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具有增强的电催化性能的钌修饰的稳健铜基纳米海绵结构用于环境氮气还原为氨。

Robust Copper-Based Nanosponge Architecture Decorated by Ruthenium with Enhanced Electrocatalytic Performance for Ambient Nitrogen Reduction to Ammonia.

机构信息

Nanodynamics and High-Efficiency Lab for Propulsion and Power, Department of Mechanical, Aerospace & Biomedical Engineering, UT Space Institute, University of Tennessee, Knoxville, Tullahoma, Tennessee 37388, United States.

Center for Nanophase Materials Science, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States.

出版信息

ACS Appl Mater Interfaces. 2023 Mar 8;15(9):11703-11712. doi: 10.1021/acsami.2c20809. Epub 2023 Feb 22.

DOI:10.1021/acsami.2c20809
PMID:36812428
Abstract

Electrochemical conversion of nitrogen to green ammonia is an attractive alternative to the Haber-Bosch process. However, it is currently bottlenecked by the lack of highly efficient electrocatalysts to drive the sluggish nitrogen reduction reaction (NRR). Herein, we strategically design a cost-effective bimetallic Ru-Cu mixture catalyst in a nanosponge (NS) architecture a rapid and facile method. The porous NS mixture catalysts exhibit a large electrochemical active surface area and enhanced specific activity arising from the charge redistribution for improved activation and adsorption of the activated nitrogen species. Benefiting from the synergistic effect of the Cu constituent on morphology decoration and thermodynamic suppression of the competing hydrogen evolution reaction, the optimized RuCu NS catalyst presents an impressive NRR performance with an ammonia yield rate of 26.25 μg h mg (corresponding to 10.5 μg h cm) and Faradic efficiency of 4.39% as well as superior stability in alkaline medium, which was superior to that of monometallic Ru and Cu nanostructures. Additionally, this work develops a new bimetallic combination of Ru and Cu, which promotes the strategy to design efficient electrocatalysts for electrochemical ammonia production under ambient conditions.

摘要

电化学氮气转化为绿色氨是替代哈伯-博世工艺的一种有吸引力的方法。然而,目前它受到缺乏高效电催化剂来驱动缓慢的氮气还原反应(NRR)的限制。在此,我们通过一种快速简便的方法,在纳米海绵(NS)结构中策略性地设计了一种具有成本效益的双金属 Ru-Cu 混合物催化剂。多孔 NS 混合物催化剂表现出大的电化学活性表面积和增强的比活性,这是由于电荷再分配改善了活化氮物种的活化和吸附。受益于 Cu 成分对形态修饰和热力学抑制竞争析氢反应的协同作用,优化的 RuCu NS 催化剂在碱性介质中表现出令人印象深刻的 NRR 性能,氨生成速率为 26.25 μg h mg(对应于 10.5 μg h cm)和 4.39%的法拉第效率,以及优异的稳定性,优于单金属 Ru 和 Cu 纳米结构。此外,这项工作开发了一种新的 Ru 和 Cu 双金属组合,促进了在环境条件下设计高效电催化剂用于电化学氨生产的策略。

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