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添加金的硫化铜空心球用于调节电化学合成氨中氮吸附位点的强度和活性面积。

Au-Added CuS Hollow Spheres to Regulate the Strength and Active Area of N Adsorption Sites for Electrochemical NH Production.

作者信息

Choi Jihyun, Liu Cun, Sung Yung-Eun, Park Hyun S, Yu Taekyung

机构信息

Center for Hydrogen-Fuel Cell Research, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea.

School of Chemical and Biological Engineering, Seoul National University (SNU), 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea.

出版信息

ACS Appl Mater Interfaces. 2025 Jan 15;17(2):3116-3126. doi: 10.1021/acsami.4c10517. Epub 2024 Oct 24.

Abstract

Ammonia is a chemical compound in considerable global demand and plays a crucial role as an environmentally friendly energy carrier for hydrogen energy storage. The electrochemical nitrogen reduction reaction (eNRR) using copper sulfide catalysts is being extensively studied as an environmentally sustainable approach to the energy-intensive Haber-Bosch process for ammonia production. In this study, we aimed to prepare CuS hollow spheres modified with Au nanoparticles using an antisolvent crystallization-based method to be used as the catalysts for eNRR. During the addition of Au to the CuS catalysts, the nitrogen adsorption strength and surface area of the CuS catalysts are significantly regulated and expanded, leading to a noticeable enhancement in electrocatalytic performance for eNRR. Specifically, the ammonia production rate of 2.4 μmol cm h or = 0.2 mA cm is achieved at a selectivity of 52% in neutral aqueous electrolyte, which is more than a 2-fold increase compared to the unmodified CuS catalyst. The findings of this study can contribute to the development of sustainable and environmentally friendly ammonia production in the future.

摘要

氨是一种全球需求量很大的化合物,作为一种用于氢能储存的环境友好型能量载体发挥着关键作用。使用硫化铜催化剂的电化学氮还原反应(eNRR)作为一种环境可持续的方法,正在被广泛研究,以替代用于氨生产的能源密集型哈伯-博施法。在本研究中,我们旨在使用基于反溶剂结晶的方法制备用金纳米颗粒修饰的硫化铜空心球,用作eNRR的催化剂。在向硫化铜催化剂中添加金的过程中,硫化铜催化剂的氮吸附强度和表面积得到显著调节和扩大,从而导致eNRR的电催化性能显著增强。具体而言,在中性水性电解质中,在52%的选择性下实现了2.4 μmol cm⁻² h⁻¹或j = 0.2 mA cm⁻²的氨生成速率,与未修饰的硫化铜催化剂相比增加了两倍多。本研究的结果有助于未来可持续和环境友好型氨生产的发展。

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