通过在立方亚微米 SnO 颗粒上电还原 N 合成环境 NH。

Ambient NH synthesis via electrochemical reduction of N over cubic sub-micron SnO particles.

机构信息

Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China.

出版信息

Chem Commun (Camb). 2018 Nov 15;54(92):12966-12969. doi: 10.1039/c8cc06524a.

DOI:10.1039/c8cc06524a

PMID:30382249

Abstract

Electrochemical N2-to-NH3 fixation under ambient conditions is emerging as a promising alternative to the energy-intensive and CO2-emitting Haber-Bosch process. However, this process involves difficulty in N2 activation, underlining the demand of electrocatalysts for the N2 reduction reaction (NRR). In this work, cubic sub-micron SnO2 particles on carbon cloth (SnO2/CC) are proposed as an efficient NRR electrocatalyst for ambient N2 conversion to NH3 with excellent selectivity. Electrochemical tests reveal that SnO2/CC attains a large NH3 yield of 1.47 × 10-10 mol s-1 cm-2 at -0.8 V vs. reversible hydrogen electrode (RHE) and a high Faradaic efficiency of 2.17% at -0.7 V vs. RHE in 0.1 M Na2SO4, outperforming most reported aqueous-based NRR electrocatalysts. Notably, it also shows strong electrochemical stability.

摘要

在常温常压条件下进行电化学 N2 到 NH3 的固定，正逐渐成为替代能源密集型且会排放 CO2 的 Haber-Bosch 工艺的一种很有前景的方法。然而，该过程涉及到 N2 活化的困难，这凸显了对用于氮气还原反应 (NRR) 的电催化剂的需求。在这项工作中，提出了在碳纤维布上的立方亚微米 SnO2 颗粒 (SnO2/CC)，作为一种高效的 NRR 电催化剂，可在常温常压下将 N2 转化为 NH3，具有出色的选择性。电化学测试表明，SnO2/CC 在 -0.8 V 相对于可逆氢电极 (RHE) 时可达到 1.47 × 10-10 mol s-1 cm-2 的较大 NH3 产率，在 -0.7 V 相对于 RHE 时可达到 2.17%的高法拉第效率，在 0.1 M Na2SO4 中优于大多数报道的基于水相的 NRR 电催化剂。值得注意的是，它还表现出很强的电化学稳定性。