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Target-oriented confinement of Ru-Co nanoparticles inside N-doped carbon spheres via a benzoic acid guided process for high-efficient low-temperature ammonia synthesis
Journal of Energy Chemistry ( IF 14.0 ) Pub Date : 2020-09-08 , DOI: 10.1016/j.jechem.2020.08.067
Jun Ni , Zhenni Tan , Qianjin Sai , Jie Zhu , Xiuyun Wang , Bingyu Lin , Jianxin Lin , Chak-tong Au , Lilong Jiang

Ru-based heterogeneous catalysts have been used in a wide range of important reactions. However, due to the sintering of Ru nanoparticles their practical applications are somewhat restricted. Herein, for the first time we report a new and facile strategy to confine Ru and/or Co nanoparticles (NPs) in the channels of N-doped carbon using benzoic acid to guide the deposition location of Ru. The developed catalyst with confined RuCo alloy particles exhibits high resistance against Ru sintering and displays excellent activity and long term stability for NH3 synthesis, achieving an NH3 synthesis rate of up to 18.9 mmolNH3 gcat−1 h−1 at 400 °C, which is ca. 2.25 times that of the catalyst prepared without confinement (with metal deposited on the support surface). In the latter case, there is increase of nanoparticle size from 2.52 to 4.25 nm together with ca. 48% decrease of NH3 synthesis rate after 68 h at 400 °C. This study provides a new avenue for simple fabrication of precious-metal-based catalysts that are highly resistant against sintering, specifically suitable for low-temperature synthesis of ammonia with outstanding efficiency.



中文翻译:

通过苯甲酸引导的过程,将Ru-Co纳米粒子定向定向限制在N掺杂碳球中,以实现高效的低温氨合成

钌基非均相催化剂已用于许多重要的反应中。但是,由于Ru纳米颗粒的烧结,其实际应用受到一定限制。在本文中,我们首次报道了一种新的且简便的策略,即使用苯甲酸引导Ru的沉积位置,将Ru和/或Co纳米颗粒(NPs)限制在N掺杂碳的通道中。开发的具有受限的RuCo合金颗粒的催化剂显示出高的抗Ru烧结性,并显示出优异的活性和对NH 3合成的长期稳定性,实现了高达18.9 mmol的NH 3合成速率NH3 g cat -1 h -1在400°C,大约 是未限制催化剂(金属沉积在载体表面上)制备的催化剂的2.25倍。在后一种情况下,纳米粒子的尺寸从2.52 nm增加到约4.25 nm。在400°C下放置68 h后,NH 3合成速率降低了48%。这项研究为简单制备具有高抗烧结性的贵金属基催化剂提供了一条新途径,特别适用于低温合成氨,效率极高。

更新日期:2020-09-09
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