Synthesis of Ultrathin Mesoporous CuxRu Nanomeshes for Efficient Kilowatt-Level Nitrate Reduction to Ammonia

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Haitao Xu, Ali Han, Yang Yang, Hongfei Wu, Hao Zhang, Canglang Yao, Yunfei Bu, Zhengping Fu, Yalin Lu, Gang Liu, Jong-Beom Baek, Feng Li, Dongyuan Zhao
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Abstract

The electrochemical conversion of abundant nitrate ions from industrial wastewater and polluted groundwater into value-added ammonia represents an important route for the sustainable development of human society. However, developing efficient and stable catalysts remains a huge challenge. Herein, the synthesis of ultrathin mesoporous CuxRu nanomeshes is reported via a theory-guided ion exchange method for efficient nitrate reduction to ammonia. The prepared CuxRu nanomeshes are composed of Cu atoms anchored ultrathin mesoporous Ru nanomeshes, with a thickness of ≈2–3 nm and a pore distribution between 2 and 10 nm. It offers a high nitrate reduction performance, including a positive onset potential (0.41 V), a high ammonia Faradaic efficiency (94.5%) and a highest ammonia mass activity (0.7 A mg−1) at 0 V up to date. Moreover, a kilowatt-level nitrate reduction is first verified in a flow electrolyzer, with the fastest reported NO3 removal velocity of 12.4 mmol min−1. In situ characterizations and theoretical calculations clearly reveal that Cu atoms can balance the energy barriers in nitrate reduction and competitive hydrogen evolution reactions, leading to improved catalytic performance.

Abstract Image

超薄介孔CuxRu纳米网的合成及其在千瓦级硝酸盐还原制氨中的应用
将工业废水和污染地下水中丰富的硝酸盐离子电化学转化为增值氨是人类社会可持续发展的重要途径。然而,开发高效稳定的催化剂仍然是一个巨大的挑战。本文报道了通过理论指导离子交换法合成超薄介孔CuxRu纳米网,以有效还原硝酸盐为氨。制备的CuxRu纳米网由Cu原子锚定的超薄介孔Ru纳米网组成,其厚度约为2 ~ 3 nm,孔径分布在2 ~ 10 nm之间。它具有很高的硝酸盐还原性能,包括正起始电位(0.41 V),高氨法拉第效率(94.5%)和最高氨质量活性(0.7 a mg−1)。此外,在流动电解槽中首次验证了千瓦级的硝酸盐还原,最快的NO3−去除速度为12.4 mmol min−1。原位表征和理论计算清楚地表明,Cu原子可以平衡硝酸还原和竞争性析氢反应中的能量垒,从而提高催化性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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