR catalysts at pH 14 (0.28 V vs. RHE), and has good-to-excellent activity at pH values down to 0. It shows high faradaic efficiency for oxidation to N (3.6 e /N H ), and is perfectly stable for at least 2000 cycles.
我们报道了一种用于肼氧化的高效电催化剂,肼是燃料电池中有前景的燃料,也是健康和环境监测中的重要分析物。为了设计这种材料,我们模仿了天然氮循环酶,重点设计了一个协同的、多掺杂的活性位点。催化氧化发生在FeMoC纳米颗粒和边缘位置的氮掺杂剂上,它们都很好地分散在分级多孔的石墨碳基质上,该基质使活性位点能够接触传质和电荷流动。这种新型催化剂是第一种具有肼氧化还原(HzOR)活性的碳化物。它在pH = 14时以报道的基于碳的HzOR催化剂中最负的起始电位运行(相对于可逆氢电极(RHE)为0.28 V),并且在低至pH = 0时具有良好到优异的活性。它对氧化为N₂显示出高法拉第效率(3.6 e⁻/N₂H₄),并且在至少2000次循环中完全稳定。