硫点-石墨烯纳米杂化材料：一种在环境条件下高效进行 N 到 NH 固定的无金属电催化剂。

Sulfur dots-graphene nanohybrid: a metal-free electrocatalyst for efficient N-to-NH fixation under ambient conditions.

机构信息

Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province, School of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637002, Sichuan, China.

出版信息

Chem Commun (Camb). 2019 Mar 7;55(21):3152-3155. doi: 10.1039/c9cc00461k.

DOI:10.1039/c9cc00461k

PMID:30801101

Abstract

NH3 is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber-Bosch process with huge CO2 emission. Electrochemical N2 reduction offers a carbon-neutral process to convert N2 to NH3 under ambient conditions, but it requires efficient and stable catalysts to drive the N2 reduction reaction. Herein, we report that a sulfur dots-graphene nanohybrid acts as a metal-free electrocatalyst for ambient N2-to-NH3 conversion with excellent selectivity. When operated in 0.5 M LiClO4, this electrocatalyst achieves a large NH3 yield of 28.56 μg h-1 mgcat.-1 and a high Faradaic efficiency of 7.07% at -0.85 V vs. reversible hydrogen electrode. Notably, it also shows good electrochemical stability.

摘要

氨是一种具有广泛应用的重要化学物质，但它的合成主要依赖于具有大量二氧化碳排放的苛刻哈伯-博世工艺。电化学氮气还原为在环境条件下将氮气转化为氨提供了一种碳中和的过程，但它需要高效和稳定的催化剂来驱动氮气还原反应。在此，我们报告了一种硫点-石墨烯纳米杂化物作为无金属电催化剂，用于环境氮气到氨的转化，具有优异的选择性。当在 0.5 M LiClO4 中运行时，该电催化剂在相对于可逆氢电极的-0.85 V 下实现了 28.56 μg h-1 mgcat.-1 的大氨产率和 7.07%的高法拉第效率。值得注意的是，它还表现出良好的电化学稳定性。