You Mingzhu, Yi Shasha, Hou Xinghui, Wang Zhaowu, Ji Haipeng, Zhang Liying, Wang Yu, Zhang Zongtao, Chen Deliang
School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China.
School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China.
J Colloid Interface Sci. 2021 Oct;599:849-856. doi: 10.1016/j.jcis.2021.03.160. Epub 2021 Mar 31.
Defect engineering is an important strategy to regulate electronic structure of electrocatalysts for electrochemical N fixation, aiming at improving the electron state density and enhancing the adsorption and activation of inert N. In this paper, a high-temperature strategy to anneal the natural molybdenite under Ar atmosphere was developed, and the as-obtained molybdenite with S vacancies boosted a high activity for N reduction reaction. In 0.1 M HCl, the catalyst annealed at 800 °C exhibits a high Faradic efficiency of 17.9% and a NH yield of 23.38 μg h mg at -0.35 V versus reversible hydrogen electrode, two times higher than that of the pristine molybdenite. The facile one-step annealing method introduces the defects (e.g., S vacancies) in the surface of the natural molybdenite particles to prepare catalysts for generating ammonia by reducing nitrogen at room temperature under ordinary pressure, promoting the development of low-carbon economic prospect.
缺陷工程是调控用于电化学固氮的电催化剂电子结构的重要策略，旨在改善电子态密度并增强对惰性氮的吸附和活化。本文开发了一种在氩气气氛下对天然辉钼矿进行退火的高温策略，所获得的具有硫空位的辉钼矿对氮还原反应具有高活性。在0.1 M HCl中，800℃退火的催化剂在相对于可逆氢电极-0.35 V时表现出17.9%的高法拉第效率和23.38 μg h mg的氨产率，是原始辉钼矿的两倍。这种简便的一步退火方法在天然辉钼矿颗粒表面引入缺陷（如硫空位），以制备在常压室温下通过还原氮生成氨的催化剂，推动了低碳经济前景的发展。
