Metal-organic framework supported Au nanoparticles with organosilicone coating for high-efficiency electrocatalytic N2 reduction to NH3

He, Hongming ¹Zhu, Qian-Qian ¹Yan, Ying ¹Zhang, Han-Wen ¹Han, Zhang-Ye ¹Sun, Hongming ¹Chen, Jing ¹Zhang, Zhihong ²Du, Miao ¹Li, Cheng-Peng¹

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作者信息

1. Tianjin Normal Univ
2. Zhengzhou Univ Light Ind
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Abstract

The development of electrocatalysts for nitrogen reduction reaction (NRR) at ambient conditions, with both high NH3 yield and Faradaic efficiency, is currently a great challenge. To this aim, a unique metal-organic framework (MOF) crystalline matrix with disulfide trimeric unit as the building block was in situ synthesized by integration of dynamic covalent chemistry and coordination chemistry. This MOF with high porosity and excellent stability could be used as a host material to encapsulate well-dispersed Au nanoparticles (NPs) with ultrafine size of 1.9 +/- 0.4 nm. After surface modification of Au@MOF by using organosilicone, the hydrophobic-treated Au@MOF (HT Au@MOF) composite shows remarkable electrocatalytic performances for NRR, with the highest NH3 yield of 49.5 mu g h-1 mgcat.-1 and the state-of-the-art Faradaic efficiency of 60.9% in water medium at ambient conditions. The favorable role of MOFs with functional sulfur groups on modulating the active Au sites and the great effect of hydrophobic coatings on suppressing the competitive hydrogen evolution reaction (HER) have been further demonstrated. This work provides a universal strategy to design composite electrocatalysts for high-efficient and long-term NH3 production.

Key words

Ammonia synthesis/Nitrogen reduction reaction/Au@MOF composite/Electrocatalysis/Hydrophobic layer/NITROGEN REDUCTION/AMMONIA/GOLD/ADSORPTION/CATALYSTS/FIXATION/WATER

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出版年

2022

Applied Catalysis

ISSN：0926-3373

被引量80

参考文献量63

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