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Structural evolution of CrN nanocube electrocatalysts during nitrogen reduction reaction.
Nanoscale ( IF 6.7 ) Pub Date : 2020-09-09 , DOI: 10.1039/d0nr04981f
Zili Ma 1 , Jianhong Chen 2 , Dongbao Luo 3 , Thomas Thersleff 2 , Richard Dronskowski 3 , Adam Slabon 2
Affiliation  

Metal nitrides have been suggested as prospective catalysts for the electrochemical nitrogen reduction reaction (NRR) in order to obtain ammonia at room temperature under ambient pressure. Herein, we report that templated chromium nitride porous microspheres built up by nanocubes (NCs) are an efficient noble-metal-free electrocatalyst for NRR. The CrN NCs catalyst exhibits both a high stability and NH3 yield of 31.11 μg h−1 mgcat.−1 with a Faradaic efficiency (FE) of 16.6% in 0.1 M HCl electrolyte. Complementary physical characterization techniques demonstrate partial oxidation of the pristine CrN NCs during reaction. Structural characterization by means of scanning transmission electron microscopy (STEM) combining electron energy loss spectrum (EELS) and energy dispersive X-ray spectroscopy (EDX) analysis reveals the NC structure to consist of an O-rich core and N-rich shell after NRR. This gradient distribution of nitrogen within the CrN NCs upon completed NRR is distinct to previously reported metal nitride NRR catalysts, because no significant loss of nitrogen occurs at the catalyst surface.

中文翻译:

CrN纳米立方体电催化剂在氮还原反应过程中的结构演变。

已经提出金属氮化物作为电化学氮还原反应(NRR)的预期催化剂,以便在室温和环境压力下获得氨。在这里,我们报道由纳米立方体(NCs)建立的模板化氮化铬多孔微球是NRR的有效的无贵金属电催化剂。CrN NCs催化剂显示出31.11μgh -1 mg cat的高稳定性和NH 3收率-1在0.1 M HCl电解液中的法拉第效率(FE)为16.6%。互补的物理表征技术证明了反应过程中原始CrN NCs的部分氧化。通过结合电子能量损失谱(EELS)和能量色散X射线能谱(EDX)分析的扫描透射电子显微镜(STEM)进行结构表征,揭示了NC结构由NRR后的富含O的核和富含N的壳组成。完成NRR后,CrN NCs中氮的这种梯度分布与以前报道的金属氮化物NRR催化剂不同,因为在催化剂表面不会发生明显的氮损失。
更新日期:2020-10-02
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