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一种用于高效肼氧化的多掺杂电催化剂。

A Multi-Doped Electrocatalyst for Efficient Hydrazine Oxidation.

作者信息

Ojha Kasinath, Farber Eliyahu M, Burshtein Tomer Y, Eisenberg David

机构信息

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.

出版信息

Angew Chem Int Ed Engl. 2018 Dec 21;57(52):17168-17172. doi: 10.1002/anie.201810960. Epub 2018 Nov 27.

Abstract

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.

摘要

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。

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