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铜掺杂铈形成多个氧空位,显著提高了环境条件下氮气的还原性能。

Cu doping in CeO to form multiple oxygen vacancies for dramatically enhanced ambient N reduction performance.

机构信息

Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, China.

出版信息

Chem Commun (Camb). 2019 Mar 5;55(20):2952-2955. doi: 10.1039/c9cc00123a.

Abstract

Here, we report the synthesis of Cu-doped CeO2 nanorods (denoted as Cu-CeO2-x, x represents the mass content (wt%) of the doped Cu) by a facile hydrothermal method, followed by thermal treatment in an H2/Ar atmosphere. As the electrocatalyst, Cu-CeO2-3.9 with a large surface area of 95.2 m2 g-1 and mesoporous structure exhibits high electrocatalytic activity toward the N2 reduction reaction (NRR), delivering an NH3 yield rate of 5.3 × 10-10 mol s-1 cm-2 and a faradaic efficiency of 19.1% at -0.45 V (vs. RHE) in a 0.1 M Na2SO4 electrolyte (pH = 6.3), much higher than the NRR performance achieved with pure CeO2 nanorods. The Cu doping can effectively tune the concentration of multiple oxygen vacancies in CeO2, thus resulting in significantly improved NRR activity.

摘要

在这里,我们通过一种简便的水热法合成了掺铜的 CeO2 纳米棒(表示为 Cu-CeO2-x,x 代表掺杂的 Cu 的质量含量(wt%)),然后在 H2/Ar 气氛中进行热处理。作为电催化剂,具有 95.2 m2 g-1 大表面积和介孔结构的 Cu-CeO2-3.9 对 N2 还原反应(NRR)表现出高电催化活性,在 0.1 M Na2SO4 电解质(pH = 6.3)中,在-0.45 V(相对于 RHE)时可提供 5.3 × 10-10 mol s-1 cm-2 的 NH3 产率和 19.1%的法拉第效率,远高于纯 CeO2 纳米棒的 NRR 性能。Cu 掺杂可以有效地调节 CeO2 中多种氧空位的浓度,从而显著提高了 NRR 活性。

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